Review

Advancing Textile Waste Recycling: Challenges and

Opportunities Across Polymer and Non-Polymer Fiber Types
Mehrdad Seifali Abbas-Abadi 1,2,† , Brecht Tomme 3,† , Bahman Goshayeshi 1,4 , Oleksii Mynko 1 , Yihan Wang 1 ,
Sangram Roy 1 , Rohit Kumar 1 , Bhargav Baruah 1 , Karen De Clerck 3 , Steven De Meester 5 ,
Dagmar R. D’hooge 1,3 and Kevin M. Van Geem 1, *

1 Laboratory for Chemical Technology, Department of Materials, Textiles, and Chemical Engineering,
Faculty of Engineering and Architecture, Ghent University, Technologiepark 121, 9052 Zwijnaarde, Belgium;
[email protected] (M.S.A.-A.); [email protected] (B.G.);
[email protected] (O.M.); [email protected] (Y.W.); [email protected] (S.R.);
[email protected] (R.K.); [email protected] (B.B.); [email protected] (D.R.D.)
2 Synpet Technology, R&D Center, Avenue Louise 523, 1050 Brussels, Belgium
3 Centre for Textile Science and Engineering, Department of Materials, Textiles, and Chemical Engineering,
Faculty of Engineering and Architecture, Ghent University, Technologiepark 70a, 9052 Zwijnaarde, Belgium;
[email protected] (B.T.); [email protected] (K.D.C.)
4 Laboratory of Petrochemical Technology (LPT), Department of Chemical Engineering, Aristotle University of
Thessaloniki, University Campus, 54124 Thessaloniki, Greece
5 Laboratory for Circular Process Engineering (LCPE), Department of Green Chemistry and Technology,
Ghent University, 8500 Kortrijk, Belgium; [email protected]
* Correspondence: [email protected]
† These authors contributed equally to this work.

Abstract: The growing environmental impact of textile waste, fueled by the rapid rise in
global fiber production, underscores the urgent need for sustainable end-of-life solutions.
This review explores cutting-edge pathways for textile waste management, spotlighting
innovations that reduce reliance on incineration and landfilling while driving material
circularity. It highlights advancements in collection, sorting, and pretreatment technologies,
as well as both established and emerging recycling methods. Smart collection systems
Academic Editor: Alexey L. Iordanskii utilizing tags and sensors show great promise in streamlining logistics by automating
Received: 9 January 2025
pick-up routes and transactions. For sorting, automated technologies like near-infrared and
Revised: 31 January 2025 hyperspectral imaging lead the way in accurate and scalable fiber separation. Automated
Accepted: 20 February 2025 disassembly techniques are effective at removing problematic elements, though other pre-
Published: 26 February 2025 treatments, such as color and finish removal, still need to be customized for specific waste
Citation: Seifali Abbas-Abadi, M.; streams. Mechanical fiber recycling is ideal for textiles with strong mechanical properties
Tomme, B.; Goshayeshi, B.; Mynko, O.; but has limitations, particularly with blended fabrics, and cannot be repeated endlessly.
Wang, Y.; Roy, S.; Kumar, R.; Baruah, B.; Polymer recycling—through melting or dissolving waste polymers—produces higher-
De Clerck, K.; De Meester, S.; et al.
quality recycled materials but comes with high energy and solvent demands. Chemical
Advancing Textile Waste Recycling:
Challenges and Opportunities Across
recycling, especially solvolysis and pyrolysis, excels at breaking down synthetic polymers
Polymer and Non-Polymer Fiber like polyester, with the potential to yield virgin-quality monomers. Meanwhile, biologi-
Types. Polymers 2025, 17, 628. cal methods, though still in their infancy, show promise for recycling natural fibers like
https://doi.org/10.3390/ cotton and wool. When other methods are not viable, gasification can be used to convert
polym17050628 waste into synthesis gas. The review concludes that the future of sustainable textile recy-
Copyright: © 2025 by the authors. cling hinges on integrating automated sorting systems and advancing solvent-based and
Licensee MDPI, Basel, Switzerland. chemical recycling technologies. These innovations, supported by eco-design principles,
This article is an open access article progressive policies, and industry collaboration, are essential to building a resilient, circular
distributed under the terms and
textile economy.
conditions of the Creative Commons
Attribution (CC BY) license
(https://creativecommons.org/
licenses/by/4.0/).

Polymers 2025, 17, 628 https://doi.org/10.3390/polym17050628

Polymers 2025, 17, 628 2 of 94

Keywords: textile waste; end of life; sustainability; reuse; mechanical recycling; chemical
recycling

1. Introduction
Textiles are an integral part of our society because clothes provide comfort, protection,
and temperature regulation to people, while domestic textiles provide utility around the
house, and technical textiles play crucial roles in their respective industries [1,2]. These
industrial applications may even have positive effects on sustainability, such as textiles used
for wastewater treatment and material recovery [3–11]. While the global significance of
textiles is unquestionable, the sustainability of the textile sector is still far from optimal [12,13].
A sustainable industry can be defined as one that provides for the needs of the current
generation without compromising future generations’ ability to do the same, smartly inte-
grating material usage and the environmental impact of production [14,15]. More generally,
three aspects of the industry can be looked at: the economic, social, and environmental
aspects. This is the so-called “triple bottom line” framework coined by John Elkington [16]
in 1994.
When it comes to the economic aspect, the textile industry is a global giant. The
worldwide production of textile fibers reached 113 million tons in 2021—up from approxi-
mately 24 million tons in 1976—and continues to grow at a consistent rate of 3.4% [17]. This
represents a vital fraction of the world’s economy, with textiles representing 4.19% (USD
882 billion) of the world’s total trade in 2021 as the seventh most-traded product [18]. This
is expected to grow to USD 1320 billion by 2030 [19]. Within Europe, this industry’s largest
subsectors are clothing and accessories (37%, including workwear), industrial and technical
textiles (17%), fabrics (15%), and home textiles (14%) [20].
Textile production is a source of employment for millions of people. While the exact
number of employees in the textile industry is unknown, conservative estimates yielded
430 million in 2017, including those who produced or harvested the raw materials necessary
for the sector [21]. The World Bank estimates the global labor force to be 3.36 billion people
this year, meaning that approximately one out of every eight workers worldwide is affiliated
with the textile industry [22]. While this employment is a huge boon to the social aspect of
the industry, there are also many concerns regarding related issues, such as worker abuse,
low wages, gender equality, child labor, worker health and safety, and a high environmental
cost [23,24].
The environmental aspect is associated with the mass production of textiles because
the textile industry is ranked the fourth most environmentally damaging sector in the
world [25,26]. In 2020, it had the third-highest impact on land use after the food and housing
sectors [27], and it consumes enormous amounts of resources. In 2015, the industry used
over 96 million tons of non-renewable resources, such as oil, fertilizers, dyes, and finishing
chemicals, which will grow to an estimated 295 million tons by 2050 if no changes are
made [28]. Additionally, 79 billion m3 of freshwater were used, with up to 2700 L of water
required to produce a single T-shirt [29]. This freshwater use, particularly for the dyeing
and finishing of textile products, made the sector responsible for approximately 20% of
global clean water pollution [25]. Annually, around 0.5 million tons of microfibers from the
washing of synthetic textiles are also discharged into water bodies, with synthetic clothing
production responsible for 35% of the primary microplastic pollution in the environment.
A single load of laundry for polyester clothing can release up to 700,000 microplastic fibers,
which can ultimately enter the food chain [30]. Other emissions are just as large, with
Polymers 2025, 17, 628 3 of 94

the textile industry accounting for approximately 10% of the world’s total greenhouse gas
(GHG) emissions [31,32].
It is important to note that both industry and consumers are responsible for the afore-
mentioned environmental statistics. From 2000 to 2015, for example, clothing production
doubled from 50 billion units to over 100 billion units, not solely due to a growing world
population and gross domestic product, but disproportionately due to the concept of “fast
fashion” [28]. This consumerist trend entails clothing collections changing much more
frequently and people wearing each garment fewer times before discarding it. Within
those 15 years, the average clothing utilization dropped by 36% across nearly every apparel
category worldwide, although this varies strongly by country, with China seeing a utiliza-
tion rate drop of 70% and US citizens wearing garments for just a quarter of the global
average [28]. It is estimated that more than half of all fast fashion clothing is discarded
within one year of purchase [33]. In addition to social education on fashion culture, a
fundamental revolution should also be considered in the recycling industry and in textile
disposal methods to maximize textile recovery in different ways.
In the initial stage, progress can be initiated by implementing separate bins for textiles
in households and public spaces [34,35]. Currently, textile waste is mainly manually sorted,
with some types being exported or reused, while the remaining textiles are discarded. This
initial phase with better textile sorting is one of the basic steps of recycling but can currently
be time-consuming and expensive because mixed fibers and composites are used in several
textiles. As such, this initial stage is difficult, requiring combined recycling processes [36–38].
To overcome limitations in the current manual sorting system, the automatic sorting of
textiles could be utilized. Many techniques are currently being developed to address the
separation of different textiles [39].
After sorting the design, we should further improve the various methods that have
been developed to recycle textiles. These include physical recycling [40–42], chemical recy-
cling [43–45] (differentiating between solvolysis [46], pyrolysis [47,48], and gasification [49],
all aiming at different small chemical products depending on the type of process and textile
waste [50]), biological recycling (e.g., enzymolysis and fermentation) [51], composting [52],
and mechanical recycling [53] (in which the polymer structure of the textile is preserved).
Mechanical recycling techniques may involve fiber, yarn, and/or fabric recycling, or the
conversion of textiles into primary raw materials through dissolution and/or re-extrusion
to enable fiber production or for other purposes [54–57].
In general, numerous studies have explored various methods of textile recycling. In
this paper, we aim to identify appropriate recycling techniques for different types of textiles
based on their chemical and physical structures [44,58–60]. In what follows, we first discuss
the main textile polymer types and their blends, as well as their manufacturing, to highlight
how advances in sorting and recycling technologies can improve textile waste management.
The review is completed with a life cycle analysis (LCA) section to further help the reader
identify the environmental dimensions of textile waste.

2. Raw Materials, Chemical Principles, and Manufacturing of Textiles

To understand the different end-of-life options for textile products, it is important
to know how they are built because recycling processes follow this same structure, but
backwards. As illustrated in Figure 1, textiles start their life cycle as non-polymers, naturally
occurring polymers, or building blocks that are synthesized into synthetic polymers. These
polymers can then be extruded into fibers, although naturally occurring fibers that do
not need to be extruded also exist, such as cotton or wool. Whatever their composition,
many fibers can, at a further stage, be combined by spinning them into yarns to then make
fabrics via different processes (weaving, knitting, braiding, etc.), or they can be bound
 Polymers
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Polymers 2025, 17, x FOR PEER REVIEW 4 of 94 4 of 10

(e.g., by
(e.g., by adhesives)
(e.g.,and
adhesives) by turned
turnedinto
andadhesives) nonwoven
into
andnonwoven fabrics.
turned into Final
fabrics. processing
Final
nonwoven intoprocessing
processing
fabrics. Final a finished
into a finished
into a finishe
textile product
textile productinvolves
involves coloration
colorationand finishing
and treatments
finishing [61–63].
treatments [61–63].
textile product involves coloration and finishing treatments [61–63].

Figure 1. Thetextile
1. The textilemanufacturing
manufacturing chain,
chain, from
from building
building block
block to end
to end product.
product.
Figure 1. The textile manufacturing chain, from building block to end product.

In the
In the following
followingsections,
sections,the
the main
main categories
categories of fiber
of fiber production,
production, as well as their
as production,
well as their
In the following sections, the main categories of fiber as well as thei
embedding
embedding inintextile
textilemanufacturing
manufacturing processes,
processes, areare elaborated on.
elaborated
embedding in textile manufacturing processes,on.
are elaborated on.
2.1. Fiber Production
2.1. Fiber ProductionRoutes
Routes
2.1. Fiber Production Routes
Fibers can
Fibers canbe
benaturally
naturallyoccurring
occurring or or man-made.
man-made. Historically, textiles
werewere produced
Fibers can be naturally occurringHistorically,
or man-made. textiles
Historically,produced
textiles were produce
from naturally occurring
occurring fibers,
fibers, such
such as
as animal
animal wool,
wool, cotton,
cotton, silk,
silk, various
various types
types ofof cellulosic
cellu-
from naturally occurring fibers, such as animal wool, cotton, silk, various types of cellu
products, and and
losic products, asbestos [64].[64].
losicasbestos
products, However,
andHowever,
asbestos thethe
emergence
However,ofof
emergence
[64]. commercial
the emergencesynthetic
commercial synthetic polymers
poly-
of commercial synthetic poly
mersadvanced
and and advanced
fiber fiber production
production processes
processes hashas
led led
to to
thethe widespread
widespread usage
usage
mers and advanced fiber production processes has led to the widespread usage of man of
of man-
man-made
made fibers,
fibers, such as such
madeas those
those basedbased
fibers, on the
such on the synthetic
as synthetic
those based onpolymers
polymers polyester,
polyester,
the synthetic polyamide,
polyamide,
polymers poly-
polyolefins,
polyester, polyamide, poly
olefins,
and and polyurethane
polyurethane (PU), (PU),
man-made man-made
natural natural
polymerspolymers
(e.g., (e.g.,
viscose viscose
olefins, and polyurethane (PU), man-made natural polymers (e.g., viscoseand and lyocell),
lyocell), and non-
and lyocell
and non-polymers
polymers (e.g.,and (e.g.,
carbon carbon and glass)
and glass)(e.g.,
non-polymers [65,66]. [65,66].
carbon Examples
Examples
and glass) of these
of[65,66].
these three three categories
categories
Examples of theseareare
shown
three categories ar
shown
in Figurein Figure
2. 2.
shown in Figure 2.

Figure 2. Fiber categories based on polymer and fiber types.

Figure 2. Fiber
Figure 2. Fiber categories basedcategories based
on polymer andonfiber
polymer and fiber types.
types.

Global
Global fiber
fiber production has
Global fiber
production reestablished
hasproduction
reestablished hasaareestablished
growing
growing trend
trend after
after aa slight
a growing slight decline
after ain
trenddecline inslight
2020 decline i
2020 due to the2020
coronavirus disease
duedisease 2019
to the coronavirus (COVID-19) pandemic.
diseasepandemic.
2019 (COVID-19) In 2022, a record
In 116
due to the coronavirus 2019 (COVID-19) In 2022,pandemic.
a record 116 2022, a record 11
million
million tons of fibers
millionwere produced,
tons of fibers which
were is expected
produced, to reach
which is 147 million
expected to tons147
reach by million
2030 tons by 203
tons of fibers were produced, which is expected to reach 147 million tons by 2030 if business
if business continues per the currentper
if business standard [67]. Among them,
[67]. polyester fiberspolyester
ac-
continues per the current continues
standard [67].the current
Among standard
them, polyester Amongaccounted
fibers them, for an fibers ac
counted for an counted
overwhelming
for an majority of
overwhelming 54% of the
majority net
of produced
54% of the fibers,
net followed
produced by followed b
fibers,
overwhelming majority of 54% of the net produced fibers, followed by cotton at 22%.
cotton at 22%. Man-made cellulosic
cotton at 22%. Man-madefibers cellulosic
(MMCFs)fibersand polyamide
(MMCFs) and fibers are the next
polyamide twoare the next tw
fibers
Man-made cellulosic fibers (MMCFs) and polyamide fibers are the next two most important
fibers, accounting for 6% and 5% of global fiber production, respectively. Animal-derived
fibers accounted for only 2% of the total, while other natural fibers accounted for 6%, and
 Polymers 2025, 17, x FOR PEER REVIEW 5 of 104

Polymers 2025, 17, 628 5 of 94

most important fibers, accounting for 6% and 5% of global fiber production, respectively.
Animal-derived fibers accounted for only 2% of the total, while other natural fibers ac-
other man-made
counted for 6%, andfibers of synthetic
other man-madepolymers
fibers of (e.g., polyolefins
synthetic polymers and polyacrylics)
(e.g., polyolefinsaccounted
and
for 5% (see Figure 3) [17]. Besides these commonly used fibers
polyacrylics) accounted for 5% (see Figure 3) [17]. Besides these commonly produced in used
largefibers
quantities,
there are unique
produced in large industrial
quantities, fibers produced
there are from bothfibers
unique industrial organic and inorganic
produced from bothmaterials,
or-
such as optical poly(methyl methacrylate) (PMMA) fibers [68], aramid
ganic and inorganic materials, such as optical poly(methyl methacrylate) (PMMA) fibers fibers, and carbon
fibersaramid
[68], [69], which serve
fibers, and specialized
carbon industrial
fibers [69], applications
which serve and
specialized are produced
industrial in limited
applications
and are produced
quantities in limited
(not included in quantities
Figure 3). (not included in Figure 3).

Figure
Figure 3.
3. Worldwide
Worldwidedistribution
distributionofoffiber
fiberextraction
extractionand production.
and Natural
production. fibers
Natural represent
fibers 30%30% of
represent
of
thethe total,
total, whileman-made
while man-madefibers
fibersrepresent
represent 70% [17].
[17].

2.1.1. Natural
2.1.1. NaturalFibers
Fibers
Naturalfibers
Natural fibersoccur
occurinintheir
theirfibrous
fibrousstructure
structureininnature
natureand
andcan
canbebeextracted
extracted
forfor
in-indus-
trial use.use.
dustrial TheyTheyareare
mostly
mostlymade
made upupofofnatural
naturalpolymers
polymers produced
produced byby plants
plantsand
andani-
animals,
mals, but there
but there are also
are also non-polymer
non-polymer mineralfibers
mineral fibers that
that occur
occurnaturally
naturallythrough
throughgeologi-
geological
cal processes
processes [70].
[70].

Natural
NaturalFibers
FibersofofNatural
NaturalPolymers
Polymers
Natural
Natural fibers
fibers of natural polymers
of natural polymers can canbebecategorized
categorizedintointopolysaccharide
polysaccharidefibers,
fibers,which
which are plant-based, and protein fibers, which are animal-based.
are plant-based, and protein fibers, which are animal-based. Polysaccharide fibers Polysaccharide fibers
consist
consist of monosaccharide units linked by glycosidic bonds [59]. By far the
of monosaccharide units linked by glycosidic bonds [59]. By far the most important polysac- most important
polysaccharide
charide in the in the textile
textile industry
industry is cellulose,
is cellulose, which
which is is composedof
composed of D-glucose
D-glucose mono-
monomers
mers linked by β-(1,4)-glycosidic bonds [59]. Cellulose is a main constituent of plant cell
linked by β-(1,4)-glycosidic bonds [59]. Cellulose is a main constituent of plant cell walls
walls and is found in many different natural plant fibers: seed fibers (e.g., cotton and ka-
and is found in many different natural plant fibers: seed fibers (e.g., cotton and kapok), bast
pok), bast fibers (e.g., flax, hemp, jute, and ramie), leaf fibers (e.g., pineapple and sisal),
fibers (e.g., flax, hemp, jute, and ramie), leaf fibers (e.g., pineapple and sisal), fruit fibers
fruit fibers (e.g., coir), and grass and reed fibers (e.g., bamboo) [71]. In addition to cellu-
(e.g., coir), and grass and reed fibers (e.g., bamboo) [71]. In addition to cellulose, these fibers
lose, these fibers may contain traces of water, waxes, pectins, and fats [72]. Of the afore-
may contain traces of water, waxes, pectins, and fats [72]. Of the aforementioned plant
mentioned plant fibers, cotton is the most used, with a share of 22% of the global fiber
fibers, cotton
market in 2021,iswhile
the most used,
all other with afibers
natural sharecombined
of 22% ofhad theaglobal
share offiber market
6% [73]. in 2021, while
Worldwide,
all other natural fibers combined had a share of 6% [73]. Worldwide,
cotton is produced at approximately 25 million tons annually, utilizing 2.5% of the world’s cotton is produced at
approximately
arable land [74].25 million
After tons
cotton, annually,
flax, hemp, and utilizing 2.5%
jute are theof the common
most world’s arable land [74].
plant-based (cel- After
cotton, flax, hemp,
lulose) fibers [75]. and jute are the most common plant-based (cellulose) fibers [75].
Animal-basedfibers
Animal-based fibersareareprimarily
primarilycomposed
composed ofof collagen
collagen oror keratin,
keratin, proteins
proteins consisting
consist-
of amino
ing of aminoacid
acidunits
unitsthat
thatare
areconnected
connected by by peptide
peptidebondsbonds [70].
[70]. α-Keratin is theismain
α-Keratin the main
componentofofhair
component hairfibers
fibers(e.g.,
(e.g., wool,
wool, alpaca
alpaca wool,
wool, cashmere,
cashmere, mohair,
mohair, and angora
and angora wool),wool),
while β-keratins—chief among which is fibroin—are the main components of feather and
silk fibers (e.g., silk and spider silk). Collagen fibers are mostly found in mammalian skin
and tendons and are not used in conventional textile fibers but are the base material for
Polymers 2025, 17, 628 6 of 94

leather [76]. The most important animal-based fibers in the current textile industry are
sheep’s wool, camel hair, angora wool, and silk [75].
In general, the natural fibers of natural polymers have a low density and high crys-
tallinity, leading to a high specific strength and modulus. Due to their abundant supply,
and renewability in tandem with these mechanical properties, they are used from everyday
products, such as clothing, to more advanced products, such as fiber-reinforced polymer
composites. An important advantage of these natural fibers is that they are both biodegrad-
able and recyclable at the end of their lives via several recycling processes, except for those
that require high temperatures (e.g., melt re-extrusion) because natural polymers degrade
at such temperatures [77,78].

Natural Fibers of Non-Polymers

The only naturally occurring fibers of non-polymers are asbestos fibers. They are
composed of silicate groups that have fully crystallized into long, thin, fibrous crystals,
each comprised of even smaller fibrils [79]. There are six types of asbestos, split into
two groups: serpentine asbestos and amphibole asbestos [80,81]. Each type consists of
silicate (SiO2 ) and some other minerals in its chemical structure: aluminum oxide (Al2 O3 ),
ferric oxide (Fe2 O3 ), FeO, magnesium oxide (MgO), calcium oxide (CaO), and/or sodium
oxide [82].
Asbestos fibers have excellent fire resistance and thermal, electrical, and sound-
insulating properties, leading to their main use in the construction sector. However, as they
have been documented to cause mesothelioma (a type of cancer in the chest and abdominal
cavities) and asbestosis (lung scarring due to asbestos fiber inhalation) in people who work
with them, they have been banned in approximately 60 countries [83,84].
Asbestos fibers are non-biodegradable and can contaminate waters and the surround-
ing atmosphere if landfilled improperly. They can be mechanically recycled through heat
treatment at temperatures above 1000 ◦ C or through irradiation with microwaves, at which
point the hydrate silicate fibers turn into inert Mg-Fe silicate glass, which can be used for
the fabrication of traditional ceramic materials [82].
Man-made fibers derived from non-polymers, such as inorganic fibers or fibers made
from natural substances like cellulose, are increasingly being explored for various ap-
plications. These fibers can offer unique advantages, such as enhanced durability, heat
resistance, and biodegradability. They are commonly used in specialized fields like construc-
tion, automotive, and medical industries, where their specific properties—like strength, fire
resistance, and environmental friendliness—are highly valued. The applicability of these
fibers continues to grow as technology advances, offering new possibilities for sustainable
and functional materials [85].

2.1.2. Man-Made Fibers

Seventy percent of the fibers used globally do not occur in nature and are produced
industrially via melt or solution spinning processes [17]. The basic premise of fiber pro-
duction is that the polymer material must be liquefied in some way, either via melting
or dissolution, after which it can be processed into thin, elongated structures, thus form-
ing fibers [86]. These can be staple fibers with a short length similar to natural fibers or
filaments with an “infinite” length (limited only by stopping the spinning process).
Today, thermoplastic polymers are preferably processed via melt spinning over disso-
lution spinning because melt spinning processes typically yield higher spinning speeds
and do not require solvent separation or recovery [87]. For non-thermoplastic polymers,
solution spinning is a viable alternative, possibly after pretreatment steps, to allow for
suitable solubility for less soluble polymers (e.g., the rayon spinning process). Further
Polymers 2025, 17, 628 7 of 94

exceptions are the emulsion spinning process used for fluorocarbons or the production of
certain ceramic materials via a sacrificial polymer solution (e.g., cellulose), which is then
burned away, leaving only the sintered mass in fiber form [88].
Melt spinning typically starts with dried polymer chips melted continuously in screw
melters to yield a stable, pure, and homogeneous melt. Certain thermoplastic polymers,
such as polyester and polyamide, are synthesized in a molten state and can be processed im-
mediately after polymerization without the need to be turned into polymer chips first [89].
In any case, the polymer melt is pushed through the spinneret holes into a quench chamber,
in which air (or water) currents remove heat from the liquid protofibers to solidify them. In
addition, other melt-based technologies exist, such as centrifuge spinning (e.g., glass), split-
film spinning (e.g., polypropylene), melt electrospinning (e.g., polylactic acid), preform
drawing (e.g., glass), melt blowing (e.g., polypropylene), and spun bonding (e.g., polyethy-
lene terephthalate [PET]) [90].
The two main solution spinning techniques are dry and wet spinning (including gel
spinning). Both extrude a polymer solution through spinneret holes, after which the fiber is
formed through the solvent’s evaporation out of the protofiber through the application of
heat in a solidification chamber for dry spinning [87,91] or through the use of a coagulation
bath containing a non-solvent for wet spinning [87]. More specialized solvent spinning
techniques include solvent electrospinning, centrifuge spinning (e.g., polycaprolactone),
and flash spinning (e.g., polyethylene [PE]) [92].
It should be noted that the conventional melt and solution spinning processes include
a final shared step. During or after solidification of the protofibers, they are drawn to
several times their original length by a series of rolls that rotate at increasing speeds. This
aligns the crystalline sections of the fiber structures in a lengthwise direction to improve
the fibers’ mechanical properties. To ensure that this process happens smoothly, a finish
may be applied to the solidified fibers.

Man-Made Fibers of Natural Polymers

Some fibers do not occur in nature but do contain natural polymers. Chief among
these are MMCFs, which are created by processing cellulose-containing raw materials, such
as wood or cotton waste [93]. MMCFS can generally be categorized into two types: regen-
erated cellulose and cellulose esters (e.g., cellulose acetate and cellulose triacetate). The
primary category, commonly known as viscose, encompasses the majority of production.
These fibers are primarily produced using two industrially dominant technologies: the
viscose process, which involves the chemical modification of cellulose and its regenera-
tion, and the lyocell process, a direct dissolving process that does not require chemical
modification. Both technologies are employed to create fibers with different properties
and characteristics.
In general, the use of strong acids and bases during chemical treatments of MMCFs
reduces the average molar mass of cellulose, resulting in MMCFs with lower mechanical
properties compared to cotton. However, finishing processes, such as calendering [94],
sanforization [95], and coating [96], can partially compensate for these lower properties,
but cotton still provides higher quality [97–99].
Viscose is the most commonly used MMCF [100]. As it is made up of pure α-cellulose,
there are many hydroxyl groups on its surface. These functional groups are highly reactive
and have a strong interaction with a polar polymer matrix due to hydrogen (H2 ) bonding.
To manufacture viscose (Figure 4), wood pulp is first chemically converted into a
soluble compound to obtain pure cellulose. Then, aqueous sodium hydroxide (NaOH) is
used to form alkali cellulose and depolymerize cellulose to some extent. Carbon disulfide is
added to the alkali solution to form sodium cellulose xanthate. Finally, sulfuric acid (H2 SO4 )
Polymers 2025, 17, x FOR PEER REVIEW 8 of 104

Polymers 2025, 17, 628 8 of 94

used to form alkali cellulose and depolymerize cellulose to some extent. Carbon disulfide
is added to the alkali solution to form sodium cellulose xanthate. Finally, sulfuric acid
(His2SO
used
4) isto hydrolyze
used the alkali
to hydrolyze solution
the alkali and regenerate
solution cellulose
and regenerate and carbon
cellulose disulfide.
and carbon di- The
sulfide.
qualityThe qualitypulp,
of wood of wood pulp, theofamount
the amount of chemicals
chemicals used, theused,
(net) the (net)ofdegree
degree of de-
depolymerization,
polymerization,
and hydrolysisand hydrolysis
influence the influence
properties the
ofproperties of the final
the final product product [101,102].
[101,102].

Figure 4. The viscose production process [101,102].

Figure 4. The viscose production process [101,102].
Lyocell is a revolutionary technology for manufacturing MMCFs that involves a
sustainable
Lyocell isand environmentally
a revolutionary friendly
technology for process.
manufacturingAs shown MMCFs in Figure 5, the process
that involves a sus- starts
with dissolving
tainable cellulose, usually
and environmentally friendlyderived
process.from wood pulp,
As shown in Figurein a5,nontoxic solvent,
the process startssuch as
with dissolving cellulose,N-oxide
N-methylmorpholine usually derived
(NMMO) from wood
[103]. This pulp, in a nontoxic
solution solvent, such
is then extruded as fine
through
N-methylmorpholine
spinnerets to createN-oxide individual (NMMO) [103].These
filaments. This solution
filaments is then extruded
are washed andthrough
dried fineto remove
spinnerets to create
the solvent, individual
resulting in pure filaments.
celluloseThese filaments
fibers [104].are Thewashed
entireand dried to
process is remove
a closed-loop
the solvent, resulting in pure cellulose fibers [104]. The entire
system, in which the solvent is continuously recovered and reused, minimizing process is a closed-loop sys- waste
tem,
andinchemical
which the solvent is The
emissions. continuously
resultingrecovered
lyocell fibers and exhibit
reused, excellent
minimizing waste andsuch as
properties,
high strength, softness, moisture absorption, and breathability, making themas
chemical emissions. The resulting lyocell fibers exhibit excellent properties, such high for a
suitable
strength, softness, moisture absorption, and breathability, making them suitable for a
wide range of applications, including textiles, apparel, and nonwoven products. Moreover,
wide range of applications, including textiles, apparel, and nonwoven products. Moreo-
lyocell is considered a sustainable choice due to its renewable raw material source, low
ver, lyocell is considered a sustainable choice due to its renewable raw material source,
environmental impact, and biodegradability [105].
low environmental impact, and biodegradability [105].
Besides cellulose, there is another natural polysaccharide used to make man-made
Besides cellulose, there is another natural polysaccharide used to make man-made
textile fibers: chitin and its derivative, chitosan. These polymers are very similar in structure
textile fibers: chitin and its derivative, chitosan. These polymers are very similar in struc-
to cellulose,
ture to cellulose,butbuttheir
theirglucose
glucosemonomers
monomers are are slightly
slightlydifferent.
different.For For chitosan,
chitosan, thetheglu-glucose
molecule has an amine functional group (glucosamine), and
cose molecule has an amine functional group (glucosamine), and for chitin, this glucosa- for chitin, this glucosamine has
an additional
mine acetyl group
has an additional acetylattached to the amine
group attached to thegroup
amine(acetylglucosamine)
group (acetylglucosamine) [106]. Chitin’s
biological function is also similar to that of cellulose, making
[106]. Chitin’s biological function is also similar to that of cellulose, making up the cell up the cell walls of many
living
walls organisms.
of many living In this case,Initthis
organisms. is not
case, found in plants
it is not found in but in fungi
plants but in and theand
fungi exoskeletons
the
of certain animals, such as insects and arthropods. Chitosan
exoskeletons of certain animals, such as insects and arthropods. Chitosan fibers are made fibers are made through the
deacetylation
through of chitin of
the deacetylation with a strong
chitin with a alkali
strong (e.g.,
alkaliNaOH)
(e.g., NaOH)at high temperatures,
at high temperatures, and then
and then dissolving
dissolving the chitosan
the chitosan in an acidicin ansolvent,
acidic solvent,
typically typically
acetic acidacetic(CH acid
3 (CH₃COOH),
COOH), which can be
which can be wet spun into a coagulation bath of NaOH or ethanol
wet spun into a coagulation bath of NaOH or ethanol (EtOH) [107]. Despite the potential (EtOH) [107]. Despite
the
forpotential for their applications
their applications in the textile in industry,
the textilechitin
industry, andchitin
chitosanandrepresent
chitosan represent
less than 1% of
less than 1% of the total fiber market, with use only in medical and
the total fiber market, with use only in medical and specialty applications due to their specialty applications
due to their biodegradable
biodegradable and antimicrobial
and antimicrobial properties properties
[108]. [108].
Polymers 2025, 17, 628 9 of 94

Figure 5. The lyocell production process [109].

Man-Made Fibers of Synthetic Polymers

Synthetic polymers result from chemically converting monomers, oligomers, or poly-
mers that occur in nature or are in turn produced from a petroleum (or alternative) base.
Overall, there are two types of polymer synthesis: chain-growth polymerization and
step-growth polymerization [110].
Figure 6 displays examples of the overall reaction of various polymerization pro-
cesses. Chain-growth polymerization [111–113] is used to produce vinyl polymers, such
as PE, polypropylene (PP), PMMA, butadiene rubber (BR) polymer, and acrylic polymers,
Polymers 2025, 17, x FOR PEER REVIEW 10 of 104
while step-growth polymerization [114,115] is used for polymers, such as PET (in general
polyesters), polyamide, and PU.

Figure 6. Overall reaction for important polymerizations. The targeted polymer is listed above the
Figure 6. Overall reaction for important polymerizations. The targeted polymer is listed above the
arrow for clarity [111,112,114].
arrow for clarity [111,112,114].

Polyesters
Linear polyesters are manufactured from the condensation polymerization of a bi-
functional carboxylic acid with a bifunctional alcohol [124]. PET is the dominant polyester
Polymers 2025, 17, 628 10 of 94

The diverse characteristics of polymers have led to their widespread use in the textile
industry, ranging from (poly)acrylic fibers (primarily composed of copolymers of acry-
lonitrile and other vinyl monomers, such as vinyl chloride) [116] to polyolefin fibers [117],
synthetic leather made from polyvinyl chloride (PVC) [118], foam made from PU [119],
and rubbers used as adhesives [120]. Additionally, polyvinyl acetate (PVAc) and polyvinyl
alcohol (PVA) have been utilized as reinforcement fibers and adhesives [121–123].
In the following sections, a more detailed description of PET and polyamide fiber
synthesis is provided.
Polyesters
Linear polyesters are manufactured from the condensation polymerization of a bi-
functional carboxylic acid with a bifunctional alcohol [124]. PET is the dominant polyester
utilized in the textile industry (and for bottle grades), whereas other polyesters are limited
to specific applications [125–127]. The main features of the important polyesters are shown
in Table 1. The chemical structures of polyesters primarily affect their melting temper-
ature (Tm ) and glass transition temperature (Tg ), with a structure that corresponds to a
higher Tm leading to physical properties such as thermal and mechanical stability, while a
structure that yields a lower Tg results in increased flexibility and softness [125,128,129].
Semi-crystalline engineering plastics, such as PE, can be oriented and self-crystallized
during extrusion, resulting in enhanced superior physical and mechanical properties.
The three main stages involved in PET polymerization are depicted as the first three
entries in Figure 7. This polymerization initially involves (trans)esterification. For example,
esterification between terephthalic acid (TPA) and ethylene glycol (EG) takes place at a high
temperature and pressure (360 ◦ C, 4 bar). To prevent reverse reactions, methanol (CH3 OH)
is removed. Bis(2-hydroxyethyl terephthalate) (BHET) is generated, and it serves as the
oligomer for the second stage, which takes place catalytically (usually through the presence
of antimony trioxide [Sb2 O3 ]) at a moderate temperature and low pressure (270 ◦ C, 6.5 kPa).
Subsequently, the average molar mass is increased to the commercial polymer grade in the
Polymers 2025, 17, x FOR PEER REVIEW 11 of 104
third stage, which is carried out under high vacuum conditions that release H2 O, EG, and
light oligomers (290 ◦ C, 0.65 kPa).

Figure 7.
Figure 7. The
The industrial
industrialpolymerization
polymerizationand structure
and of PET
structure [130,131].
of PET [130,131].

complementary extra
A complementary extrastage
stage(the fourth
(the entry
fourth in Figure
entry 7) is7)called
in Figure solid-state
is called poly-poly-
solid-state
condensation (SSP). Through this process, Sb O remains in the final product,
condensation (SSP). Through this process, Sb2 O3 remains in the final product, and PET
2 3 and PET may
may contain
contain around
around 170–300
170–300 mg/kgmg/kg antimony
antimony (Sb)
(Sb) as as well
well asas othermetals,
other metals,such
suchas
ascobalt
cobalt (Co),
(Co), iron (Fe), manganese (Mn), and chromium (Cr). Similarly, liquid-state
iron (Fe), manganese (Mn), and chromium (Cr). Similarly, liquid-state polycondensation polyconden-
sationinvolves
(LSP) (LSP) involves the removal
the removal of by-products
of by-products at high
at high temperatures
temperatures during
during thethe melting
melting of PET.
of PET. By using LSP, high-performance PET fibers can be produced directly from the
melt, without the need for a spinning process. During both the SSP and LSP processes, the
average molar mass can be kept within the desired range by adjusting the pressure, tem-
perature, and catalyst type and amount [130,131].
Intrinsic viscosity (IV) is commonly used as a means of characterizing PET, which
 A7.
Figure
Figure 7.complementary
The industrial
The extra stage (the
industrial polymerization
polymerization andfourth
and entry
structure
structure in Figure
of PET
of PET 7) is called solid-state poly-
[130,131].
[130,131].
condensation
A complementary (SSP). Through
extra stage this (the
process,
fourth Sbentry
2O3 remains
in Figure in 7)theis final
calledproduct,
solid-stateandpoly-PET
may AA complementary
complementary
contain around extra
extra
170–300 stage
stage
mg/kg (the
(the fourth
fourth
antimony entry
entry
(Sb) in
in
as
condensation (SSP). Through this process, Sb2O3 remains in the final product, and PETFigure
Figure
well as 7)
7) is
is
other called
called
metals, solid-state
solid-state
such as poly-
poly-
cobalt
Polymers 2025, 17, 628 condensation
condensation
(Co),contain
may iron (Fe), (SSP).
(SSP). Through
Through
manganese
around 170–300 (Mn),thisand
this
mg/kg process,
process,
chromium
antimony Sb22(Sb)
Sb OO33(Cr).
remains
remains in other
in
Similarly,
as well as theliquid-state
the final
final product,
product,
metals, such and
and
polyconden-
as PET
PET
cobalt 11 of 94
may
may
sation
(Co), contain
contain
(LSP)
iron (Fe), around
around
involves 170–300
170–300
the removal
manganese (Mn),mg/kg
mg/kgand antimony
of antimony
by-products
chromium (Sb)
(Sb) as
atas
high
(Cr). well
well as other
as other
temperatures
Similarly, metals,
metals,
during
liquid-state such
such as cobalt
theasmelting
cobalt
polyconden-
(Co),
(Co),
of PET.
sation iron
iron
(LSP) (Fe),
By(Fe),
using manganese
manganese
involves LSP, (Mn), and
(Mn),
thehigh-performance
removal and chromium
chromium
of by-productsPET fibers(Cr).
(Cr).
at high Similarly,
Similarly,
can be produced
temperatures liquid-state
liquid-state
during polyconden-
polyconden-
directly
thefrom
melting the
sation
By using
sation
melt, (LSP)
LSP,
(LSP)
without involves
involves
the need the
high-performance
the forremoval
removal
a spinningof
PET
of by-products
fibers
by-products
process. can be
During at
at high
high
of PET. By using LSP, high-performance PET fibers can be produced directly from the temperatures
produced directly
temperatures
both the SSP and during
from
during
LSP thethe
the melting
melt,
melting
processes, without
the
of
the
of PET.
need
PET.
average
melt, By
for
By using
a
using
molarthe
without massLSP,
spinning
LSP,
needcan high-performance
process. During
high-performance
forbea spinning
kept within PET
both
PET fibers
the SSP
fibers
the desired
process. Duringrange can
and
can be
be
both by LSPproduced
processes,
produced
theadjusting
SSP and LSP directly
the
directly from
average
from
the pressure,
processes,tem- the
themolar
the
melt,
melt,
mass
average without
without
canmolar
perature, be
andkeptthe
the need
need
within
catalyst
mass can for
for
type a
beathespinning
spinning
and
kept desired
amount
within process.
process.
range During
During
by adjusting
[130,131].
the desired both
bothby
range the
the the SSP
SSP and
and LSP
pressure,
adjusting LSP processes,
processes,tem-
temperature,
the pressure, the and
the
average
average
catalyst molar
molar
Intrinsic
perature, type
andand mass
mass
viscositycan
can
amount
catalyst be[130,131].
be
(IV)
type kept
kept
and within the
within
is commonly
amount theused
desired
desired
[130,131]. range
as arange
means byofadjusting
by adjusting the pressure,
the
characterizing pressure,
PET, which tem-
tem-
perature,
perature,
provides
Intrinsic
Intrinsic and
and
indirectcatalyst
catalyst
viscosity
viscosity type
type
information and
and amount
amount
on
(IV)isiscommonly
(IV) commonly [130,131].
[130,131].
the average used
used molar
as as amass
a means meansand configuration
of characterizing
of characterizing of the
PET, PET,poly-
which which
Intrinsic
mer.Intrinsic
provides
provides Typically,
indirect
indirect viscosity
viscosity
PET (IV) is
(IV)
polymers
information
information is commonly
commonly
with
on
on the
thea higher used
used
average
average as aa means
as
average
molar
molar means
molar
mass
massand of characterizing
of
mass
and characterizing
exhibit higher
configuration
configuration PET,
PET,
of IV
ofthe which
which
values.
the poly-
polymer.
provides
provides
PET Typically,
mer. indirect
fiberindirect
and bottle
PET information
information
grades
polymers on the
on the
generally
with average
average
have
a higher IV molarmolar
molar
values
average mass
mass
rangingand
and
mass configuration
configuration
from 0.57higher
exhibit to 0.62
higher ofIV
of the
the
dL·g poly-
poly-
−1 and PET
values.
Typically, PET polymers with a higher average molar mass exhibit IV values.
mer.
mer.
from Typically,
Typically,
0.72
PET fiber to 0.85
and bottlePET
PET
dL·gpolymers
polymers with
with
−1, respectively
grades generally a
a higher
higher
[132,133].average
average molar
molar mass
mass exhibit
exhibit higher
higher IV
IV −values.
values.
fiber and bottle grades generally havehave IV values
IV values ranging
ranging from from0.57 0.57
to to
0.620.62
dLdL·g
·g and1−1 andfrom
PET fiber
PET
from fiber
0.72 and
and
to bottle
bottle
0.85 dL·g
− 1 grades
grades generally[132,133].
generally
−1, respectively have IV
have IV values
values ranging
ranging from from 0.57 0.57 to
to 0.62
0.62 dL·g
dL·g−1−1 and
and
0.72 to 0.85 dL·g , respectively [132,133].
from
from 0.72
Table0.72 to 0.85
to
1. Different 0.85 types
dL·g of,, respectively
dL·g −1
−1 respectively
polyesters used [132,133].
[132,133].
in textile and manufacturing applications [125,128,129].

Polyester Full Name Table1.

Table 1. Different
DifferentStructure
types
types of
ofpolyesters
polyestersused usedinintextile
textile
T and
m (°C) and1manufacturing
Tmanufacturing
g (°C) 2
applications
applications
Assets [125,128,129].
[125,128,129].
Ref.
Table 1.
Table 1. Different
Different O
types
types of
of polyesters
polyesters
O
used
used in
in textile
textile and
and manufacturing
manufacturing applications
applications [125,128,129].
[125,128,129].
Polyester Polyethylene
Full Nameter- Structure Tm1 (°C) T◦g (°C)
1 2 A common Assetstype of Ref.
PET
Polyester Full Name Structure Tm (◦ C) 250–265 (Tg70–80
2 Assets [134]Ref.
Polyester Polyethylene
Polyester Full
Full Name
Name
ephthalate ter-
( O Structure
O Structure OO )n T (°C)T1g1 T
Tmm (°C) gC)
(°C) 22 A common
(°C) Assets
Assets
polyester type of Ref. Ref.
PET Polyethylene
Polyethylene
Polytri- ter-
ter-
Polyethylene ( OO
O
O
OOO
)n 250–265 70–80 A common
A common
Apolyester
common type
type typeof
of [134]
PET
PET
PET ephthalate O
250–265 250–26570–80
250–265 70–80 Superior
70–80 [134][134]
terephthalate (( OO OO ))nn of softness [134]
polyester
PTT ephthalate
ephthalate
methylene
Polytri- ter- ( O O OO )n 220–230 30–40 polyester
polyester [135]
and drape
Superior softness
PTT Polytri-
Polytri-
ephthalate
methylene ter- O O 220–230 30–40 Superior
Polytrimethylene ( O
O O
O )n Superior
Superior
and drape softness [135]
softness
softness
PTT
PTT
PTT methylene
methylene ter-
ter- 220–230 220–23030–40
220–230 30–40 Good
30–40 mechanical [135][135]
[135]
ephthalate
terephthalate (( OO O
O ))nn and
and drape drape
drape
O O and
ephthalate
ephthalate
Polybutylene properties and re-
PBT ( OO OO )n
225–235 50–60 Good Good
mechanical
mechanical [136]
terephthalate
Polybutylene
Polybutylene Good
sistance
Good
properties mechanical
to chemi-
mechanical
and re-
PBT
PBT OO OO 225–235 225–235 50–60 50–60 properties properties and [136] [136]
Polybutylene
Polybutylene
terephthalate
terephthalate ( O O )n properties
sistance cals and re-
totoand
chemi- re-
PBT
PBT ( O )
225–235
225–235 50–60
50–60 resistance [136]
chemicals[136]
terephthalate
terephthalate
Poly(1,4-cyclo- ( O
O O ) nn sistance
sistance to
to chemi-
chemi-
Polymers 2025, 17, x FOR PEER REVIEW High cals and 12 of 104
stretch
Poly(1,4-cyclohexylene- O O cals
hexylene-di- )n Highcals stretch and
PCDT2025,Poly(1,4-cyclo-
PCDT
Polymers dimethylene
17, x FOR PEER REVIEW O O
255–270 255–27060–70 60–70 High recovery stretchproper-
and 12 [137]
of [137]
104
Poly(1,4-cyclo-
methylene
Poly(1,4-cyclo-
hexylene-di- ter- ( O O
)n recovery properties
PCDT2025, 17, terephthalate) OO OO High
High
255–270 60–70 recovery proper- 12 stretch
ties
stretch and
and [137]
Polymers x FOR PEER REVIEW
hexylene-di-
ephthalate)
hexylene-di- ( OO O ))nn of 104
PCDT2025, methylene
Polymers
PCDT 17, x FOR PEERter-
REVIEW 255–270
255–270 60–70
60–70 recovery
recovery
High
High proper-
proper-
strength,
ties
temperature [137]
12 of 104
[137]
methylene
methylene
Polybutylene ter-
ter-
Polyethylene
ephthalate) (( OO O
O O High temperature
PEN
PBN ( OO O 260–275 250–265 120–140
55–65 resistance
stiffness, ties
tiesand ther-
and excellent[139][138]
ephthalate)
naphthalate
ephthalate)
Polyethylene
naphthalate OOO )n High High
resistance strength,
and
temperature ex-
PEN Polybutylene ( O O 260–275 120–140 dimensional
mal stability stability [138]
PBN naphthalate
Polyethylene ( OO O
O )n 250–265 55–65 stiffness,
High
High cellent
High
resistance and
temperature
dimen-
temperature
strength, ther-
and ex- [139]
PEN naphthalate
Polybutylene ( O
O
OO
OO ) n 260–275 120–140 A biodegradable
High strength, [138]
PBN Polyethylene
Polyethylene
Polybutylene
naphthalate
Polybutylene ( OO OO
O
O )n 250–265 55–65 High mal
resistance
resistance
sional
stiffness,
cellent stability
andther-
and
stability
and
dimen-
strength, ex- [139]
ex-
stiffness,
PEN
PEN
PBN
PBN naphthalate ((( O O ) 250–265 260–275
260–275
250–26555–65 120–140
120–140 polyester
55–65 stiffness, ther- [138]
derived
and [138]
[139][139]
OO A biodegradable
naphthalate
naphthalate
naphthalate
naphthalate O )))nnn cellent
cellent
andmal dimen-
dimen-
stability
thermal
sional stability stability
O n
( O from malrenewable
polyester stability re-
derived [140]
PLA Polylactic acid )
n 130–180 50–65 A sional
sional stability
stability
biodegradable
O O Asources,
from A such asre-
biodegradable
biodegradable
renewable
PLA Polylactic acid ( ) 130–180 50–65 polyester polyester derived
n cornstarch
polyester
sources, and
derived
derived
such as from[140]
(
OO from renewable re-
PLA
PLA Polylactic
Polylactic acidacid ) 130–180 130–18050–65 50–65 from renewable
sugarcane
renewable resources,
re- [140][140]
PLA Polylactic acid ( O O )n 130–180 50–65 sources, cornstarch such andas [140]
Polyethylene n such
sources, as cornstarch
such as
O
Less sugarcane
cornstarch
shrinkage
and sugarcane and for
PETG Tere-phthalate
Polyethylene 230–260 80–95 cornstarch and [141]
Less sugarcane
printed
shrinkageparts
Polyethylene
Glycol Less shrinkagefor
sugarcane for
PETG
PETG Tere-phthalate
Polyethylene Glycol 230–260230–26080–95 80–95 [141][141]
Tere-phthalate
Polyethylene 1 Tm, melting temperature of the bulk polymer; 2 Tg, glass transition temperature Less printed
printed
shrinkage parts
parts
of the for
bulk polymer.
PETG Glycol
Tere-phthalate 1 230–260 80–95 Less shrinkage for [141]
PETG Tere-phthalate T1 T , melting temperature of the bulk polymer; 2 T2g230–260 80–95 printed parts [141]
Glycol mm , melting temperature of the bulk polymer; ,Tglass transition temperature
g, glass transition temperature
of the
printed of
bulk polymer.
the bulk polymer.
parts
Glycol Polyamides
1 Tm, melting temperature of the bulk polymer; 2 Tg, glass transition temperature of the bulk polymer.
1 Tm, melting temperature of the bulk polymer; 2 Tg, glass transition temperature of the bulk polymer.
Linear polyamide, also known as nylon, is a synthetic polymer formed through the
Polyamides
Polyamides
condensation
Polyamides polymerization
Linear polyamide,
polyamide, also of a bifunctionalisamine and carboxylic acid. Polyamide fi-
Linear
Polyamides also known
knownasasnylon, nylon, isa asynthetic
synthetic polymer
polymer formed
formed through
through the the
bers are highly
condensation valued
polymerizationfor their resilience,
of aa bifunctional
bifunctional durability,
amine and strength,
and carboxylic
carboxylic as well
acid. as for their
Linear polyamide,
condensation polymerization also known of as nylon, isamine a synthetic
and polymer formed acid. Polyamide
through the
Polyamide fi-
fibers
bers Linear
flexibility topolyamide,
are highly
condensation valued also
be molded
polymerization
into known
various
for their as
of aresilience,
nylon,durability,
shapes
bifunctional
is a synthetic
[142,143].
amine
Ifand
and
polymer
strength,formed
a monomer
carboxylic
containing
as well
acid.
through
as two
Polyamide
the
car-
for their fi-
are highly valued for their resilience, durability, and strength, as well as for their flexibility
condensation
boxyl and amine
flexibility to be polymerization
functions
molded into of a bifunctional
is utilized,
various the resulting
shapes amine
[142,143]. and
polymerIf a carboxylic acid. where
is labeled containing
monomer PAx, Polyamide x is car-
two fi-
the
bers
to are
be are highly
molded valued
into variousfor their
shapes resilience,
[142,143]. durability,
If aif monomerand strength,
containing as well as for
twoascarboxyl their and
bers
number
boxyl andtohighly
of carbons
amine valued
in the
functionsfor their
monomer. resilience,
Conversely,durability, two and strength,
separate units as well
consisting for
of their
a bi-
flexibility
amine functionsbe molded
is intoisvarious
utilized,
utilized,shapes
the resulting
the resulting
[142,143].
polymer
polymer
is
is labeledcontaining
a monomer
Iflabeled PAx,
PAx, where
where x is twox iscar-
the
the
number
flexibility
functional
number to be molded
amine into
andinbifunctional various shapes
carboxyl are[142,143].
used, a monomer
theIfpolyamide containing
is called PAx,y, twowherecar-
boxyl
of andofamine
carbons in
carbons
the
the
functions
monomer.
monomer.
is utilized,
Conversely,
Conversely,
the resulting
if two
ifpolymer
two
separate
separate units
is labeled
units
consisting
PAx,
consisting where
of a xofisathebi-
bifunctional
xboxyl
and y and
functional amine
indicate
amine functions
the
andnumber isof
bifunctional utilized,
carbons the
carboxylin resulting
theareamine
used, polymer
and
the is labeled
carboxyl
polyamide units,
is PAx, where
respectively
called PAx,y, xwhere
is(Fig-
the
number of carbons in the monomer. Conversely, if two separate units consisting of a bi-
amine 8).and
number of bifunctional
carbons in thecarboxyl
monomer. areConversely,
used, the polyamide
if two separate is called PAx,y, where xbi-
and y
ure
x and
functionaly indicate
aminethe andnumber
bifunctional of carbons
carboxyl in the
areamine
used, the carboxylunits
andpolyamide units, consisting
respectively
is called
of a(Fig-
PAx,y, where
indicate An the
functional number
amine
important and of carbonsisinPA6,6,
bifunctional
polyamide the amine
carboxyl are and
whose used, carboxyl
the polyamide
synthesis units, is
involves respectively
called
two PAx,y,
stages. (Figure
where8).
Initially,
xureand8).y indicate the number of carbons in the amine and carboxyl units, respectively (Fig-
x and y indicate
adipic acid and hexamethylene diamine are combined in an aqueous medium at a (Fig-
the number of carbons in the amine and carboxyl units, respectively high
ure 8).An important polyamide is PA6,6, whose synthesis involves two stages. Initially,
ure 8).
temperature
adipic and pressure (254 °C, 18 bar) for pre-polymerization. Subsequently, the
Anacid and hexamethylene
important polyamide isdiamine PA6,6, whose are combinedsynthesis in involves
an aqueous twomedium
stages. at a high
Initially,
An
temperatureimportant
polymerization and polyamide
process is sustained
pressure (254diamineis PA6,6,
through
°C, 18 bar) whose melt synthesis
polycondensationinvolves
for pre-polymerization. two
at a stages.
high Initially,
temperature
Subsequently, the
adipic acid and hexamethylene are combined in an aqueous medium at a high
adipic
(267 °C)acid
andand
polymerization hexamethylene
atmospheric
process is pressure
sustained diamine
tothrough
attainarean combined
meltaverage in an aqueous
molar
polycondensation weightatwithinmedium
a high the at a high
commer-
temperature
temperature and pressure (254 °C, 18 bar) for pre-polymerization. Subsequently, the
temperature
cial
(267range
°C) and andTo
[130]. pressure
atmosphericachieve (254
higher
pressure °C,toaverage
18 bar)an
attain for
molar pre-polymerization.
averagemasses,molar it weight
is essential Subsequently,
to the
remove the
by-
polymerization process is sustained through melt polycondensation at within commer-
a high temperature
polymerization
products
cial °C)
range from process
the reactoris sustained
through through
the LSP melt
and/or polycondensation
SSP process, whichat a high
helps temperature
prevent the
(267 and[130]. To achieve
atmospheric highertoaverage
pressure attain anmolar average masses,
molaritweight is essential
withintothe remove
commer- by-
(267
kinetic°C)relevance
products and
from atmospheric
ofreactor
the pressure
reversibility
through and tothe
attain an
depolymerization
LSP average
and/or SSP molar
reactions.
process, weight
which within
helps the commer-
prevent the
cial range [130]. To achieve higher average molar masses, it is essential to remove by-
cial range
kinetic [130]. To
Therelevance
various types
of achieve higher
of polyamides
reversibility and average
possessmolar unique
depolymerization masses,
properties it is and
reactions. essential to remove
applications. For by-in-
products from the reactor through the LSP and/or SSP process, which helps prevent the
products
stance, The fromisthe
PA6,6
various reactor
commonly
types through
used in the
of polyamides fiber LSP and/or
production,
possess unique SSP process,
while
propertiesPA6 is which helps prevent
frequently utilized the for
kinetic relevance of reversibility and depolymerization reactions.and applications. For in-
kinetic
injection relevance
molding of reversibility
and less often and
as depolymerization
fibers (e.g., fishing reactions.
nets)
stance, PA6,6 is commonly used in fiber production, while PA6 is frequently utilized for [144].
 products from the reactor through the LSP and/or SSP process, which helps prevent the
kinetic relevance of reversibility and depolymerization reactions.
Polymers 2025, 17, 628
The various types of polyamides possess unique properties and applications. For in-
12 of 94
stance, PA6,6 is commonly used in fiber production, while PA6 is frequently utilized for
injection molding and less often as fibers (e.g., fishing nets) [144].

Figure PA6,6 vs.

Figure 8. PA6,6 vs.PA6.
PA6.

An important
Man-Made Fibers of polyamide
Non-Polymersis PA6,6, whose synthesis involves two stages. Initially,
adipic acid and hexamethylene diamine are that
There are four categories of non-polymers combined
are commonin an in
aqueous
man-mademedium
fibers: at a high
car-
temperature and pressure ◦
(254AllC,of 18 bar) for pre-polymerization.
bon, glass, ceramics, and metals. these building blocks are inorganic,Subsequently,
although car- the
polymerization
bon and several process is sustained through
ceramic non-polymer structuresmelt polycondensation
(e.g., at often
silicon carbide) are a high temperature
produced
(267 ◦ C) and atmospheric pressure to attain an average molar weight within the commercial
from organic polymers [145–147].
range [130]. To achieve higher average molar masses, it is essential to remove by-products
from the reactor through the LSP and/or SSP process, which helps prevent the kinetic
relevance of reversibility and depolymerization reactions.
The various types of polyamides possess unique properties and applications. For
instance, PA6,6 is commonly used in fiber production, while PA6 is frequently utilized for
injection molding and less often as fibers (e.g., fishing nets) [144].

Man-Made Fibers of Non-Polymers

There are four categories of non-polymers that are common in man-made fibers:
carbon, glass, ceramics, and metals. All of these building blocks are inorganic, although
carbon and several ceramic non-polymer structures (e.g., silicon carbide) are often produced
from organic polymers [145–147].
Carbon fiber, at its chemical structure level, very similar to graphite, is composed almost
entirely of carbon atoms in a regular hexagonal pattern [148,149]. It is a lightweight, high-
strength material composed of carbon atoms bonded together in a crystalline structure,
offering exceptional mechanical properties. Its engineering applications span the aerospace,
automotive, sporting goods, and renewable energy sectors due to its strength-to-weight ratio.
It is manufactured by converting precursor materials, such as polyacrylonitrile (PAN) fibers
or pitch, into carbon fibers through processes such as oxidation and carbonization [150,151].
Glass fiber, also known as fiberglass, is a versatile engineering material composed
of fine fibers made from glass. It exhibits excellent strength, durability, and resistance to
heat and corrosion, making it ideal for various applications [152]. While some would call
glass an inorganic cross-linked polymer, it is not classified as such due to the inability to
distinguish individual polymer chains in the silica network [145–147].

2.2. Blended Fiber Textiles

Blended fiber textiles are made of yarns composed of two or more different types
of fibers (so-called combination yarns) or of two or more different yarns of a single fiber
type each (creating a so-called mixed fabric). This blending offers unique properties and
advantages that are not found in individual fibers alone [153,154]. Several examples of
blended textiles are given below. For example, the polyester–cotton blend is one of the
most common and popular mixed textile combinations. The resulting fabric combines the
softness and breathability of cotton with the durability and wrinkle resistance of polyester.
It is commonly used in various garments, including shirts, trousers, and bedsheets [155,156].
Furthermore, a wool–synthetic blend is a blended wool with synthetic fibers, such as
polyamide or polyester, creating a fabric that combines the warmth, softness, and moisture-
Polymers 2025, 17, 628 13 of 94

wicking properties of wool with the strength, durability, and quick-drying characteristics of
synthetics. This blend is often used in outdoor clothing, such as jackets and sweaters [157].
The silk–linen blend is known for its strength and breathability. This combination
results in a fabric that has a luxurious feel, good moisture absorption, and improved
durability. It is commonly used in dresses, scarves, and home furnishings [158].
A viscose–polyester blend is used to create a fabric that combines the comfort, drape,
and moisture absorption of viscose with the durability and wrinkle resistance of polyester.
This blend is often used in dresses, skirts, and blouses [159,160].
In addition, an acrylic–wool blend is employed to create a fabric that retains the
warmth, softness, and insulating properties of wool while reducing its cost and enhancing
its resistance to shrinkage and stretching. This blend is commonly used in knitwear,
blankets, and accessories [161].
The foregoing are just a few examples of blended fiber textiles. Numerous other com-
binations are available, depending on the desired properties and application of the fabric.
The blending of textiles allows manufacturers to create fabrics that offer a combination of
desirable characteristics from different types of fibers [162].
Furthermore, in the textile industry, various additives are used to enhance the per-
formance, appearance, and functionality of fabrics. These additives can be added during
the manufacturing process or applied as a finishing treatment [163]. They include dyes
and pigments [164], flame retardants [165], antimicrobial agents [166], UV stabilizers [167],
softeners [168], water repellents [169], and antistatic agents [170].
The recycling of mixed fibers and additives in the textile industry poses several
challenges, such as fiber separation, contamination by including different additives, loss
of performance during the recycling process, lack of infrastructure, limited demand for
recycled mixed fibers, and lack of standardization [162,171–174].

2.3. Fabrics
Fabric manufacturing encompasses various methods, including weaving, knitting,
braiding, and nonwoven techniques, each yielding distinct textile structures. Woven
fabrics are created by interlacing two sets of yarns (warp and weft) at right angles on a
loom, forming a stable and structured material, such as cotton, silk, or polyester. Knitting
involves interloping yarns to produce flexible and stretchable fabrics, such as sweaters or
socks [175–178].
Braiding combines yarns in a diagonal pattern, resulting in the strong and tubular
structures used in ropes or cables. Nonwoven fabrics are made by bonding fibers together
mechanically, chemically, or thermally, producing materials such as felt or geotextiles. Each
production method offers unique characteristics in terms of texture, strength, and suitability
for various applications in the fashion, industrial, and technical sectors [179,180].

2.4. Textile Products

Textile products encompass a broad array of goods that serve both practical and
aesthetic purposes in everyday life and industrial settings. Apparel, ranging from clothing
items to accessories such as hats and footwear, represents a substantial segment of the
textile market [181].
Home textiles, including bedding, towels, curtains, and upholstery fabrics, are es-
sential for furnishing and decorating living spaces. Technical textiles play vital roles in
industries such as automotive, medical, and construction, providing functional solutions,
such as airbags, medical textiles, and geotextiles [182].
Sports and outdoor textiles cater to the demands of active lifestyles, with specialized
clothing and gear designed for performance and comfort. Industrial textiles serve various
Polymers 2025, 17, 628 14 of 94

industrial applications, including filtration, reinforcement, and packaging, contributing to

the efficiency and safety of industrial processes [183].
Industrial textiles include specialized fabrics used in applications such as geotextiles,
filtration, protective clothing, automotive components, medical devices, aerospace, and
construction materials [184].
The diverse applications and versatility of textile products underscore their importance
across different sectors and consumer needs [185].

3. End-of-Life Options for Textile Waste

The International Organization for Standardization (ISO) presents the overall envi-
ronmental aspects of textiles in ISO 5157:2023. It states that the end-of-life stage of textile
materials “begins when the used product is ready for disposal, recycling, reuse, etc., and
ends when the product is returned to nature (combustion, deterioration), or is recycled or
reused” [186]. Before reuse, recycling, or returning to nature can occur, textile waste must
be collected and sorted—both at the household and industrial levels—which involves the
challenging yet crucial step of separating textiles from other waste fractions. Currently,
textile waste is mainly sorted manually, although the use of automated sorting techniques
is gaining traction [34,187].
Reuse signifies recovering a product as a whole rather than disassembling it into
materials. This product can be lightly damaged and undergo minor reparations as long as
it is restored to a usable state, as intended by its original design [186].
Recycling is performed when the product itself cannot be restored but the materials
that make up the product can be recovered for use in a new product, usually after some form
of pretreatment. As most textile waste consists of polymer materials, ISO 472:2013—the
standard on plastics vocabulary—can be consulted for terminology purposes. This standard
categorizes recycling methods based on whether changes occur in the chemical structure of
the building blocks during the recycling process. It recognizes two categories: mechanical
recycling, during which the chemical structure of the material does not significantly change;
and chemical recycling, during which the chemical structure of the material significantly
changes, such as polymers that are converted into monomers or oligomers [188].
Note that the textile-specific standard ISO 5157:2023 instead categorizes recycling
methods based on the process used and has three categories: mechanical, thermomechan-
ical, and chemical recycling [186]. In this review, a broader plastic vocabulary is used.
The thermomechanical recycling processes that involve melting polymers mentioned in
ISO 5157:2023 then become a subset of mechanical recycling.
Alternatively, recycling can be categorized by the level to which the waste textiles
are degraded before they are turned into new products (i.e., fabric, yarn, fiber, polymer,
oligomer, or monomer) [189]. Fabric, yarn, fiber, and polymer recycling all employ me-
chanical recycling techniques, while oligomer and monomer recycling employ chemical
recycling techniques [190].
Another classification is that of primary, secondary, tertiary, or quaternary recycling,
which is used by the American Society for Testing and Materials in definition D5033 [191].
Here, primary recycling indicates a process whereby recycled materials (also called sec-
ondary raw materials) are used to create a product identical to the original product (before
it became waste). Secondary recycling turns product waste into a new product that is not
directly related to the original product. Tertiary recycling turns waste into basic chemicals
or fuels. Quaternary recycling turns waste into heat [192]. The latter is another name for
incineration or combustion and does not conserve any materials; thus, it is incorrect to call
it recycling and should instead fall under “returning to nature” in ISO 5157:2023. Directive
2008/122/EC of the European Parliament and of the Council also states that “recycling [. . .]
Polymers 2025, 17, 628 15 of 94

does not include energy recovery and the reprocessing into materials that are to be used as
fuels or for backfilling operations” [193]. This clearly demarcates the border between what
ISO 5157:2023 considers recycling and what it considers “returning to nature”, the latter
being any process that recovers only energy or fuels but not materials, or where nothing is
recovered at all (e.g., landfilling) [194].
Furthermore, recycling can be categorized as closed-loop recycling, whereby the origi-
nal product is reformed (identical to primary recycling), or open-loop recycling, whereby
the waste is turned into a product that differs from the original product (this can be sec-
ondary or tertiary recycling). Within open-loop recycling, a distinction is made between
upcycling, side-cycling, and downcycling depending on whether the new product is of
higher, equal, or lower quality than the original product, respectively [189].
It is important to realize that all the mentioned end-of-life options for textile
waste—other than landfilling—have some value, but that value is not always equal. To
choose the best end-of-life option for a certain waste product, the costs and benefits of each
option should be evaluated. In Figure 9, a staircase is shown with all the end-of-life options
ordered from top to bottom. The European Union (EU) calls this the “waste hierarchy” in
their Waste Framework Directive (Directive 2008/98/EC) [195]. Generally, the higher up
on the staircase an option is, the lower the environmental impact and economic cost of that
process, due largely to the lower number of production process steps required to return to
a recycled end product. The flip side of this coin is that the less costly processes
Polymers 2025, 17, x FOR PEER REVIEW 16 ofalso
104 have
a more limited impact on the quality range of the secondary product. Reused products
essentially have the same quality as the original products before the latter became waste at
the endwaste
became of their lives,
at the endwhile chemically
of their lives, whilerecycled products
chemically recycledare reprocessed
products so thoroughly
are reprocessed
so thoroughly
that they will that
oftenthey
be will often be
of similar of similar
quality quality
to virgin to virgin products.
products.

Wastehierarchy
Figure9.9.Waste
Figure hierarchy staircase
staircase forfor textile
textile end-of-life
end-of-life options.
options. Ideally,
Ideally, processes
processes at the at
topthe
aretop are
useduntil
used untilthey
theynonolonger
longer yield
yield a product
a product or secondary
or secondary raw raw material
material of sufficient
of sufficient quality,
quality, in which
in which
caseaaprocess
case processlower
lowerdown
down should
should be be used,
used, except
except for for incineration
incineration or landfill.
or landfill.

Inan
In anideal
idealworld,
world,anyany time
time a product
a product reaches
reaches the the
endend of itsoflife—whether
its life—whether that was
that was
its first life (i.e., the product was virgin) or a later one (i.e., the product had already been been
its first life (i.e., the product was virgin) or a later one (i.e., the product had already
reusedor
reused orrecycled
recycledatatleast
least once)—one
once)—one would
would optopt for the
for the highest
highest levellevel
on theonstaircase
the staircase
in in
Figure 9 as long as that yields a secondary product of sufficient quality.
Figure 9 as long as that yields a secondary product of sufficient quality. As such, optimal As such, optimal
productand
product andmaterial
material recovery
recovery cancan be achieved
be achieved by cascading
by cascading down the down the staircase
staircase [189]. In [189].
theory,
In theory,the the
bottom
bottomtwotwoend-of-life options
end-of-life (incineration
options and landfill)
(incineration and landfill)should nevernever
should be be
taken because chemically recycled materials should be of equal quality to virgin
taken because chemically recycled materials should be of equal quality to virgin materials, materials,
meaning that process can be repeated infinitely. Incineration and disposal do not recover
any materials and thus do not contribute to a closed-loop economy, meaning they should
be resorted to only if the reuse or recycling process is impossible for the product or mate-
rial in question [196].
Historically, however, most textile waste has been dealt with through landfill dis-
Polymers 2025, 17, 628 16 of 94

meaning that process can be repeated infinitely. Incineration and disposal do not recover
any materials and thus do not contribute to a closed-loop economy, meaning they should
be resorted to only if the reuse or recycling process is impossible for the product or material
in question [196].
Historically, however, most textile waste has been dealt with through landfill disposal
or incineration due to its low operating cost, despite its lack of product or material recovery.
Only in recent decades—in light of environmental concerns—has this very linear model
been challenged and has the closed-loop economy become a focal point. However, there is
still a lack of mature, efficient recycling technologies and supported initiatives, meaning that
the textile industry still scores badly in terms of sustainability. This evolution can be seen
in Figure 10, which illustrates waste management in the US from 1960 to 2018, excluding
textiles that are reused or that illegally end up in nature. The trends show that until the
1980s, waste textiles ended up primarily as landfills. Afterwards, textile incineration and
recycling gradually increased. In 2018, textile waste management consisted of 15% recycling,
19% incineration, and 66% landfill [197]. Wool is a natural fiber primarily composed of the
Polymers 2025, 17, x FOR PEER REVIEW 17 of 104
protein keratin, which is found in the hair fibers of animals such as sheep, alpacas, goats
(cashmere), and other mammals [198–200].

Figure Textilewaste
10. Textile
Figure 10. wastemanagement
managementinin
thethe U.S.
U.S. (1960–2018)
(1960–2018) [197].
[197].

The aforementioned
The aforementioneddefinitions
definitions andand statistics
statistics on on textile
textile waste
waste management
management highlight
highlight
the need
needforforaccelerated
accelerated recycling
recycling of textiles
of textiles because
because current
current methodsmethods are inadequate
are inadequate in
addressing
in truetrue
addressing environmental
environmentalchallenges [201,202].
challenges Subsequently,
[201,202]. feasible feasible
Subsequently, solutionssolutions
for
achieving
for complete
achieving textiletextile
complete waste recycling are reviewed
waste recycling in the following
are reviewed in thesections,
followinginclud-
sections,
ing collecting,
including automated
collecting, textile textile
automated sortingsorting
(ATS),(ATS),
and different types types
and different of textile recycling
of textile recycling
technologies [203,204].
technologies [203,204].

3.1. Collection
Collectionand
andSorting
Sorting
3.1.1. Collection
Collection
Textile waste
waste isiscategorized
categorizedasaspre-consumer
pre-consumerwaste wasteoror
post-consumer
post-consumer waste depend-
waste depending
ingits
on onsource
its source
[205].[205]. Pre-consumer
Pre-consumer waste
waste is is generallyeasy
generally easytotocollect
collectand
and can
can be
be subdivided
subdi-
vided(i)into
into (i) production
production waste,waste,
whichwhich is generated
is generated duringthe
during productmanufacturing
theproduct manufacturing pro-
process [206], (ii) post-industrial waste, which is generated by non-textile
cess [206], (ii) post-industrial waste, which is generated by non-textile manufacturing manufacturing
industries that
industries thatsimply
simplyuse usetextiles asas
textiles inputs
inputs or or
outputs [207],
outputs andand
[207], (iii) (iii)
finished products
finished products
that become damaged or remain unsold in retail establishments [208].
that become damaged or remain unsold in retail establishments [208].
Production waste from a textile product can range from 10% to 50% of the raw mate-
Production waste from a textile product can range from 10% to 50% of the raw material
rial used to manufacture it but can easily be collected by the company internally. This
used to manufacture it but can easily be collected by the company internally. This makes it
makes it the most collected type of textile waste [206].
the most collected type of textile waste [206].
In theory, so-called post-industrial waste is also easy to collect separately from mu-
nicipal waste by setting up waste collection schemes between the textile and non-textile
industries. In practice, however, this waste is often not collected separately because the
collection creates logistical difficulties, and much of the waste ends up being so contami-
nated that it can no longer be reused or recycled, such as medical textiles used in hospitals
[207].
Polymers 2025, 17, 628 17 of 94

In theory, so-called post-industrial waste is also easy to collect separately from mu-
nicipal waste by setting up waste collection schemes between the textile and non-textile
industries. In practice, however, this waste is often not collected separately because the col-
lection creates logistical difficulties, and much of the waste ends up being so contaminated
that it can no longer be reused or recycled, such as medical textiles used in hospitals [207].
The unsold or lightly damaged finished products found in store inventories (most
often clothing and footwear) are extremely suitable for reuse and should be collected
and recovered as such. Once again, most of these products are not collected for reuse;
instead, they are destroyed to avoid collection, sorting, and possible recycling costs, to
avoid devaluing the brand value, and to avoid paying inventory taxes [209]. In 2023, the
EU agreed upon a resolution to ban the destruction of unsold clothing, which could help in
the sustainable collection of this waste category if the resolution can be enforced, although
this would still not prevent companies from exporting their waste outside the EU first [210].
It should be further highlighted that post-consumer or household textile waste is
more difficult to collect because it comes from many individual sources and must be
separated from regular municipal waste to be of use [211]. A large portion of textile waste
is currently still collected without separation from municipal waste. For example, in 2023,
the EU generated 13.9 million tons of post-consumer textile waste (approximately 12 kg
per person) but collected only 22% of it in a way that would enable reuse or recycling. To
improve these numbers, EU legislation will require member states to collect textile waste
separately from municipal waste starting in 2025 [195].
Separation from other municipal waste can occur by having charitable organizations
or retail stores take in waste textiles, or by installing separate collection bins for textile
waste and incentivizing consumers to use such bins. In general, the most important factor
for collection rates is consumer convenience, which is geographically dependent, with
collection bins being more accessible in more developed regions [205,212].
Recurring problems for post-consumer textile waste collection are unclear regulations
for collecting organizations (including the definition of what is and is not classified as waste)
and a lack of control over permits for collection bins. Additionally, a lack of sanctions
for incorrect collection can lead to illegal textile containers and a lack of transparency
throughout the collection process [213]. In addition, (domestic) high-grade recycling
possibilities are still scarce for most textile types, meaning that waste textiles generally
have a low value, especially because the incineration costs for any collected but unused or
unrecycled material are high [213]. For the few recyclable textiles, product saturation can
also be a concern, making the diversity of textile waste collection important [214].
Fortunately, modern technologies, such as the Internet of Things (IoT), big data analy-
sis, and blockchain technology, can make textile waste collection more sustainable. Waste
products, collection bins, and collection vehicles can all be linked in an IoT network, such
as by incorporating smart tags (e.g., radio-frequency identification [RFID] tags) into textile
products and suitable sensors into waste containers and collection vehicles. This allows
collection services to track the amount, type, location, and even condition of textile waste
that is deposited into collection bins or currently loaded onto collection vehicles. These big
data can then be fed into predictive algorithms and decision-making tools to optimize col-
lection routes both ahead of time and in real time, increasing collection rates and reducing
transportation costs (both financial and ecological) [215–217]. If these data are transferred
through a blockchain accessible by all stakeholders, they can also improve the traceability,
transparency, and accountability of the waste collection process, thus even minimizing
illegal dumping and collection [206].
Further down the line, smart contracts can be set up between waste collection services
and textile recyclers to automate transactions and to ensure that the quantity and quality of
Polymers 2025, 17, 628 18 of 94

waste being delivered are correct without the need for labor-intensive manual verification
and paper-based documentation [218]. Even consumers can be involved by supplying
mobile apps and platforms that provide information (and thus awareness), incentives for
correct disposal, and a feedback option. These tasks would also allow consumers to request,
schedule, track, and pay for individualized services [206].
The downside to the aforementioned technological aids is that they all require specific
infrastructure, good connectivity, and security for all users. While possible, these are
accompanied by extra maintenance costs and a need for regulation from higher-level
platforms [206,218]. Additionally, due to the little manual involvement in this automated
collection system, there can be more contamination in the collected textiles, which can
cause issues down the line [213]. The current technology is also still maturing in this field,
and certain elements, such as cheap, waterproof, and flexible sensors for collection bins,
are not yet available [219].
It is important to note that a large amount of textile waste collected in developed
countries is exported to developing countries. In 2019, for example, almost 1.9 million
tons of waste clothing collected in the EU were exported mostly to countries in Africa
(e.g., Tunisia, Ghana, Cameroon, and Togo), Asia (e.g., Pakistan, the United Arab Emirates,
and India), or Europe (e.g., Ukraine). This represents 25% of the textiles consumed each
year in the EU and marks a large increase from the approximately 600,000 tons exported in
2000. Most of this waste becomes untraceable for the origin country and is not necessarily
recovered; used textiles in Africa often get reused locally, while the waste in Asia is mostly
downcycled into rags or fillers, but a large portion of the waste streams is likely to end
up in open landfills [220]. More recently, many Asian and African countries have started
banning the import of waste clothing to boost their domestic textile industries and reduce
the environmental impact of that waste ending up in landfills [221].

3.1.2. Sorting
While sorting is not required for pure waste streams, it is required for all mixed waste
streams, such as post-consumer textile waste. By sorting, textile waste of different colors,
chemical compositions, sizes, and qualities can be separated [108,110]. For example, the
quality of a waste product can determine whether it is fit for reuse, must be recycled, or
needs to be incinerated or disposed of [222]. Chemical composition is very important for
recycling processes because these processes are tuned to specific fiber types, and color is
similarly important for recycling without prior decolorization because the secondary raw
materials resulting from such recycling processes will end up having the same color or a
blend of the input colors [223–225].
Currently, textile waste is mainly sorted manually. This is cheap in developing coun-
tries where labor costs are low, and it allows for a good estimation of quality, particularly
whether a waste product is reusable or must be processed further. However, there are clear
downsides to manual sorting. It is very time-consuming and cannot efficiently deal with
high volumes of textile waste nor separate waste based on chemical composition other
than by relying on product labels, which can be faulty or missing [36–38,203]. In addi-
tion, workers often experience less evident working conditions, which leads to unreliable
sorting [226].
To overcome these limitations, ATS is being developed. To be effective, this sorting
system must be nondestructive, able to distinguish qualitatively between fiber types, able
to quantitatively analyze fiber blends, and have high throughput [227]. The focus is
placed on the separation of waste by color and chemical composition because ATS systems
currently cannot distinguish quality differences to the level where they can sort reusable
from non-reusable textiles [213].
Polymers 2025, 17, 628 19 of 94

Physical sorting methods, such as sorting based on density or melting point, can be
used in an ATS system. Melting point indicators are considered by some to be inexpen-
sive [214] while others consider them expensive [226], but in any case, these physical sorting
methods are rather slow, require rigid training from the operator, and have limitations
on the chemical composition they can distinguish (e.g., melting point indicators cannot
distinguish PA6,6 from polyester fibers) [214,226].
A promising sorting method for the future is the use of RFID tags in textile products.
These tags can contain information on the product (e.g., its chemical makeup, color, and
age), which can be read remotely by an in-line sensor in a sorting facility. Unfortunately,
these RFID tags are currently used only for clothing and often fail after several laundry
cycles [228].
A concept similar to RFID tags is the exploitation of photonic crystals, as described by
Lezzi et al. [229]. These polymeric photonic crystals can be introduced into textile
Polymers 2025, 17, x FOR PEER REVIEW fibers
20 of 104
and exhibit characteristic infrared reflectance responses in the 1–5.5 µm wavelength range,
which can be read by spectroscopes at different angles, thus acting as an information tag
within the material
While RFID tags itself.
and photonic crystal technology are still being developed, the focus
of theWhile RFIDon
literature tags
ATS and photonic
today crystal technology
is on spectroscopic are an
methods, stilloverview
being developed,
of which isthe focus of
given
the literature
in Table on ATS
2. Color todaybe
can easily is detected
on spectroscopic methods,
by a computer an overview
system of which
using sensors is given
that pick up in
reflected visible light (wavelengths roughly between 400 and 700 nm). However,
Table 2. Color can easily be detected by a computer system using sensors that pick up reflected to detect
chemical
visible composition,
light (wavelengths lightroughly
in the infrared
betweenwavelength
400 and 700domain is required.toState-of-the-
nm). However, detect chemical
art research on textile sorting is mainly concerned with NIR spectroscopy,
composition, light in the infrared wavelength domain is required. State-of-the-art research which uses on
wavelengths between 800 and 2500 nm [226,230], but also sometimes studies
textile sorting is mainly concerned with NIR spectroscopy, which uses wavelengths between mid-infrared
(MIR)
800 andspectroscopy, whichbut
2500 nm [226,230], encompasses the wavelength
also sometimes range of 2500
studies mid-infrared nm‒25
(MIR) µm [24,231–
spectroscopy, which
235]. Occasionally, visible near-infrared (VNIR) spectroscopy
encompasses the wavelength range of 2500 nm–25 µm [24,231–235]. Occasionally, is mentioned, which isvisible
a
combination of visible light and NIR light with wavelengths between 400 and 1000 nm.
near-infrared (VNIR) spectroscopy is mentioned, which is a combination of visible light and
Various types of textiles, such as cotton, wool, and polyester, possess distinct spectral sig-
NIR light with wavelengths between 400 and 1000 nm. Various types of textiles, such as
natures that can be detected in this range [236]. An example of chemical-composition iden-
cotton, wool, and polyester, possess distinct spectral signatures that can be detected in this
tification via infrared spectroscopy is shown in Figure 11. Here, ATR-FTIR spectroscopy
range [236]. An example of chemical-composition identification via infrared spectroscopy
has been used in the MIR domain.
is shown in Figure 11. Here, ATR-FTIR spectroscopy has been used in the MIR domain.

Figure 11. Example of the attenuated total reflection–Fourier transform infrared (ATR-FTIR) spectra
Figure
of 11. Example
common of the attenuated total reflection–Fourier transform infrared (ATR-FTIR) spectra
fibers [231–234].
of common fibers [231–234].
For the actual sorting and classification of any identified fiber type, advanced machine
For software
learning the actual tools
sorting
canand
be classification of any
used for pattern identified fiber
recognition and totype, advanced
process ma-
the collected
chine learning
infrared software Typical
data [203,237]. tools canexamples
be used forarepattern recognition
also listed in Tableand
2. to process the col-
lected infrared data [203,237]. Typical examples are also listed in
Furthermore, a study conducted by Riba et al. [24] aimed to enhance Table 2. textile sorting
Furthermore, a study conducted by Riba et al. [24] aimed to enhance textile sorting
using an automatic sensing and sorting approach, which involved analyzing 350 well-
using an automatic sensing and sorting approach, which involved analyzing 350 well-
defined textile samples composed of a single fiber type. The ATR-FTIR spectrum was uti-
lized in combination with various algorithms, including principal component analysis
(PCA), k-nearest neighbors (k-NN), and canonical variate analysis (CVA). The outcomes
demonstrated that unknown samples could be sorted automatically with high speed and
excellent accuracy without the need for any prior analytical treatment.
Polymers 2025, 17, 628 20 of 94

defined textile samples composed of a single fiber type. The ATR-FTIR spectrum was
utilized in combination with various algorithms, including principal component analysis
(PCA), k-nearest neighbors (k-NN), and canonical variate analysis (CVA). The outcomes
demonstrated that unknown samples could be sorted automatically with high speed and
excellent accuracy without the need for any prior analytical treatment.
Chen et al. [238] used NIR with the partial least squares (PLS) and extreme learning
machine (ELM) algorithms to categorize textile fibers. According to the findings, the
ELM-based predictive models showed higher accuracy than those generated by PLS while
having a similar computational cost. Similarly, Liu et al. [239] utilized various machine
learning algorithms, including a support vector machine (SVM), multilayer perceptron
(MLP), and convolutional neural networks (CNNs), in combination with the NIR spectrum,
to classify waste textile fibers. CNN was claimed to demonstrate a higher classification rate,
ranging from 92% to 98%.
Zhou et al. [230] utilized NIR spectroscopy in combination with PCA, soft independent
modeling by class analogy (SIMCA), and latent Dirichlet allocation (LDA) algorithms to
identify seven common, well-defined fibers rapidly and precisely. Their findings revealed
that cotton, lyocell, PP, and PET could be efficiently classified, with an almost perfect
recognition rate. However, wool, cashmere, and PLA had overlapping features in their
chemical and physical analyses, resulting in lower recognition rates when the SIMCA
algorithm was utilized. However, through the utilization of LDA and some modifications,
the fibers could be completely classified. Consequently, the NIR spectroscopy method
utilizing various algorithms has demonstrated the efficient and accurate classification of
many important types of textile fibers.
The aforementioned studies show that spectroscopy techniques have many advantages
for use in ATS because they can be performed in real time with good throughput while
being nondestructive methods [228]. Combining visual and infrared light can yield very
accurate detection of not just fiber types but also dyes, thin coatings, and finishes at the
surface of such fibers [206]. A drawback of the discussed spectroscopic technologies,
however, is that they allow for the identification of only one point in the sample, which is
often not good enough when it comes to complex heterogeneous samples, such as textile
waste [240].
A possible solution to this problem is hyperspectral imaging (HSI), which combines
both spatial and spectral scanning. Essentially, a two-dimensional scan of the waste sample
is taken, and at each point (pixel) on the surface, an infrared scan is performed to generate its
spectrum. This allows for the detection of multiple fiber types or contamination on a waste
sample [240]. For example, Jiang et al. used HSI in the NIR range to identify contamination
in cotton lint samples, with 90% accuracy [241]. Blanch-Perez-del-Notario et al. reported
that HSI in the visible-NIR range can be used to identify wool and polyamide samples with
high accuracy while losing some accuracy on cotton, viscose, and PET samples, especially
in the case of fiber blends. Importantly, the system can discriminate between denim and
non-denim fabrics of the same color, which is otherwise difficult to distinguish for ATS
systems [236].
While HSI allows for the identification of components in heterogeneous waste at
both high accuracy and speed [242], it shares a major limitation with more conventional
spectroscopic techniques: a lack of depth perception due to the low penetration of visible
and infrared radiation. All spectroscopic techniques can characterize only the surface
layer of a waste sample. Thus, textiles with thicker coatings or multilayers cannot be
identified by infrared spectroscopy, and even functional finishes can pose problems for
sensors [203]. Moreover, infrared technology can be costly, particularly for large-scale
ATS, because regular calibration of infrared sensors and cameras is necessary to maintain
 Polymers 2025, 17, 628 21 of 94

the requested high sensitivity and proper functioning, and extensive spectral libraries are
required to analyze the gathered data. Fortunately, these libraries can also be built using
other analytical techniques, such as solid-state nuclear magnetic resonance [227]. On the
processing side, fast computers with a large data storage capacity (doubly so for HSI) are
required. Any noise or interference encountered during the infrared scanning process can
also have a substantial detrimental effect on neural network accuracy [206].
Despite the foregoing minor issues with spectroscopy-based ATS, the main obstacle
and practical challenge is the complexity of textile waste, including the (multiple) presence
of dyes, finishes, buttons, zippers, and prints, but mostly the increasing prevalence of
mixed textiles consisting of different fiber types, including those products where different
fiber-type threads are used for the seams [227]. While HSI could be an early contender
Polymers 2025, 17, x FOR PEER REVIEW for tackling this problem, dealing with mixed textiles in the future will certainly 22 of 104 demand
additional resources and efforts from the scientific community.
For completeness, additional emphasis is placed on the fiber recovery of tire and
rubber products (Figure
For completeness, 12). With
additional an annual
emphasis production
is placed on the fiberofrecovery
approximately 60 rub-
of tire and million tons
ber of tires and
products rubber
(Figure products,
12). With an the textile
annual sector accounts
production for roughly
of approximately 5% of this
60 million tonstotal,
of which
tiresequates
and rubberto theproducts, the textile sector1–1.2
use of approximately accounts for roughly
million 5% of this
tons of fibers total, which
primarily made of PET
equates
and, to the use of
a lesser approximately
extent, polyamide. 1–1.2 millionmaximum
To ensure tons of fibers primarily
safety and reducemadethe of risk
PET of harm,
and,tire
to atextiles
lesser extent, polyamide. To ensure maximum safety and reduce the risk
are made using high-quality PET grades that have significantly high IV values, of harm,
tiretypically
textiles arefalling
made within
using high-quality
the range of PET grades that
0.95–1.05 dL·have significantly
g−1 [133]. high IV values,
The exceptional quality and
typically falling within the range of 0.95‒1.05 dL·g −1 [133]. The exceptional
significant quantity of utilized textile fibers necessitate distinct approaches for reusing quality and
significant quantity
them, thereby of utilized textile
underscoring fibers necessitate
the significance of tire distinct
recycling.approaches for reusing
them, thereby underscoring the significance of tire recycling.
The first step in recycling the aforementioned textiles involves separating the vari-
The first step in recycling the aforementioned textiles involves separating the various
ous components of the tires, including rubber compounds, steel wires, and textile fibers.
components of the tires, including rubber compounds, steel wires, and textile fibers. Cry-
Cryogenic and ambient grinding [243], water jet pulverization [244], and supercritical
ogenic and ambient grinding [243], water jet pulverization [244], and supercritical solvent
solvent pulverization [245] are among the methods currently proposed for powderizing
pulverization [245] are among the methods currently proposed for powderizing tires
tires while separating the steel and textile components. Methods such as water jet and
while separating the steel and textile components. Methods such as water jet and super-
supercritical
critical carbon dioxidecarbon(CO dioxide (CO2 ) pulverization
2) pulverization are particularly are particularlybecause
advantageous advantageous
they are because
they are environmentally friendly and partially devulcanize the
environmentally friendly and partially devulcanize the tires during the process. Once sep-tires during the process.
Once
arated fromseparated from
the tire and the tire
sorted, theand sorted,
fibers can bethe fibers using
recycled can bestandard
recycledmethods.
using standard
How- meth-
ods. However, the presence of impurities, such as tire particles, can
ever, the presence of impurities, such as tire particles, can hinder the recycling process. hinder the recycling
process. Supplementary
Supplementary procedures areprocedures
thus requiredaretothus required
remove rubber toparticles
remove before
rubberrecycling
particles before
recycling
[246]. [246].

Figure 12. Tire

Figure textile
12. Tire recovery
textile [247].[247].
recovery
Polymers 2025, 17, 628 22 of 94

Table 2. Overview of ATS using different IR methods; accuracy based on selected test cases in the main references.

IR Method Algorithm Fiber Accuracy Challenges Advantages Ref.

Cotton/viscose 68%
PET 70%
Polyamide 100%

Quadratic Wool 100% A more extensive sample set is needed to Compared to the NIR range, the VNIR range offers
VNIR discriminant Misclassified guarantee a robust sorting system for all higher spatial resolution, cheaper and compact [236]
classifier, SVM, PCA 50% as cotton textile varieties. cameras, and blue denim sorting.
Cotton and PET
and 40%
as PET
Misclassified
PET and cotton
as cotton
For real sorting machinery, implementing
the specific software to establish a robust
IR-spectra database for correctly classifying
dirty-wet textile waste.
Polyamide, PET, viscose, Post-sorting, a second sorting by color is Automatically classified fiber samples with 100%
ATR-FTIR PCA, CVA, k-NN cotton, linen, wool, silk 100% required to reduce additional dyeing. accuracy and high speed, without any involvement [24]
Strict maintenance protocol must be of prior analytical treatment of the textile samples.
ensured for the contact between the sensor
and the textile to register and compare the
IR spectrum with the database
for classification.
Pure PET slash, pure
PET normal, pure wool,
To ensure higher prediction accuracy, a The proposed method is simple and practical,
pure cotton normal,
more comprehensive sample spectrum presents a fast identification speed and a higher
NIR SVM, MLP, CNN PET/polyamide, 92–98% [239]
information is required to be included in recognition rate, and can be applied to a wide
PET/wool,
the established standard spectral library. range of applications.
PET/cotton slash,
PET/cotton, polyamide
Cotton 93% Low accuracy arises for cotton and This is a nondestructive, simple, and fast method
NIR SIMCA PET 92% polyester due to their relatively close that can identify fibers with a total recognition rate [226]
spectral characteristics. higher than 95%.
PA6,6, acrylic, wool, silk 100%
Polymers 2025, 17, 628 23 of 94

Table 2. Cont.

IR Method Algorithm Fiber Accuracy Challenges Advantages Ref.

As there are many overlapping features in

Cotton, TencelTM , Using the mentioned algorithm for this method,
the chemical and physical analyses of wool
NIR PCA, SIMCA, LDA PP, PLA, PET, 100% seven textile fiber types were identified quickly [230]
and cashmere, there is lower accuracy for
wool, cashmere and accurately.
both textiles.

Wool, silk, cotton, linen,

Mixed textiles are highly inhomogeneous.
viscose, PET, PA6,6, ATR-FTIR spectroscopy enables quick, easy, and
Thus, in such cases, homogeneity is tested
ATR-FTIR PCA acetate, TencelTM , n.d. 1 nondestructive classification and semi-quantitative [235]
using microscopic or
acrylic, elastane, 15 analysis of textiles.
IR-microspectroscopic analysis.
two-component textiles

For the analysis, the number of spectral The ELM method is superior to the
variables was reduced. However, the key to conventional PLS.
Not the successful utilization of an NIR-based The developed procedure may have commercial
NIR PLS, ELM Wool, PET, PAN, PA6,6 [238]
mentioned analytical method is to construct a robust and regulatory potential to avoid laborious,
calibration model using samples with time-consuming, and expensive wet
sufficient representativeness. chemical analysis.

Obtaining a good-quality r-FTIR spectrum

Principal of elastane was problematic as the r-FTIR is a suitable technique for the quick, easy,
Wool, silk, cotton, linen, 99% (r-FTIR)
component-based reflectance spectra of the used elastane nondestructive, and non-invasive analysis of
ATR-FTIR, jute, sisal, viscose,
discriminant analysis thread was distorted. different types of textile samples.
r-FTIR, acetate, TencelTM , [234]
and random
mATR-FTIR fiberglass, PET, PA6,6,
forest-based For extraneous materials on sample fibers For analyzing very small threads (up to
acrylic, elastane, PE, PP 96%
machine learning (additives or contaminants), the spectrum 10 individual fibers), a possible mATR-FTIR
(mATR-FTIR) approach should be preferred.
recorded is influenced by contaminants.

The developed data-mining models can be

The combination of spectroscopy and
made more extensive by adding more data
Viscose, PA6,6, chemometrics has led to a highly desirable method
FTIR PCA, SIMCA 97% of different fiber types, which will result in [248]
acrylic, PET for clustering and classifying 138 synthetic fiber
a sophisticated forensic tool for
samples into four groups.
fiber discrimination.
1 Not determined.
Polymers 2025, 17, 628 24 of 94

3.2. Reuse
Through collection and manual sorting, end-of-life textile products with sufficiently
high quality can be identified as fit for reuse. This quality requirement leads to the absence
of technical textiles in the reuse industry because these textiles are developed for their
functions rather than their aesthetics. This means that they are generally used until their
functions fail, after which they are no longer suitable for reuse [249]. The opposite is true for
clothing, which is often discarded before the mechanical properties fail for fashion reasons.
As such, much of the literature on textile reuse is centered on secondhand clothing [250].
Household textiles are situated between these two extremities and are generally reused in
some capacity, but not as much as clothing is [251].
In the context of ISO 5157:2023, “reuse” appears to be an umbrella term for three
separate end-of-life processes—reuse, repair, and remanufacturing—as noted in other
definitions in the same standard [186]. All these processes involve at least minor treatments
to the product, but crucially, the product is maintained throughout the process rather than
being dismantled into secondary raw materials that may be used to create other products.
Actual reuse—sometimes called secondary use—involves the least amount of treat-
ment and is usually limited to washing and sometimes refinishing or refreshing of
color [186,252]. This happens more on an informal level, through the exchange or do-
nation of clothing or household textiles within families or between friend groups, than at
an industrial level [253]. The more formal market is established by charity organizations
and secondhand shops, internet platforms, and textile libraries, where secondhand textiles
can be bought or exchanged [254].
In Europe, 22% of clothing waste is collected for reuse or recycling, of which 7–10% is
suitable for reuse but only 1–3% consists of clothing items that are fully functional and have
a market value by virtue of their being fashionable, hence entering the market for actual
reuse [189,250]. In recent years, these numbers have been increasing due to the Extended
Producer Responsibility for Textiles Decree, which states that from 2025 onward, producers
will be responsible for the preparation of textiles for reuse or recycling at the end of their
lives [255].
Repair denotes a process in which waste textile products are not fully functional but
still do not have major defects, and there is a simple replacement of damaged parts [186].
For most clothing or household textiles, this involves repairing small details, such as
patches of fabric, buttons, or zippers, although items with integrated or hidden electronics
can be a hindrance to this process [256]. After repair, the products are entered into the
secondhand clothing or household textile market, as if they were fully reused.
Remanufacture can occur if more major (industrial) procedures are required to return
a product to its original condition [186]. While there is no universally accepted definition
of remanufacturing [257], Lund presented a general working definition as early as 1984:
“Through a series of industrial processes in a factory environment, a discarded product is
completely disassembled. Useable parts are cleaned, refurbished, and put into inventory.
Then the product is reassembled from the old parts (and, where necessary, new parts)
to produce a unit fully equivalent and sometimes superior in performance and expected
lifetime to the original new product” [258]. This has been used for decennia within the
engineering and electrical and electronics industries but is a new concept for the textile
industry [259]. While it is necessary to reassemble the product after disassembly, the
reassembled product does not need to have the same identity as the original (waste)
product. Clothing items can be transformed from one piece into another (e.g., a pair of
jeans into a jacket), depending on fashion trends, for example [259].
Reuse is higher up on the waste hierarchy than recycling because it has inherent
advantages. It does not require as much sorting, packaging, transportation, manufacturing,
Polymers 2025, 17, 628 25 of 94

nor a whole recycling process, and thus results in a larger net decrease in a product’s
environmental and economic impact [260]. For example, clothing libraries were found to
be environmentally beneficial if a garment’s service life was considerably extended [195].
An extension of 3 months leads to an average reduction in its carbon and water footprints
of 5–10% [261,262].
While more advantageous than recycling in the aforementioned aspect, it should be
noted that an extension equal to its original service life, wherein a new owner uses the prod-
uct as many times as the virgin product—i.e., a 1:1 replacement rate—is unrealistic [189].
This is mostly because textiles are damaged during the use phase of their lifetimes, and
this damage is not repaired during reuse processing. For textiles that are washed during
their use phase, most of the damage is incurred due to the mechanical stress that fibers are
placed under during laundering [227]. Aging is also an important factor, for both clothing
and household textiles. Physical or mechanical aging is caused by bending, stretching, and
abrasion of the fibers [263], which cause an ordering of amorphous polymer chains and
thus increases crystallinity, which makes the fibers stiffer and more brittle, with a tendency
to deform plastically or break under stress due to a decrease in the molecular mobility of
the polymer [264]. Chemical aging, on the other hand, is caused by the presence of aqueous
solutions, oxygen, or high temperatures [263], which can cause changes in the molecular
bonds in the polymer chains (e.g., through hydrolysis, oxidation, and thermal scission).
Scissions in polymer chains can cause a rapid decrease in the degree of polymerization
and, thus, average molar mass. In turn, this decreases the tensile strength and elasticity of
the fibers and can also introduce more reactive sites to the polymer chains, thus affecting
their chemical reactivity [265]. This decrease in fiber quality means that products can be
reused only for a certain amount of time and should be recycled when they are no longer
of sufficient quality.
Besides the technical limitations, reuse is also highly dependent on local legislation,
which may allow or prohibit the reuse of certain items (e.g., the reuse of baby clothing is
sometimes prohibited due to the possibility of it transmitting diseases) [260], and on the
education of consumers, who require a level of awareness for secondhand shopping to be
developed profitably [266].

3.3. Pretreatment Prior to Recycling

Textile waste that is not fit for reuse often requires some form of treatment before it
can be recycled, incinerated, or landfilled. This is especially true for waste that is destined
to be recycled, as the quality of the outputs of recycling processes is highly dependent on
the quality of their inputs, and virtually all recycling technologies are limited to textiles
with specific compositions. This is why sorting is important (see Section 3.1.2), but the
sorting process takes only the chemical composition of the bulk of the waste into account.
In reality, textile waste often comes with so-called hard points (e.g., zippers, buttons, or
labels), is colored with dyes or pigments, is finished or coated with specific chemicals, or
may have been contaminated during its use phase [267,268]. Certain contaminants can
simply be washed away, but certain additives are much more difficult to remove, yet they
must be removed for optimal recycling. In addition, not all recycling technologies can
accept waste of any shape or structure, so size reduction pretreatment is often necessary.
This size reduction is often the first step of any pretreatment and can even take place before
the sorting phase for waste that cannot be reused as a product (e.g., pre-consumer waste).
In practice, it usually consists of simple mechanical cutting and shredding operations [269].
Waste textile materials can even be ground into powder to increase their accessible surface
areas and decrease their crystallinity, but this destroys any fiber structure and is thus
not applicable to mechanical fabric, yarn, or fiber recycling. Additionally, it limits the
Polymers 2025, 17, 628 26 of 94

separation options for blended fibers and should thus be used only for single-polymer
textile waste [270]. Some mechanical fiber blend separation techniques using centrifuges,
cyclones, sink-float baths, or electrostatic separators do exist, but these increase the cost
of the process and are highly limited by the degree of entanglement of the different fiber
types [271].
On the other hand, the forms of textiles, whether in the form of yarns or fabrics,
significantly impact the challenges faced during recycling. Yarns, especially those made
from blended fibers, can become tangled or knotted in machinery, leading to clogging
and inefficiencies. Their fine, flexible structures make mechanical recycling difficult, often
resulting in jams and equipment wear. Fabrics, particularly those woven or knitted from
blends such as polycotton or elastane with polyester, present additional hurdles due to their
tightly interlaced structures, which resist separation and can deform during processing,
causing inconsistent recycling results. Blended textiles, with their varying fiber properties,
complicate both mechanical and chemical recycling because differences in melting points or
chemical behaviors often lead to contamination and reduced quality of recycled materials.
These challenges necessitate the use of specialized recycling techniques to effectively
manage and process diverse textile forms [272,273].
Disassembly (or trim removal) is the name given to the pretreatment steps that involve
the removal of hard points from textile waste. These include elements not made of textile
materials, such as zippers, buttons, and rivets, but also elements made of textile materials
with compositions different from those of the bulk textile, such as labels, patches, and
linings [274]. These foreign elements can be removed from textile waste by hand, which
provides high removal accuracy and minimizes the lost textile surface area, but this is very
labor-intensive and thus expensive. For this reason, automated textile disassembly (ATD)
techniques are being developed [269].
The oldest and only commercially prevalent ATD technique is built into the mechanical
fiber recycling process, rather than being a separate pretreatment step. In this case, textile
waste that has been cut down to size is subjected to pickers that open the textiles and tear
off the hard points before being garneted fully. During these picking or garneting phases,
other mechanical separation systems can also be implemented, such as cyclone separators,
sink-float baths, or magnetic separators. The major downside of this built-in system is that
it does not remove all types of hard points, focusing mainly on the non-textile elements but
ignoring the labels, patches, linings, etc. Machinery manufacturers ANDRITZ Laroche and
Dell’Orco & Villani offer tearing lines with this built-in ATD technique [268].
The second type of ATD system is a more recent newcomer to the market. It requires
that the waste be cut up into square pieces (clippings) by two successive cutting machines,
after which the squares are separated into squares with hard points and squares without
hard points, either by visual means (camera identification) or mechanical means (based
on physical characteristics, such as density or shape). In this system, the size of the
clippings plays a major role because smaller clippings lead to less material loss when a
square is expelled, but they also place a limit on the fiber length, which is detrimental
for mechanical fabric/yarn/fiber recycling [194,269]. An example of this ATD system
is Trimclean, developed by Valvan, which utilizes cameras that feed images into neural
network software. This software decides which squares should be separated from the bulk
through pneumatic ejection. It also uses metal sensors to detect non-textile trims more
accurately [275].
The ATD technology that is most difficult to implement is automated customized
cutting, where the waste does not need to be cut into clippings; instead, a robot cuts hard
points from the waste item on an article-by-article basis, either with a blade or a laser. The
hard points are then separated from the rest of the material by the robot itself or by any
Polymers 2025, 17, 628 27 of 94

of the aforementioned mechanical separation techniques. This process requires accurate

cameras and algorithms to recognize the type of waste and its hard points. It also requires
that the waste articles be laid out properly before being scanned. Despite these challenges
and their associated costs, the advantages are that minimal recyclable fabric is wasted and
the fiber length of that material is kept at its maximum. This system is still being researched
by companies such as CETIA and is not yet commercially available [269,276].
Besides hard points, colorants (in the form of dyes or pigments) are often present in
textile waste. These rarely interfere with recycling processes, although they have been
reported to coagulate and form insoluble particles in re-extrusion or chemical recycling
processes, which gives rise to problems during spinning [277]. If colorants are not removed
during a pretreatment step, they will also be present in the secondary raw material, limiting
the market for the material and lowering its value.
Theoretically, there are two options for the removal of color from a material: removal
of the colorant molecules themselves or destruction of their chromophore groups. The
latter renders them inert but leaves them in the material. As the removal of colorants from
textile waste is not a crucial step in the overall recycling process, there has not been much
research on it. It is likely, however, that for the colorant extraction method, principles
similar to those applied to the removal of colorants from textile wastewater after the
dyeing process (e.g., adsorption, coagulation, flocculation, and solvent extraction) can be
used if the colorants can first be extracted from the solid waste and placed in a liquid
environment [7,8,278–283].
For example, Yousef et al. noted that treating denim waste with nitric acid (HNO3 ;
concentration below 60%) can leach dyes from the fabrics, after which the spent acid can
be regenerated with activated carbon (AC) [284]. The chromophore destruction method
was investigated by Powar, who found that textiles colored with reactive dyes (mostly
cellulose-based textiles, such as cotton) can undergo a conventional alkaline reductive
treatment using NaOH and a reducing agent (e.g., sodium hydrosulfite) for color stripping.
Alternatively, they can be treated with ozone for up to 98% color removal, though with
serious mechanical damage incurred to the fibers [285,286].
Glucose as a green reducing agent was proposed as a third option and was found to re-
move color with much less incurred damage—even less damage than with the conventional
alkaline treatment—but with the requirement of a higher processing temperature. Powar
also noted that this was only possible for dyed textiles because pigments were extremely
difficult to destroy, even with ozone [287]. Määttänen et al. also found alkaline washing
and ozone treatments to work for the destruction of dyes from cotton materials alongside
treatment with hydrogen peroxide [288]. This color removal is made very challenging
specifically in post-consumer waste because information on which dyes or pigments were
used in a product or their remaining contents at the end of their lives is often lacking [289].
Other major additives present in textile waste are the chemicals used in the finish-
ing or coating of the fibers. These chemicals are applied to give the product functional
properties, such as anti-microbial properties, anti-wrinkle properties, softness to the touch,
and flame retardancy, but they often remain in significant quantities in textile products
at the end of their lives [290,291]. Some of these chemicals can be ignored for recycling
purposes, thus remaining in any secondary raw material. Other chemicals must be removed
during the pretreatment step, or they will interfere with the recycling process itself and
lead to technical problems, such as low solubility and decreased dyability [267,292]. For
example, Björquist [293] found that cotton treated with dimethylol dihydroxyethyleneurea
(DMDHEU)—an “easy-care” anti-wrinkle finish—was difficult to dissolve into NMMO
during the production of lyocell fibers, even though that is their conventional solvent
Polymers 2025, 17, 628 28 of 94

Similarly, Egan et al. [270] discovered that the presence of DMDHEU on cotton presented a
large obstacle to enzymatic biodegradation.
The method required for the removal of the aforementioned chemicals depends entirely
on the chemical structure of the finishing chemical and its method of application onto the
textile substrate. In general, chemical degradation and subsequent dissolution of the
finishes is the most common, as is the case for the aforementioned DMDHEU examples,
where the finishes were removed via acidic and alkaline hydrolysis treatments [294,295].
The CreaSolv process by CreaCycle GmbH is an example of a treatment used to remove
thicker coatings or layers of textiles adhered to each other with an adhesive. For example,
it could delaminate or dissolve PU, polyamide, PVC, and acrylate coatings from PET and
polyamide substrates [194].
An alternative to dissolution for coatings is the use of an adhesive polymer material
between the coatings and the substrate, which can be activated with a certain trigger. An
example of this is the INDAR system by Rescoll Technological Center, which includes
blowing agents in its adhesive activated at a certain temperature (130 ◦ C, 150 ◦ C, or 170 ◦ C),
thus causing easy debonding at that temperature. This is conceptually similar to the ADT
system using disintegrable stitching threads, and it has the same downside of requiring this
adhesive upon conception of the product. It has been proven to work for the debonding of
PU coatings from PET textile substrates [296,297].
A third option is the PolySep process, in which shredded, coated textile waste is
soaked in a solvent and then brought into contact with hot water or steam, leading to flash
evaporation of the solvent and detachment of the coating from the substrate. This was
originally developed for the removal of PVC layers from PET substrates [298].
Contrary to the aforementioned examples, some chemical processes are adapted to
finishing chemicals and can non-selectively degrade them while degrading the polymer,
making a separate finish removal pretreatment unnecessary [267]. It should be noted
that removal of finishing chemicals can usually occur before or after the size reduction
pretreatment step [299].
While methods can be found to remove all the aforementioned additives, more focus
should be placed on the application of these additives during the design of the textile
product, also known as design for recycling. Options such as the use of destructible
stitching threads and triggerable adhesives that cause delamination should be considered
more, and legislation should take into account which colorants and finishing chemicals are
currently removable to enforce their use or restrict the use of others.
In addition, to treat wastewater from textile recycling, advanced composite adsorbents
are utilized for the efficient removal of contaminants. These adsorbents, such as those
incorporating mesoporous silica combined with specific organic ligands, are designed
to selectively capture and separate targeted metal ions, such as ytterbium (Yb(III)) and
samarium (Sm(III)). The composite adsorbents, with high surface areas and specific bonding
capabilities, operate effectively under controlled pH conditions to avoid issues such as
hydroxide precipitation. For instance, the materials exhibit high selectivity and adsorption
capacities, with Yb(III) and Sm(III) ions being successfully removed even in the presence
of other competing ions. Additionally, these adsorbents can be regenerated and reused
multiple times, maintaining their efficiency throughout numerous cycles of adsorption and
elution. This method not only improves the quality of treated water by removing hazardous
metal ions but also offers a sustainable solution for recycling and resource recovery in
textile processing [280–283,300].
Polymers 2025, 17, 628 29 of 94

3.4. Mechanical Recycling

When reuse is no longer possible for a waste textile product, the next-best end-of-life
option is mechanical recycling. Contrary to reuse, mechanical (and chemical) recycling does
not attempt to maintain the waste product but instead breaks it down into materials which
can then be used in manufacturing processes to create new products, whether the same as
the original (primary or closed-loop recycling) or different from the original (secondary or
open-loop recycling) [189,191,192].
According to ISO 472:2013, mechanical recycling specifically includes all recycling
processes that do not cause a significant change in the chemical structure of the polymers
that make up the material [188]. This includes breaking down the waste textile product into
its fabric, yarn, fiber, or polymer building blocks and allowing a classification embedding
physical recycling. In the following sections, the main mechanical recycling methods
are addressed.

3.4.1. Fabric, Yarn, and Fiber Recycling

Textile products can be broken down into fabrics, yarns, or fibers through purely
mechanical processes, such as cutting, pulling, and blending [301,302]. While fabric and
yarn recycling are possible in theory, there is almost no literature on these processes, and
the few sources that do speak of fabric recycling conflate it with remanufacturing, which is
similar in practice but maintains the product as a whole, rather than viewing the fabric as a
secondary raw material output of the end-of-life process.
In contrast, fiber recycling is a well-developed technology and is currently by far
the most used method in industry for the recycling of textile waste, more prevalent than
polymer recycling or any form of chemical recycling [303]. The objective of this technique
is to remove any impurities in textile waste and restore the fibers to their original state so
that they can be reused in the production of new textiles [304]. The main process of this
restoration consists of the tearing and opening or garneting of textiles into loose fibers by
a so-called Garnett machine [305,306], after which the fibers can be respun into yarns or
processed into nonwovens.
Fiber recycling uses almost no chemicals, very little water, and less energy than other
recycling methods, largely because it requires the fewest processing steps to achieve a new
product [60,267]. While this makes fiber recycling the cheapest recycling process, it also
has downsides. For example, the heavy mechanical strain that the fibers experience during
the recycling process causes shortening of the fibers, and a non-recycled fraction of dust is
left over by the process. This reduction in the length of the fiber can pose limitations to its
processability into yarn and means that the fibers have reduced mechanical properties, such
as tensile strength [307]. This is the reason why up to 95% of mechanically recycled fibers
are currently used as flocks in nonwovens or as additives in other products (e.g., bricks),
rather than being respun into lower-quality yarns [308,309]. In other words, due to the
damage sustained by the fibers during mechanical recycling, this method can be considered
open-loop downcycling. Ensuring consistent quality in the recycled fibers produced can
thus be challenging [310].
The only way to achieve open-loop side cycling or closed-loop recycling through
mechanical means is by adding longer virgin fibers to the shortened fibers upon spinning
them into new yarns. Notably, this often still requires at least 50% virgin fibers [311]
because only this can allow the new yarns to achieve the required mechanical properties.
However, studies have pointed out that lubricants (e.g., a polyethylene glycol 4000 aqueous
solution) can be applied to fabrics before shredding to reduce inter-fiber cohesion and
friction and thus reduce the damage caused by the garneting process [311]. In general, this
true closed-loop recycling is attempted only with pre-consumer textile waste that is clean,
Polymers 2025, 17, 628 30 of 94

sorted, and of high purity [312,313]. Despite this reduction in fiber quality, a good approach
to textile recycling would be to allow mechanical fiber recycling until the fiber length has
been reduced to a level at which the material is no longer fit for reuse or for fabric, yarn, or
fiber recycling, and to then cascade into polymer recycling or chemical oligomer/monomer
recycling [189].
While fiber recycling can usually process textile waste with additives, such as colorants
and finishing chemicals, without their removal in the pretreatment step, these additives are
left in the recycled product. This limits the purpose for which the secondary raw material
can be used because it continues to contain the same finishing chemicals, which can affect
the mechanical properties of the recycled fibers [314]. In addition, mixes of unsorted colors
often come out as black or gray [309]. These factors can reduce the value of the secondary
raw material and lead to conflicts with the EU regulation on the registration, evaluation,
authorization and restriction of chemicals (REACH) [267,314].
Similarly, fiber recycling has no easy solution for fiber blends, such as cotton–polyester,
viscose–polyester, or cotton–elastane. Processing these fibers together generally results in
a lower-quality fiber of mixed colors and fiber length [312]. Even pre-consumer blends
can be problematic. This is especially true for any fiber blended with elastane because the
characteristics of the highly elastic elastane fibers are very different from those of other
fibers. As such, most firms send textiles containing elastane straight to landfills rather than
attempting to recycle them [315]. The combination of these factors indicates that a rigorous
pretreatment is required for most textile waste prior to fiber recycling (cf. Section 3.3).
In the current industrial landscape, fiber recycling is applied mostly to fibers of natural
polymers, such as cotton, animal fibers (wool, cashmere, etc.), and man-made cellulose
fibers (viscose, lyocell, viscose, cupro, bamboo viscose, etc.), but it is also applied to
polyester products and waste with combinations of natural polymer fibers and polyester
fibers [316]. Although significant investments in technology and infrastructure are still
necessary to overcome the challenges posed by fiber recycling and to fully achieve its
benefits [317–319], there are already some very successful fiber recycling plants.
At Hilaturas Ferre in Spain, for example, pre-consumer cotton waste (and, optionally,
a small amount of post-consumer waste) is recycled into staple fibers of 10–15 mm in length,
which can be blended with acrylic or (recycled) polyester fibers to produce new yarns
with 90% recycled content [320]. They also have plants for recycling polyester and wool
from post-industrial sources [289]. Similarly, Pure Waste in Finland recycles pre-consumer
cotton waste via shredding, and the company claims to be able to produce 100% recycled
yarns, which can be mixed with recycled polyester or viscose yarns for the production of
clothing [321].

3.4.2. Polymer Recycling via Melting

After fiber recycling, the next method in the waste treatment hierarchy is polymer
recycling (see Figure 9) [195]. This entails the breaking down of fibers into their constituent
polymers without further degrading the polymers in any pronounced way, after which
they can again be extruded into fibers. As such, polymer recycling is often called re-
extrusion. This is still considered mechanical recycling because the chemical structure of
the polymer remains intact [188]. Because polymers can be used as the input material for
the same product or an entirely different product, polymer recycling can be both closed-
loop (primary) and open-loop (secondary) recycling. In the latter case, an effort is usually
made at upcycling or side cycling, but downcycling is also possible.
The most straightforward way for fibers to be broken down into polymers is by
melting them and applying mechanical forces to them. This is specifically referred to as
thermomechanical recycling in ISO 5157:2023 [186]. It is a widely used method of me-
Polymers 2025, 17, 628 31 of 94

chanical recycling, particularly for fibers of synthetic polymers [322,323], more specifically
polycondensation polymers such as PET and polyamide [324–326].
Polymers 2025, 17, x FOR PEER REVIEW The general process is very similar to the virgin extrusion of thermoplastic polymers, 33 of 104 with
differing input materials. In this case, pretreated waste fibers are usually cut, compressed into
small balls or pills, dried, and then fed into a screw extruder, which melts and immediately
and immediately
extrudes extrudes
the polymer (cf. the polymer (cf.
Man-Made Man-Made
Fibers FibersPolymers
of Synthetic of Synthetic Polymers
Section) Sec-While
[327].
tion) [327]. While compression makes the feeding easier, it also requires an
compression makes the feeding easier, it also requires an extra step, labor, and energy, and extra step,
labor,
is thusand energy, and
sometimes is thus
ignored sometimes
[328]. For lessignored [328]. material,
compressed For less compressed material, extruder
using a twin-screw us-
ing a twin-screw extruder can be beneficial [327]. The process is shown in Figure
can be beneficial [327]. The process is shown in Figure 13. Note that nonfibrous waste can 13. Note
that be
also nonfibrous
recycled waste can also
into fibers be recycled
via this method,intoand fibers viamethod
that this this method, andmore
is in fact that common
this
method
than is in fact more
fiber-to-fiber common
polymer than fiber-to-fiber
recycling polymer
in the current recycling
industry, in the current
particularly for indus-
PET bottle
try, particularly for PET bottle waste [328].
waste [328].

Figure Re-extrusionofoffibers
13. Re-extrusion
Figure 13. fibers from
from PET
PET bottle
bottle or textile
or textile waste.
waste.

A major
A majorbenefit
benefitofofthe
thethermomechanical
thermomechanical polymer
polymer recycling
recycling process
process is it
is that that it is much
is much
simpler, cheaperand
simpler, cheaper andrequires
requiresfewerfewer chemicals
chemicals thanthan
anyany chemical
chemical recycling
recycling process.
process. In In
addition,
addition, thetheeconomic
economic value
value of recycled
of recycled fibersfibers is generally
is generally higher
higher than thatthan thatorig-
of fibers of fibers
originating
inating fromfrom mechanical
mechanical fiber (instead
fiber (instead of polymer)
of polymer) recyclingrecycling
methods. methods. This is the
This is because because
re-extruded
the re-extrudedfibersfibers
do notdo suffer
not from
suffer thefrom
mechanical damage ordamage
the mechanical fiber shortening
or fiber associ-
shortening
ated with the
associated withmechanical shredding
the mechanical of fabrics.
shredding With suitable
of fabrics. care, the care,
With suitable resulting fibers canfibers
the resulting
rivalrival
can the quality of virgin
the quality fibersfibers
of virgin [329]. [329].
In
In practice,
practice,however,
however,several
several degradation
degradation reactions can can
reactions occur during
occur re-extrusion.
during re-extrusion.
Excess friction inside an extruder can lead to mechanical degradation
Excess friction inside an extruder can lead to mechanical degradation of the polymer, of the polymer, re-
action with oxygen at high temperatures can lead to thermo-oxidation
reaction with oxygen at high temperatures can lead to thermo-oxidation of the polymer, of the polymer, and
any water in the input material can lead to hydrolysis of the polymer. To address these
and any water in the input material can lead to hydrolysis of the polymer. To address these
problems, respectively, special screw designs and force feeders can be used, the re-extru-
problems, respectively, special screw designs and force feeders can be used, the re-extrusion
sion can be performed in an inert nitrogen (N2) gas atmosphere, and the material can be
can be performed in an inert nitrogen (N2 ) gas atmosphere, and the material can be dried
dried more thoroughly to a very low level of residual moisture (below 0.1 g of water per
more thoroughly to a very low level of residual moisture (below 0.1 g of water per kg of
kg of fibers) [327,328,330].
fibers) [327,328,330].
Aside from the aforementioned risks of any re-extrusion process, certain waste fibers
Aside
can also fromcontaminations,
contain the aforementioned such asrisks of any
other re-extrusion
polymers process,
(e.g., PVC, even at certain
levelswaste
as lowfibers
can also
as 100 contain
ppm, contaminations,
with hydrochloric such as
acid (HCl) other
being polymers
released), (e.g.,
carbon PVC, even
particles, at levels
pigments, dye-as low
as 100 ppm, with hydrochloric acid (HCl) being released), carbon
stuffs, Sb2O3 catalyst residue, stabilization agents, and flame retardants. These contamina- particles, pigments,
dyestuffs,
tions can allSb 2 O3 re-extruded
cause catalyst residue, stabilization
fibers to turn yellowagents, and flame
or gray [331] and thusretardants. These con-
pose challenges
taminations can all
for the production of cause
recycled re-extruded
textiles with fibers
whitetoorturn yellow
pastel shadesor[332].
gray [331] and thus pose
challenges
Some of forthe
theaforementioned
production of damagerecycledwill textiles with white and
be unavoidable or pastel
lead toshades [332].in
a decrease
the viscosity of the melt and the average molar mass of the polymers within it. As a result,
it can be necessary to increase (or prevent a further decrease in) the average molar mass
before or during re-extrusion, either through the addition of stabilizers or certain chemical
processes, until it reaches the correct average molar mass range suitable for fibers [157].
Polymers 2025, 17, 628 32 of 94

Some of the aforementioned damage will be unavoidable and lead to a decrease in

the viscosity of the melt and the average molar mass of the polymers within it. As a result,
it can be necessary to increase (or prevent a further decrease in) the average molar mass
before or during re-extrusion, either through the addition of stabilizers or certain
Polymers 2025, 17, x FOR PEER REVIEW 34 ofchemical
104
processes, until it reaches the correct average molar mass range suitable for fibers [157]. For
instance, the SSP or LSP process can be utilized to increase the average molar mass of PET
and polyamide,
For instance, the although
SSP or LSPthe high operational
process can be utilizedandto equipment
increase thecosts of both
average molarprocesses
mass of can
PET
be and polyamide,
significant although
obstacles, the hightheir
particularly operational and equipment
high energy costs of both processes
costs [333].
can be
A significant
more common obstacles, particularly
process is reactivetheir high energy
extrusion (REX),costs [333]. other molecules known
whereby
A more
as chain common
extenders (CEs)process is reactive
are added to theextrusion
waste polymer whereby other
(REX), [334–336]. molecules
Generally, CEs are
known as chain extenders (CEs) are added to the waste polymer [334–336].
bifunctional or multifunctional compounds that can link with the terminal functional Generally, CEs
are bifunctional
groups or multifunctional
of polymers. compounds
CEs can be either that can linkcompounds
low-molar-mass with the terminal functional
or macromolecules.
groups of polymers. CEs can be either low-molar-mass compounds or macromolecules.
Linear CEs are useful for fiber grades because they can enhance the chain alignment and
Linear CEs are useful for fiber grades because they can enhance the chain alignment and
crystallinity of the drawn fibers [337].
crystallinity of the drawn fibers [337].
Figure 14 shows an example of a chain extension of recycled PET using pyromellitic
Figure 14 shows an example of a chain extension of recycled PET using pyromellitic
dianhydride (PMDA), a common CE [338]. The primary suitable CEs for polyamide include
dianhydride (PMDA), a common CE [338]. The primary suitable CEs for polyamide in-
biscaprolactam [339], bisoxazolines [340], and a combination of the two [339]. PMDA [338],
clude biscaprolactam [339], bisoxazolines [340], and a combination of the two [339].
bisoxazolinones [326], different
PMDA [338], bisoxazolinones phosphides
[326], [326], bisoxazines
different phosphides [339], bisoxazolines
[326], bisoxazines [339], bisoxa-[341],
epoxidic multifunctional
zolines [341], oligomer [342],
epoxidic multifunctional bisepoxides
oligomer [339], and isocyanate
[342], bisepoxides [343] are some
[339], and isocyanate
suitable CEs for PET. In some cases, the use of CEs can lead to the formation
[343] are some suitable CEs for PET. In some cases, the use of CEs can lead to the formation of by-
products, foreign
of by-products, building
foreign blocks,
building andand
blocks, a broader
a broadermolar
molarmass
mass distribution
distribution orormolec-
molecular
weight distribution
ular weight (MWD),
distribution (MWD),which
whichcan affect
can affectplastic
plasticproperties, causingmore
properties, causing moreshrink-
shrinkage.
Therefore, under
age. Therefore, REXREX
under conditions, vacuum
conditions, vacuum evaporation
evaporationshould
shouldbe beemployed
employed to to remove
re-
by-products [344]. [344].
move by-products

Figure 14.
Figure 14. The
The chain
chainextension
extensionofofrecycled PET
recycled using
PET PMDA
using [338].
PMDA [338].

Furthermore, Lee et al. [345]

Furthermore, [345] applied
applied aminopropyl-functionalized
aminopropyl-functionalized polyhedral
polyhedraloligo-oligomeric
meric silsesquioxanes
silsesquioxanes as suitable
as suitable CEs.
CEs. By By using
using this nanoparticle-nucleating
this nanoparticle-nucleating agent,
agent, thethe
crystal-
crystallization
lization ratetemperature
rate and and temperature of PET
of PET could
could be increased
be increased 2.72.7
andand1.21.2times,
times,respectively.
respec-
tively. Similarly,
Similarly, Makkam Makkam and Harnnarongchai
and Harnnarongchai [346][346]
usedused an acrylic
an acrylic epoxy
epoxy resinasasa aCE
resin CEto in-
to increase
crease the average
the average molarmolar
massmass of The
of PET. PET.results
The results indicated
indicated thatCE
that the thecanCEbecan be ac-
accompanied
companied by chain branching or even cross-linking. They found that the
by chain branching or even cross-linking. They found that the MWD and gel content MWD and gel of
content of modified PET increased when the concentration of acrylic epoxy resin was in-
modified PET increased when the concentration of acrylic epoxy resin was increased. How-
creased. However, the melt re-extrusion recycling process has a major limitation: It can be
ever, the melt re-extrusion recycling process has a major limitation: It can be directly used
directly used only for pure thermoplastic fibers (e.g., PET, polyamide, and PP). Fiber
only for pure thermoplastic fibers (e.g., PET, polyamide, and PP). Fiber blends cannot be
blends cannot be easily processed if the flow properties of their melts and/or their melting
easily processed if the flow properties of their melts and/or their melting temperatures
temperatures are too different (they can preferably differ by, at most, 10–20 °C). Thus,
◦ C). Thus, extensive fiber
are too different (they can preferably differ by, at most, 10–20
extensive fiber separation during pretreatment is necessary. Any remaining finishing or
coating products on the fibers will also cause degradation during re-extrusion. Thus, un-
der this recycling method’s conventional conditions, it is not an option for natural poly-
mers, thermoset synthetic polymers, more complex textile blends, or coated fabrics [327].
 Polymers 2025, 17, x FOR PEER REVIEW 35 of 104

Polymers 2025, 17, 628 33 of 94

3.4.3. Polymer Recycling via Dissolution

As discussed in Section 3.4.2, the main goal of any polymer recycling process for tex-
separation during pretreatment is necessary. Any remaining finishing or coating products
tile waste is the recovery of the polymers that make up the fibers in a liquid form so that
on the fibers will also cause degradation during re-extrusion. Thus, under this recycling
they can be re-extruded into new fibers. As an alternative to melting, this liquefaction can
method’s conventional conditions, it is not an option for natural polymers, thermoset
be achieved by dissolving the waste fibers into a suitable solvent. This method of recycling
synthetic polymers, more complex textile blends, or coated fabrics [327].
is applicable for polymers that cannot melt—because, for example, they would degrade
before reaching their melting temperature—while being soluble in a suitable solvent. It
3.4.3. Polymer Recycling via Dissolution
excludes many thermoset polymers, whose cross-linked network structure prevents dis-
As discussed
solution in Section
[269]. As such, 3.4.2, the main
this dissolution goal ofaany
still covers wide polymer
span of recycling
fiber types, process
but in for
prac-textile
waste
tice, this recycling method is currently applied at a commercial scale only to cotton andthey
is the recovery of the polymers that make up the fibers in a liquid form so that
can be re-extruded
sometimes polyesterinto wastenew fibers. As
[347–349]. an alternative
Several pilot plantstoormelting,
small-scalethisoperations
liquefaction can be
do ex-
achieved
ist for otherby textile
dissolvingtypes,thesuchwaste fiberstextiles
as acrylic into a suitable solvent.
(Thai Acrylic Fibre This
Co.method
Regel inof recycling is
Bangkok,
applicable for polymers that cannot melt—because, for example,
Thailand [350]), PP and PE textiles (Obbotec-SPEX in Rotterdam, The Netherlands [351]), they would degrade before
reaching
PP textiles their melting Technologies
(PureCycle temperature—while in Orlando, being soluble
Florida, USAin a[352]),
suitable
andsolvent. It excludes
aramid textiles
(Teijinthermoset
many Aramid inpolymers,
Arnhem, whose The Netherlands
cross-linked [353]), each utilizing
network structuredifferent
preventsdissolution
dissolution re-[269].
Asactors
such,and thisparameters,
dissolutionwhich the companies
still covers a wide span do not disclose.
of fiber types,Inbutgeneral, however,
in practice, thisdisso-
recycling
lution happens
method in approximately
is currently 30 min (afterscale
applied at a commercial pretreatment) and isand
only to cotton conducted
sometimes below the
polyester
solvent’s boiling temperature [354].
waste [347–349]. Several pilot plants or small-scale operations do exist for other textile
types,Cotton
such as consists
acrylicoftextiles
cellulose, which
(Thai can be
Acrylic suspended
Fibre Co., Regel in ain
liquid and then
Bangkok, re-extruded
Thailand [350]), PP
into man-made cellulose fibers by means of wet spinning [267]. Cellulose
and PE textiles (Obbotec-SPEX in Rotterdam, The Netherlands [351]), PP textiles (PureCycle has low solubil-
ity in most chemical solvents due to the strong H2 bonds between its molecules; thus, it is
Technologies in Orlando, FL, USA [352]), and aramid textiles (Teijin Aramid in Arnhem,
necessary to first weaken or disrupt the H2 bonding to increase the dissolution rate (an
The Netherlands [353]), each utilizing different dissolution reactors and parameters, which
example is shown in Figure 15) [355]. This means that specialized solvent systems are
the companies do not disclose. In general, however, dissolution happens in approximately
required to facilitate the dissolution of cellulose, depending on various factors, such as the
30 min (after pretreatment) and is conducted below the solvent’s boiling temperature [354].
dissolution rate and temperature, pretreatment, and the rate of cellulose degradation dur-
Cotton consists of cellulose, which can be suspended in a liquid and then re-extruded
ing dissolution [40,355]. Common solvents include a cuprammonium solution (leads to
into man-made cellulose
cuprammonium fibers), NMMO fibers (leads
by means of wetand
to lyocell), spinning [267]. (ILs;
ionic liquids Cellulose
leads tohas low solu-
Ioncell-
bility in most
F ) [194,356].
® chemical solvents due to the strong H 2 bonds between its molecules; thus,
it is necessary
Cellulose to canfirst
alsoweaken
be slightlyor disrupt the H2 bonding
depolymerized to increase
without breaking the dissolution
it down entirely to rate
(an example is shown in Figure 15) [355]. This means that specialized
glucose, or its chemical structure can be modified to make dissolution easier. This leads solvent systems
are required
to mixed to facilitate the dissolution
chemical–mechanical of cellulose,
recycling results, as is thedepending
case for theon various factors,
well-known viscosesuch
as the dissolution
process. This process rateuses
andcellulose-xanthate
temperature, pretreatment, and thethrough
as an intermediate rate of treatment
cellulose degrada-
with
carbon
tion duringdisulfide and subsequent
dissolution [40,355]. dissolution into NaOH
Common solvents (leads atocuprammonium
include viscose or modal), or
solution
through
(leads treatment with urea
to cuprammonium fibers), N2O), leading
(CH4NMMO (leadstotoalyocell),
cellulose-carbamate
and ionic liquids intermediate
(ILs; leads
towhich can be
Ioncell-F ® ) dissolved
[194,356].into NaOH (leads to carbamate) [194].

Figure 15. Dissolution of cellulose in an ionic liquid using the anti-H2 bonding mechanism [357].

Cellulose can also be slightly depolymerized without breaking it down entirely to

glucose, or its chemical structure can be modified to make dissolution easier. This leads
to mixed chemical–mechanical recycling results, as is the case for the well-known viscose
Polymers 2025, 17, 628 34 of 94

Polymers 2025, 17, x FOR PEER REVIEW 36 of 104

process. This process uses cellulose-xanthate as an intermediate through treatment with

carbon disulfide and subsequent dissolution into NaOH (leads to viscose or modal), or
Figure 15.treatment
through Dissolutionwith of cellulose
urea (CH in anN ionic liquid using the anti-H2 bonding mechanism [357].
4 2 O), leading to a cellulose-carbamate intermediate
which can be dissolved into NaOH (leads to carbamate) [194].
In the literature, various strong acidic, basic, and ionic solvents have been investi-
In the literature, various strong acidic, basic, and ionic solvents have been investigated
gated for the polymer recycling of waste cotton textiles, such as phosphoric acid
for the polymer recycling of waste cotton textiles, such as phosphoric acid (H3 PO4 )/H2 O,
(H3PO4)/H2O, ILs, trifluoroacetic acid (CF3CO2H), H2O/H2SO4, H2O/NaOH/CH4N2O,
ILs, trifluoroacetic acid (CF3 CO2 H), H2 O/H2 SO4 , H2 O/NaOH/CH4 N2 O, CS2 /NaOH,
CS2/NaOH, H2O/lithium hydroxide (LiOH)/CH4N2O, and dimethylacetamide
H2 O/lithium hydroxide (LiOH)/CH4 N2 O, and dimethylacetamide (DMAc)/lithium chlo-
(DMAc)/lithium chloride (LiCl). As shown in Figure 15, cellulose is dissolved using ILs
ride (LiCl). As shown in Figure 15, cellulose is dissolved using ILs by repelling negatively
by repelling negatively charged anion–cellulose complexes through electrostatic forces
charged anion–cellulose complexes through electrostatic forces and by condensing the
and by condensing the IL cation around these complexes, leading to steric and solvopho-
IL cation around these complexes, leading to steric and solvophobic interactions. Some
bic interactions. Some solvents, such as H2O/NaOH/CH4N2O and H2O/H2SO4, have ena-
solvents, such as H2 O/NaOH/CH4 N2 O and H2 O/H2 SO4 , have enabled rapid cellulose
bled rapid cellulose dissolution at low temperatures, whereas the LiCl/DMAc system can
dissolution at low temperatures, whereas the LiCl/DMAc system can dissolve cellulose
dissolve cellulose without the need for pretreatment. Despite their advantages, all the sol-
without the need for pretreatment. Despite their advantages, all the solvents mentioned
vents mentioned
above have certain above have certain
drawbacks. drawbacks.
For instance, the For
NaOH instance,
system thehasNaOHlimited system has lim-
cellulose sol-
ited cellulose
ubility and issolubility
unable toand is unable
dissolve to dissolve
cellulose with acellulose
high degree with aofhigh degree of polymer-
polymerization, while
ization, whileisNaOH/CS
NaOH/CS 2 is a derivatizing solvent that causes severe pollution. Moreover,
a derivatizing solvent that causes severe pollution. Moreover, ILs and
2
ILs and DMAc/LiCl
DMAc/LiCl are not yet are economically
not yet economically feasible feasible due to
due to their hightheir high
costs costs [104,357].
[104,357].
Theoretically, the aforementioned solvent-based
Theoretically, the aforementioned solvent-based polymer recycling processes polymer recycling processes need need
not be
not be limited
limitedtotocotton, cotton,and and anyanycellulose-based
cellulose-based textile waste
textile wastecancanbe used as anas
be used input (e.g.,
an input
(e.g., virgin man-made cellulose fibers or wood fibers), but these sources of cellulosevary
virgin man-made cellulose fibers or wood fibers), but these sources of cellulose can can
slightly
vary in chemical
slightly structure
in chemical and lead
structure andtolead
different viscosities
to different in the dissolved
viscosities in the dissolvedstate, which
state,
wouldwould
which necessitate adaptations
necessitate in the recycling
adaptations process
in the recycling or pretreatment;
process or pretreatment; thus, cotton is the
thus, cotton
only
is themajor
only majorinput input
for these processes
for these to date
processes to[358].
date [358].
In recent years, there has been a
In recent years, there has been a significant focus significant focus on on the
the process
process of of dissolution
dissolution for for the
the
removal of
removal of impurities
impurities with with inorganic
inorganic or or organic
organic origins
origins from from polymeric
polymeric textiletextile waste
waste to to
allow the separated polymer to be recycled more efficiently.
allow the separated polymer to be recycled more efficiently. For example, the dissolution For example, the dissolution
recycling of
recycling of polyolefins
polyolefins is is being
being researched.
researched.ItIthas hasthethepotential
potential to tobebehighly
highly effective
effective in
removing impurities, separating cross-linked chains, and reducing
in removing impurities, separating cross-linked chains, and reducing gel content [359,360]. gel content [359,360].
Moreover, dissolution
Moreover, dissolution recycling
recycling can can help
help eliminate
eliminate contaminants
contaminants such such as as dyes
dyes andand addi-
addi-
tives, which enables in situ catalytic pyrolysis of polyolefins
tives, which enables in situ catalytic pyrolysis of polyolefins and greatly reduces the and greatly reduces the costs
costs
associated with
associated with pyrolysis
pyrolysis [361–363].
[361–363].
Dissolution recycling
Dissolution recycling has has the
the advantage
advantage of of requiring
requiring less less pretreatment
pretreatment compared compared to to
many other
many other recycling
recycling methods.
methods. It It can
can accept
accept material
material input
input of of any
any fabric
fabric structure
structure (woven,
(woven,
knitted, nonwoven, etc.) without cutting it to size, and
knitted, nonwoven, etc.) without cutting it to size, and it is often tolerant of it is often tolerant of dyed
dyed textiles
textiles
because the
because the colors
colors can can bebe removed
removedor orbleached
bleachedduringduringthe therecycling
recyclingprocess,
process,asaslong long asasit
is known which dyes were used [358]. Alternatively, the
it is known which dyes were used [358]. Alternatively, the color can be maintained or color can be maintained or re-
generated (in(inthe
regenerated theabsence
absenceofofcolor),
color),significantly
significantlyreducing
reducingthe thecost
cost ofof any
any future dyeing
future dyeing
processes if the same color is desired [349]. However, dissolution
processes if the same color is desired [349]. However, dissolution recycling still requires the recycling still requires
the removal
removal of hardof hardpartsparts (buttons,
(buttons, zippers,
zippers, etc.),etc.),
and theandprocess
the processyield yield
is highlyis highly depend-
dependent on
ent on the purity of the input material, so sorting
the purity of the input material, so sorting is still very important [358]. is still very important [358].
The most
The most important
important advantage
advantage of dissolution recycling
of dissolution recycling is is that
that it can deal
it can deal with
with fiber
fiber
blends without making the process too complex. This
blends without making the process too complex. This requires the use of a solvent requires the use of a solvent that
selectively
that selectively dissolves
dissolvesoneone fiberfiberwithout
without dissolving
dissolvingthe theothers.
others. For For example,
example, H H22SO
SO44,,
NaOH/CH 4N 2 O, and LiCl/DMAc solvent systems are under
NaOH/CH4 N2 O, and LiCl/DMAc solvent systems are under investigation for the selective investigation for the selective
dissolution of
dissolution of elastane
elastane out out of of cotton–elastane
cotton–elastane blends blends [364].
[364]. Similarly,
Similarly, tetrahydrofurfuryl
tetrahydrofurfuryl
alcohol and ɣ-valerolactone
alcohol and -valerolactone are green solvents that have been found to be
are green solvents that have been found to be capable
capable of of dis-
dis-
solving elastane with an efficiency comparable to that of classical
solving elastane with an efficiency comparable to that of classical solvents (DMF, DMAc), solvents (DMF, DMAc),
allowing for
allowing for thethe selective
selective dissolution
dissolution and and recycling
recycling of of polyester–elastane
polyester–elastane and and polyamide–
polyamide–
elastane blends [40]. The most common blended materials for dissolution recycling, how-
elastane blends [40]. The most common blended materials for dissolution recycling, how-
ever, contain cotton and polyester, specifically the so-called polycotton blend. In this case,
selective dissolution of the cotton fraction is usually applied, while the undissolved PET
is filtered, dried, and subsequently recycled on its own or converted into a derivative
Polymers 2025, 17, 628 35 of 94

ever, contain cotton and polyester, specifically the so-called polycotton blend. In this case,
selective dissolution of the cotton fraction is usually applied, while the undissolved PET
is filtered, dried, and subsequently recycled on its own or converted into a derivative
compound [365]. Processes that selectively dissolve the PET do exist (e.g., using sulfolane
or a switchable hydrophilicity solvent), but they have been reported to reduce the quality of
the cellulose fibers [349,366,367]. PET is also more easily recycled via the melt re-extrusion
process [365]. Two examples of companies that selectively dissolve cotton in this way
are Worn Again Technologies in Nottingham, the UK [368] and Textile Change in Vejle,
Denmark [369].
Selective dissolution is valid not only for fiber blends but also for materials with
significant nonfibrous polymer fractions, such as fiber-reinforced composites or carpets. For
example, polyamide carpets can be recycled by selectively dissolving the fibers in sulfuric,
formic or hydrochloric acid (H2 SO4 , CH2 O2 , or HCl) and subsequently precipitating them
in water [370].
While dissolution recycling has the advantage of being able to produce pure polymers
of virgin-like quality, this requires more water and energy than a process such as fiber
recycling, and it necessitates larger scales to ensure its economic viability [194]. Additionally,
the polymer quality is virgin-like only to a limited extent. Research has shown that polymers
degrade with each subsequent attempt at dissolution [312,371], meaning that the process
cannot be continued ad infinitum, thus making room for chemical recycling. This unwanted
degradation can be minimized or avoided with good process design, such as in the process
employed by Teijin Textiles in Japan, which has developed a method to dissolve PET and
create recycled PET fibers with limited loss in quality [372]. More commonly, however,
other input materials are added instead of processing 100% textile waste. Cotton dissolution
recycling, for example, is usually improved by the addition of at least 50% virgin wood
pulp to cotton pulp [373].
Furthermore, Yousef et al. [374] developed a sustainable technique for extracting
cotton from textile waste, which can serve as a new material source that guarantees good
quality and economic feasibility. The method consists of three key steps: HNO3 leaching,
dimethyl sulfoxide dissolution, and sodium hypochlorite and HCl bleaching. These steps
were employed to eliminate textile dyes, dissolve the polymeric portion, and release the
cotton fibers. It was claimed that the demonstration of the technology at the pilot scale not
only illustrated its industrial potential to achieve self-sufficiency in raw cotton fiber but
also facilitated the transition to a circular economy.
Liu et al. [348] applied alkali (LiOH or NaOH)/CH4 N2 O aqueous systems as solvents
to physically recycle cotton waste. Post-consumer cotton fabrics underwent hydrolysis
using H2 SO4 and were dissolved in these solvents to produce man-made fibers via wet
spinning. The man-made fibers showed a change in thermal stability, indicating structural
modification due to the hydrolysis and dissolving processes. Mechanical testing revealed
that the as-spun man-made fibers (without a drawing process) had similar tenacity and com-
petitive elongation to commercially available regular viscose fibers. A low drawing ratio of
1.3 resulted in a 50% increase in fiber tenacity, indicating the potential to produce stronger
fibers from cotton waste using industrial wet-spinning facilities and higher drawing ratios.
The thermal behaviors of the original, hydrolyzed, and man-made fibers were evaluated
using thermogravimetric analysis (TGA). The samples demonstrated a significant weight
loss (between 300 ◦ C and 400 ◦ C), corresponding to cellulose thermal decomposition, and
the residual char increased at varying levels from hydrolysis to regeneration, yielding about
8–18% at 600 ◦ C (Figure 16).
Polymers 2025,
Polymers 17,17,
2025, 628x FOR PEER REVIEW 38 of 104
36 of 94

Figure 16. Thermogravimetric

Figure16. Thermogravimetric analysis
analysiscurves
curvesfor
fororiginal,
original,hydrolyzed,
hydrolyzed,and
andman-made
man-madecotton
cottonfibers
fibers[348].
[348].
Yousef et al. [284] also conducted a study in which they employed an integrated and
sustainable
Yousefchemical
et al. [284]process to recover
also conducted pure cotton
a study in which andtheyPET fibers from
employed textile waste.
an integrated and The
process involved
sustainable chemicaltheprocess
removal to of textilepure
recover dyes fromand
cotton thePET
textile
fibersusing
fromacid and
textile regenerating
waste. The
process
the spentinvolved
acid with theACremoval of textile
to restore dyes from
its original the textile using
concentration acid The
(83%). and researchers
regeneratingthen
the spent
utilized acid with
a green AC to restore
dissolution process its with
original concentration
a switchable (83%). The researchers
hydrophilicity solvent to then
dissolve
utilized
the a green dissolution
PET material and liberate process with a and
high-purity switchable
thermallyhydrophilicity
stable cotton solvent
fibers.toThe
dissolve
solvent’s
the PET material
hydrophilicity wasand liberate
altered tohigh-purity
extract PETand from thermally stable reducing
the solution, cotton fibers.
powerThe consumption
solvent’s
hydrophilicity was altered to extract PET from the solution,
and PET degradation compared to conventional solvents. The study revealed that cottonreducing power consumption
and PET
fibers anddegradation
PET constituted compared 84%toand conventional
16% of thesolvents. The study revealed
fabric, respectively, with athat cotton rate
recycling
fibers and PET constituted 84% and 16% of the fabric, respectively, with a recycling rate
exceeding 96%.
exceeding 96%.
Haslinger et al. [375] applied physical recycling to effectively separate cotton from
Haslinger et al. [375] applied physical recycling to effectively separate cotton from
PET. They used 1,5-diazabicyclo [4.3.0] non-5-enium acetate ([DBNH][OAc]) to selectively
PET. They used 1,5-diazabicyclo [4.3.0] non-5-enium acetate ([DBNH][OAc]) to selectively
dissolve the cotton component and then performed dry-jet wet spinning of cellulose to
dissolve the cotton component and then performed dry-jet wet spinning of cellulose to
produce textile-grade fibers. The spun fibers were found to possess properties similar to
produce textile-grade fibers. The spun fibers were found to possess properties similar to
those
those of
of lyocell. ThePET
lyocell. The PETfraction
fractionrecovered
recovered fromfrom thethe process
process hadhad a low
a low cellulose
cellulose content
content
(1.7–2.5 wt%). However, the PET material dispersed in [DBNH][OAc]
(1.7–2.5 wt%). However, the PET material dispersed in [DBNH][OAc] underwent visible underwent visible
degradation,
degradation, as as evidenced
evidencedby byaadecrease
decreaseinin itsits average
average molarmolar mass mass
andand tensile
tensile properties
properties
(ca.
(ca. up to 50%). The results demonstrate that blended textile waste containing cellulose has
up to 50%). The results demonstrate that blended textile waste containing cellulose
the
haspotential to serve
the potential to serveas aasfeedstock
a feedstock forfor
conventional
conventionalfiber fiberspinning
spinning processes.
processes. In Ingen-
general,
physical recycling
eral, physical is one
recycling is of
one theof feasible approaches
the feasible approaches forforseparating
separating natural
naturalandandman-made
man-
fibers
madefrom
fiberssynthetic fibers,fibers,
from synthetic such as polyester,
such in mixed
as polyester, fibers.
in mixed In this
fibers. In context, Table
this context, 3 shows
Table
3 shows
the the potential
potential of this approach
of this approach to release to release
mixed mixed fiberseach
fibers from fromother.
each other.
Polymers 2025, 17, 628 37 of 94

Table 3. Overview of physical recycling (dissolution) of textile wastes.

Complementary
Process
Fiber Solvent Feed/Solvent Processes and Products Advantages Ref.
Conditions
Pretreatments
The IL was recovered.
Cotton can be regenerated using water as the
coagulated solvent.
Blends of polyester 80 ◦ C,
AMIMCl 1 2–10 wt% - Cotton, polyester Selective dissolution of the cotton component [376]
and cotton 6h
using ionic liquid.
Fully recovered and almost-pure polyester
and cotton.
The polyesters were purified as fibers after
the NMMO treatments.
Two-day enzymatic
Polyester, Up to 95% of the cellulose fibers were
An orange 50:50 polyester– hydrolysis (yield: 85%)
cotton, regenerated and collected.
cotton blend and a blue 120 ◦ C, and one-day
NMMO 2 18 wt% viscose, It is possible to recover the solvent efficiently. [377]
40:60 polyester–viscose 2h fermentation (yield:
ethanol, This process might be economically feasible.
blend 89%) of the man-made
biogas Possible NMMO degradation and cellulose
cotton and viscose
oxidation, and requires antioxidants
for stabilization.
Cotton components can be directly dissolved
and regenerated.
The recovered PET fibers can be recycled and
Waste 80 ◦ C,
AmimCl 3 4 wt% - PET, cotton reused in textiles. [378]
polyester-cotton jeans 3h
The resulting cellulose solution dope can be
used for dry-jet wet spinning to obtain
lyocell-type fibers.
One hundred percent of the disperse dyes,
acid dyes, and direct dyes were separated
DMSO, ethylene
from PET, PA6,6, and cotton, respectively.
Dyed PET, cotton, carbonate, 80–100 ◦ C,
20 wt% - Decolorized fibers Dye removal did not change the structures or [362]
PA6,6 fibers glycerol, 0.5 h
dyeability of the dyes.
tetramethylurea
The molecular weights of the polymers after
dye removal were almost the same.
Polymers 2025, 17, 628 38 of 94

Table 3. Cont.

Complementary
Process
Fiber Solvent Feed/Solvent Processes and Products Advantages Ref.
Conditions
Pretreatments
The solubility of a solvent system is also
strongly influenced by the molecular weight
of the cellulose.
The use of a binary solvent containing a low
80 ◦ C, NaOH hydrolysis, IL amount reduces the drawbacks
Colored waste garment [Bmim]OAc/DMSO Max. 18 wt% Decolorized fibers [349]
0.5 h wet spinning (e.g., high dope viscosity).
The binary solvent reduces the cost of the
solvent by 77%.
The solvent can be recovered and
reused via distillation.
A green dissolution process was employed to
dissolve polyester.
Polyester was extracted from the solution by
Decolorized cotton changing the hydrophilicity of the solvent.
Blue waste jeans 1/40– 50 ◦ C,
DMCHA 4 Dye leaching (HNO3 ) fiber and polyester The recycling rate of the [284]
(80/20 cotton/polyester) 1/120 g·mL−1 full dissolution
with high purity technology was >96%.
The economic returns are up to $1629/ton of
waste, and the carbon footprint is reduced by
1440 kg of CO2 -eq/t of waste.
1 1-allyl-3-methylimidazolium chloride; 2 N-methylmorpholine-N-oxide; 3 1-allyl-3-methylimidazolium; 4 N,N-dimethylcyclohexylamine.
Polymers 2025, 17, 628 39 of 94

3.5. Chemical Recycling: Monomer/Oligomer Recycling

Chemical recycling breaks down textiles into their chemical building blocks or
oligomers, allowing them to be reused in valuable processes. Commercial polymers,
produced through chain-growth or step-growth polymerization, differ in their chemi-
cal structures, with the former having hydrocarbon backbones and the latter featuring
functional groups within the chain.
Given the diverse applications of polymers in textiles—such as fibers, adhesives, and
labels—this section provides an overview of polymer degradation mechanisms, divided
into six categories (A–F) based on chemical composition (Figure 17). Next, key chemical re-
cycling methods like pyrolysis, gasification, solvolysis, and biological recycling techniques
are reviewed.

3.5.1. Degradation Mechanisms for Different Polymer Categories

Category A polymers are saturated polymers with a hydrocarbon backbone and
side groups connected to the backbone through a carbon bond, as shown in Figure 17
(Category A), highlighting the potential location of the initial scission (also known as fis-
sion). In these polymers, the tertiary carbons (if present) determine the preferred scission
point of the polymer chains [379–381]. Bulky functional groups in polystyrene (PS) and
PMMA can guide chain scission toward almost-full depolymerization and monomer recov-
ery [382–387]. The thermal decomposition of polyolefins at moderate temperatures results
in the creation of waxy pyrolysis oils [388–390]. However, increasing the temperature
can lead to the production of lighter olefins [361,391]. Under typical circumstances, coke
formation during the pyrolysis of this polymer category can be disregarded [392].
Category B polymers possess side functional groups connected to the backbone
through heterogeneous atoms (Cl, O; Figure 17, Category B). The initial scissions in the
degradation of this category occur primarily in the side groups and the formation of a
polyene. The chain backbone contains many double bonds, leaving the remaining polyene
susceptible to cross-linking reactions and coke formation. The degradation process for
this category involves three distinct stages: the release of heterogeneous atoms, cross-
linking, and degradation (Figure 17, Category B). Figure 18 shows the mechanism of PVC
degradation and the formation of polyene.
Polymers 2025, 17, 628 40 of 94
Polymers 2025, 17, x FOR PEER REVIEW 42 of 104

Figure17.
Figure 17. Functional
Functional groups
groupsofofsix
sixpolymer
polymertypes, with
types, examples
with theoretically
examples lumped
theoretically into into
lumped one one
chain for the compactness of the figure [392–407].
chain for the compactness of the figure [392–407].

Category B polymers possess side functional groups connected to the backbone

through heterogeneous atoms (Cl, O; Figure 17, Category B). The initial scissions in the
 polyene. The chain backbone contains many double bonds, leaving the remaining polyene
susceptible to cross-linking reactions and coke formation. The degradation process for this
category involves three distinct stages: the release of heterogeneous atoms, cross-linking,
Polymers 2025, 17, 628 41 of 94
and degradation (Figure 17, Category B). Figure 18 shows the mechanism of PVC degra-
dation and the formation of polyene.

Figure 18.
Figure 18. The
The thermal
thermaldegradation
degradationprocess
processofof
PVC [408].
PVC [408].

Category C
Category C polymers
polymersare, are,ininessence,
essence, devoted
devoted to PAN.
to PAN. TheThedegradation
degradation behavior
behaviorof of
these polymers, which are utilized in the manufacturing of acrylic fibers,
these polymers, which are utilized in the manufacturing of acrylic fibers, strongly differs strongly differs
from that
from that of
of other
other polymers
polymers(Figure
(Figure17,17,Category
Category C).C).
TheThe degradation
degradation of PAN results
of PAN in in
results
the formation of linear or multi-branched polycyclic structures through
the formation of linear or multi-branched polycyclic structures through N2 bonding with N 2 bonding with

adjacent carbon
adjacent carbon atoms,
atoms,ultimately
ultimatelyleading
leading to tothethe
formation
formation of stable cokecoke
of stable [398]. PAN’s
[398]. PAN’s
strong propensity for secondary reactions and coke formation makes it a desirable feed-
strong propensity for secondary reactions and coke formation makes it a desirable feedstock
stock for producing fibrous AC [409].
for producing fibrous AC [409].
Category D polymers are highly unsaturated polymers, such as rubbers (Figure 17,
Category D polymers are highly unsaturated polymers, such as rubbers (Figure 17,
Category D). Regarding their cis structure, most monomers are vulnerable to secondary
Category D). Regarding their cis structure, most monomers are vulnerable to secondary
reactions (e.g., Diels–Alder reactions), resulting in the formation of cyclic compounds
reactions (e.g., Diels–Alder reactions), resulting in the formation of cyclic compounds rang-
ranging from naphthenes to (poly)aromatics. As rubbers are mostly employed in a vul-
ing fromform,
canized naphthenes to (poly)aromatics.
devulcanization through fastAs rubberswith
pyrolysis are mostly employed
a low residence in acan
time vulcanized
lead
form, devulcanization through fast pyrolysis with a
to the substantial recovery of valuable diene monomers [246,396,399,401]. low residence time can lead to the
substantial recovery of valuable diene monomers [246,396,399,401].
Note that chloroprene rubber (CR) can be classified as either Category B or D, but its
Note
thermal that chloroprene
behavior is much closerrubber (CR)
to that can be classified
of Category as either
B. The presence Category
of both doubleBbondsor D, but
its
and thermal
chlorinebehavior
in the CRisstructure
much closer to that
contributes to of Category
a high B. The presence
coke formation rate, withofupbothto 50%double
bonds
produced [407]. This category typically produces a considerable amount of coke during up
and chlorine in the CR structure contributes to a high coke formation rate, with
to 50% produced
thermal degradation, [407].
whichThis
cancategory
be reduced typically produces
by increasing the aheating
considerable amount
rate [395–397]. of coke
Gen-
erally, pyrolysis
during is not recommended
thermal degradation, which can for be
thisreduced
category, byand alternative
increasing the methods
heating rate(e.g.,[395–397].
sol-
volysis, controlled
Generally, pyrolysis catalytic degradation, or using
is not recommended for thisa suitable
category, carrier gas at high pressures)
and alternative methods (e.g.,
must be employed
solvolysis, controlled to prevent
catalyticpolyene formation.
degradation, or using a suitable carrier gas at high pressures)
mustNonlinear
be employed polymers with heterogeneous
to prevent polyene formation. atoms in the polymer backbone and poten-
tiallyNonlinear
with side groups,
polymers with heterogeneous atoms(Figure
such as PET, PU, and cellulose 17, Category
in the polymer E), determine
backbone and poten-
Category E polymers [402,404,405,410]. The associated fibers are highly
tially with side groups, such as PET, PU, and cellulose (Figure 17, Category E), determine durable due to the
naphthenic and aromatic rings in the chain backbone, as well as H2 bonding in some in-
Category E polymers [402,404,405,410]. The associated fibers are highly durable due to
stances. Thus, around 90% of the world’s produced fibers belong to this group [17]. The
the naphthenic and aromatic rings in the chain backbone, as well as H2 bonding in some
production of polycondensation polymers through the step-growth polymerization pro-
instances. Thus, around 90% of the world’s produced fibers belong to this group [17]. The
cess is reversible, indicating that the bond between monomers is relatively weaker than
production of polycondensation polymers through the step-growth polymerization process
other bonds. Correspondingly, unzipping is the predominant mechanism during the deg-
isradation
reversible, indicating that the bond between monomers is relatively weaker than other
of this category in cases where the original by-product is a major component.
bonds.
Note that,Correspondingly, unzippingunzipping
unlike depolymerization, is the predominant
during pyrolysismechanism
does notduring
resultthe degrada-
in very
tion
high monomer recovery. Due to the high temperature and reaction rate, secondary reac-Note
of this category in cases where the original by-product is a major component.
that,
tionsunlike depolymerization,
occur during pyrolysis, which unzipping
results induring
a wide pyrolysis does notproducts
range of pyrolysis result in(Figure
very high
monomer
17, Category E) [411–413]. In this regard, a controlled depolymerization technique, reactions
recovery. Due to the high temperature and reaction rate, secondary such
occur duringresults
as solvolysis, pyrolysis, which results
in monomer recoveryinatalow wide range of temperatures
to moderate pyrolysis products[414]. In(Figure
other 17,
Category E) [411–413]. In this regard, a controlled depolymerization technique, such as
solvolysis, results in monomer recovery at low to moderate temperatures [414]. In other
words, (screw-based) solvolysis can be seen as the most effective chemical recycling method
for synthetic polycondensation polymers [415].
Note that while man-made and cellulosic fibers can also be converted into glucose
via enzymes or solvolysis, the dissolution and mechanical recycling approach is more
practical and desirable [349]. Considering the strong H2 bonding in polycondensation
polymers (excluding polyesters), it is essential to employ solvents capable of disrupting
these interactions during dissolution, as explained above. Specifically, PU functional groups
 method for synthetic polycondensation polymers [415].
Note that while man-made and cellulosic fibers can also be converted into glucose
via enzymes or solvolysis, the dissolution and mechanical recycling approach is more
Polymers 2025, 17, 628 42 of 94
practical and desirable [349]. Considering the strong H2 bonding in polycondensation pol-
ymers (excluding polyesters), it is essential to employ solvents capable of disrupting these
interactions during dissolution, as explained above. Specifically, PU functional groups are
are a combination of ester and amide functional groups. The presence of aromatics in the
a combination of ester and amide functional groups. The presence of aromatics in the
chain backbone causes secondary reactions to compete closely with chain scission and
chain backbone causes secondary reactions to compete closely with chain scission and
unzipping
unzipping during
during PUPUdegradation.
degradation.However,
However, thethe formation
formation of aofconsiderable
a considerable amount
amount of of
coke is prevented by bulky urethane groups
coke is prevented by bulky urethane groups [416]. [416].
Category
Category FF polymers
polymersdiffer
differfrom
fromthe
the previous
previous category
category in that
in that their
their linear
linear structure
structure
(Figure 17, Category F) leads to relatively minimal coke formation. However,
(Figure 17, Category F) leads to relatively minimal coke formation. However, the appro- the appropri-
ate recycling
priate procedures
recycling proceduresforfor
this
thiscategory
categoryare
arenotnotsubstantially
substantially distinct from those
distinct from thosefor
for the
previous category [403,406].
the previous category [403,406].
To
Tofurther
further highlight
highlight the different overall degradation
different overall degradationmechanisms
mechanismsfor forthe
thesix
sixcatego-
categories,
ries, Figure
Figure 19 shows
19 shows variations
variations in their
in their TGA TGA curves.
curves.

Figure19.
Figure 19.Thermogravimetric
Thermogravimetricanalysis
analysisgraphs
graphsofofdifferent
different polymers
polymers according
according to Figure
to Figure 17 [392–
17 [392–406,417].
406,417].
3.5.2. Biolysis
3.5.2.Currently,
Biolysis biological recycling methods for textile materials focus solely on natural
Currently, biological
and man-made recycling
fibers. Synthetic methods
plastics forthus
have textile
notmaterials focus solely
been efficiently on natural
processed through
and man-made
these methods. fibers. Synthetic
Biological plastics
recycling have thus
processes not been efficiently
encompass processed
a range of through
techniques, such as
these methods. Biological recycling processes encompass a range of techniques,
enzymolysis to produce glucose and fermentation to generate bioethanol. Compared such as to
enzymolysis to waste
lignocellulose, produce glucose
textiles and
can befermentation
biodegraded to without
generate issues
bioethanol.
causedCompared to and
by lignin
lignocellulose, waste textiles can be biodegraded without issues caused by lignin and
hemicellulose, but the high crystallinity of cellulose in cotton fibers presents a significant
hemicellulose, but the high crystallinity of cellulose in cotton fibers presents a significant
challenge. An overview of textile recycling methods using enzymolysis is provided in
Table 4. Below, some complementary examples are discussed in greater detail.
Despite concerns over the environmental impact of textile waste containing synthetic
polymers and cellulose fractions, the cellulose component holds promise for generating
biofuels, such as EtOH and biogas. Textile waste typically contains 35–40% cellulose,
making it a potential feedstock for producing biological products [418]. Cotton present in
textile waste can serve as an alternative source of renewable energy and has been studied
as a feedstock for bioethanol, biorefining, and biogas production [419]. To enhance enzyme
Polymers 2025, 17, 628 43 of 94

accessibility, it is recommended to increase the surface area of cellulose feedstocks by

modifying their porosity and reducing their crystallinity through pretreatment.
Notably, textile mill cotton waste has already been subjected to acid and alkali pretreat-
ment to expose sugars for enzymatic hydrolysis by Fusarium species’ cellulase. The enzyme
activity was enhanced, and the glucose release was higher with acid pretreatment com-
pared to alkali pretreatment. Glucose was fermented with Saccharomyces cerevisiae through
simultaneous saccharification and fermentation. In batch fermentation, 11.8 mg·mL−1 of
alcohol was produced [420].
The advantages of enzymolysis are that the cellulose fraction becomes soluble and can
be separated from other fractions in the textile blend without the need for manual sorting.
According to Wang et al. [421], the solubility of cellulose in a cold NaOH/CH4 N2 O solution
can be enhanced by enzymatic pretreatment. They observed an increase from 30% to 65%,
which was primarily linked to the enzymatic treatment reducing the average molar mass
of cellulose.
Vecchiato et al. [422] developed a circular economy solution for recycling viscose fiber
waste. They used glucose to produce bioethanol and a flame-retardant pigment to produce
new fibers. The applied enzymatic hydrolysis method allowed for the recovery of both
glucose and pigment in high yields of 98% and above 99%, respectively. The maximum
amount of released sugars was recovered after 8 h at 50 ◦ C, and this recovered glucose
was successfully used to produce EtOH through S. cerevisiae. The EtOH yield upon using
commercial glucose was almost identical to that upon using recovered glucose.
Studies on the fiber morphology and enzymatic hydrolysis yields revealed that while
alkali pretreatment of cotton fiber waste was necessary, it was not required for viscose
fiber waste. Viscose fiber outperformed cotton fiber in terms of enzymatic hydrolysis
and produced higher fermentation yields (8.1 vs. 6.9 g·L−1 ) due to the variations in their
microcrystalline structures [423]. MMCFs appear to be the favored type of fiber in the
realm of biological recycling due to their ability to be recycled with minimal expense and
environmental impact compared to other fibers.
Biological recycling methods have also been explored for wool, a complex natural
fiber composed mainly of proteins (97%) and lipids (1%). This fiber material is an ideal
substrate for several classes of enzymes, such as proteases and lipases, which increase its
biodegradation rate [423]. For example, Navone and Speight [424] suggested enzymatic
treatment of wool/polyester fabric blends as a means of selectively breaking down wool
fibers while preserving synthetic fibers. This involved the use of a protease with kerati-
nolytic activity, along with reducing agents applied to the fabric blends. The most effective
results could be obtained through a two-step enzymatic process in the presence of sodium
thioglycolate. The polyester fibers could then be recycled into polyester yarn, which could
be utilized in the production of new clothing items or other products [425].
Quartinello et al. [426] even demonstrated the efficacy of stepwise enzymatic hydrol-
ysis of cellulose–wool–polyester blends. In this process, textile waste was sequentially
treated with (1) protease to extract amino acids from wool components with 95% efficiency,
and (2) cellulases to recover glucose from cotton and viscose constituents with 85% effi-
ciency. The resulting amino acids and oligopeptides from wool degradation can serve as
replacements for carbon and N2 sources, while the glucose from cotton hydrolysis can be
fermented with S. cerevisiae to produce EtOH [423].
Polymers 2025, 17, 628 44 of 94

Table 4. Studies on the enzymolysis of different textile blends for the production of glucose.

Solvent:Polymer Glucose
Textile Enzyme Solvent for Pretreatment T (◦ C) t (h) Buffer Solution Ref.
(vol/vol%) Yield (%)
Cellulase and 0.33 mol·L−1 sodium
Cotton-based waste (jeans) H3 PO4 50:1 50 96 86.1 [419]
Tricoderma reesei citrate (pH: 4.8)
Cotton linters Celluclast NaOH/CH4 N2 O solution 100:5 50 0.5–4 Acetate (pH: 4.5) 95.0 [421]
Dyed cotton and NMMO monohydrate,
0.1 M·L−1 phosphate (pH: 5)
cotton–polyester Cellulase AP3 [BMIM]Cl, H3 PO4 , and 10:1–20:1 50 72 58.1 [427]
with 0.02% sodium azide
blend shirts NaOH/CH4 N2 O solution
Polyester–cotton
Cellusoft L Lutensol AT20 NA 1 50 1 0.1 M·L−1 of acetate (pH: 5) 100 [428]
blend shirts
Undyed cotton T-shirt Cellulase [AMIM]Cl 100:5 50 NA 2.5M ·L−1citrate (pH: 5) 86.0 [429]
Celluclast 1.5 L and 0.2 M·L−1 sodium citrate
Cotton–polyester blend NaOH/CH4 N2 O solution NA 50 96 98.7 [430]
β-glucosidase (pH 5.1)
Cotton–PET blend HiC and CTec2 Mechanical treatment NA 55 24 Sodium phosphate (pH: 7.4) 83–87 [431]
NaOH/CH4 N2 O, NaOH
Celluclast 1.5 L and Sodium acetate and 0.5 g ·L−1
Polyester–cotton blend thiourea, and 95:5 45 72 91.0 [294]
β-glucosidase sodium azide (pH: 4.8)
NaOH/CH4 N2 O/thiourea
Cellulose–wool– Cellic CTec3 and
mQ-H2 O NA 50 48 0.67 M·L−1 , Tris-HCl (pH: 9) 50–90 [426]
polyester blend Savinase 12T
Bleached cotton fabric Celluclast 1.5 L Ultrasonic treatment NA 50 1.5 0.2 M·L−1 , acetate (pH: 5) 54.0 [432]
1 Not available.
Polymers 2025, 17, 628 45 of 94

3.5.3. Pyrolysis
Pyrolysis has emerged as a pioneering approach in the transformation of waste tex-
tiles into valuable products, such as fuels and chemicals. In the realm of textile pyrolysis,
catalysts exert a substantial impact on product distribution and selectivity. The inception
of catalytic pyrolysis for synthetic textiles can be traced back to the early 2000s, when
researchers embarked on exploring the potential of various catalysts to augment the pyrol-
ysis process [433]. Over time, a myriad of catalysts, including zeolites [434], mesoporous
materials [435], and metal oxides [436], have been tested to enhance the pyrolysis process.
Pyrolysis is a suitable technique commonly used for polyolefin recycling, with direct and
indirect processes used to produce light olefins [437–440]. The direct catalytic process for
producing light olefins is being developed for industrial use but has challenges, and the
dedicated transformation of this knowledge into that on the textile level is an ongoing re-
search effort. In what follows, the main possibilities of pyrolysis are highlighted to provide
general insights based on current data and case studies, and for which textile materials
pyrolysis is a worthwhile option is explained. Table 5 provides an overview of the research
conducted in the field of pyrolysis and gasification.
An important case study is that of Eschenbacher et al. [361], who achieved 85% re-
covery of light olefins using modified zeolite catalysts in a micropyrolysis reactor. The
indirect process leading to pyrolysis oil is preferred by large refineries and petrochemi-
cals but requires pretreatment due to high levels of olefins and cyclic compounds [439].
Kusenberg et al. [388] and Abbas-Abadi et al. [380,441] studied polyolefin pyrolysis and
evaluated the challenges of producing light olefins from pyrolysis oil as well as the effect
of the presence of mineral and organic contaminations in the oil on product yields and
coke formation.
Green and Sadrameli [442] investigated the impact of temperature (400–1000 ◦ C) on
the products of high-density polyethylene (HDPE) pyrolysis using a continuous fluidized
bed (FB) reactor (Figure 20). Complete conversion of PE was achieved at temperatures
above 650 ◦ C due to short residence times. At temperatures below 500 ◦ C, C1–4 compounds
were insignificant, and C12+ compounds were predominantly produced. The production
of H2 and light hydrocarbons started to increase at 500 ◦ C and reached the maximum at
700 ◦ C. Ethylene presented a maximum peak at 900 ◦ C, and methane (CH4 ) increased in
the studied temperature range. Interestingly, the propylene and butadiene yields decreased
significantly with a slight increase in temperature above 700 ◦ C. The production of aromatics
indicated an increasing trend beyond 650 ◦ C, whereas polyaromatics appeared at 800 ◦ C.
Polymers
Polymers 2025, 17,
17, 628
x FOR PEER REVIEW 4649 of 104
of 94

Figure 20.The
Figure20. Theyields of of
yields PEPE
pyrolysis products
pyrolysis vs. temperature
products (adapted
vs. temperature from [442]).
(adapted PNA stands
from [442]). PNA for
stands
polynuclear aromatics [442].
for polynuclear aromatics [442].

The residence time is one of the key parameters that must be considered in the reactor
The residence time is one of the key parameters that must be considered in the reactor
design. It should be long enough to obtain a sufficient conversion of the feedstock into
design. It should be long enough to obtain a sufficient conversion of the feedstock into
lighter products but short enough so that light olefins are efficiently removed from the
lighter products but short enough so that light olefins are efficiently removed from the
reactor, thereby preventing secondary reactions, similarly to extrusion-based modifica-
reactor,
tions thereby
[443]. preventing
The produced lightsecondary
olefins can reactions, similarly toinextrusion-based
act as intermediates modifica-
bimolecular reactions
tions
and are[443].
then The produced
converted light olefins
into aromatic can act as
compounds andintermediates in bimolecular reactions
coke [439,440,444].
and Theare then converted
pyrolysis productsinto
of aromatic compounds
mixed polyolefins and which
(MPOs), coke [439,440,444].
make up a third important
case study, are significantly impacted by important parameters,which
The pyrolysis products of mixed polyolefins (MPOs), such asmake up a third
the PP/PE ratio,im-
portant
the amountscase study,
of other are
polymers (e.g.,impacted
significantly PS, PET, by PVC,important parameters,
and rubbers), and thesuch as the PP/PE
presence of
ratio, the amounts of other polymers (e.g., PS, PET, PVC, and
mineral and organic contaminants. PVC contamination is particularly noteworthy due rubbers), and the presence
ofits
to mineral
potentialandfor
organic contaminants.
HCl release and residualPVCstructure,
contamination
which is particularly
can noteworthy
significantly contributedue
to coke
to its potential
formation for[445].
HCl release and residual
The polyene left afterstructure,
the release which canissignificantly
of HCl contribute
a viable option for
to coke formation
absorbing [445].
light olefins andThe polyene
styrene leftenhancing
and for after the secondary
release of reactions,
HCl is a viable
such asoption
Diels– for
absorbing
Alder light(Figure
reactions olefins 21).
and During
styrenetheanddegradation
for enhancing secondary
of biomass reactions, such
contamination andas Diels–
after
deoxygenation, it exhibits characteristics similar to those of PVC and
Alder reactions (Figure 21). During the degradation of biomass contamination and after can significantly
contribute
deoxygenation,to cokeitformation [379].
exhibits characteristics similar to those of PVC and can significantly con-
In any case, the design
tribute to coke formation [379]. of a suitable pyrolysis reactor is an important factor in the
production of light olefins from MPO waste. The optimal reactor design should have proper
feeding, minimum residence time, and proper heat and mass transfer with minimum energy
consumption [446]. Different reactor designs, such as vortex [387,447,448], conical spouted
bed reactor [449], downer [450], and FB reactors [451], are being investigated. The use of
modified zeolite catalysts (promotion, steaming, and mesoporosity) can increase product
selectivity and light olefin production with lower energy consumption. Designing robust
catalysts remains a challenge for the large-scale implementation of catalytic pyrolysis [391].
Polymers 2025,
Polymers 17,17,
2025, 628x FOR PEER REVIEW 50 of 104 47 of 94

Figure 21.
Figure 21. Diagram
Diagramillustrating PVC
illustrating PVCdegradation
degradationand and
the subsequent reactions
the subsequent with light
reactions witholefins
light olefins
during the
during thepyrolysis
pyrolysisofofwaste
wastepolyolefins [441].
polyolefins [441].

In any 22
Figure case, the design
illustrates of a suitable
the typical pyrolysis
degradation reactorofisPET
reactions an important factor in
during pyrolysis the
[411,452,453].
production of light olefins from MPO waste. The optimal reactor design
At high temperatures, the C–O bonds are susceptible to breaking due to their weak bondingshould have
proper feeding,
energy. minimum
The acidic groupsresidence time,
attached toand proper(C
benzene heat and mass transfer with mini-
6 H6 ) are affected in the subsequent
mum energy
stages. consumption
The primary [446]. Different
pyrolysis productsreactor
of PET designs,
are C6such as vortex
H6 , CO [387,447,448],
2 , and carbon monoxide
conical spouted bed reactor [449], downer [450], and FB reactors [451], are being investi-
(CO), as shown in Figure 22. Although some TPA may be produced during pyrolysis, a
gated. The use of modified zeolite catalysts (promotion, steaming, and mesoporosity) can
portion of it will quickly undergo secondary reactions. The formation of coke during PET
increase product selectivity and light olefin production with lower energy consumption.
pyrolysis can be attributed to the presence of phenyl radical groups and styrene (e.g., from
Designing robust catalysts remains a challenge for the large-scale implementation of cat-
contaminants). This leads to subsequent secondary reactions, such as carbonization, Diels–
alytic pyrolysis [391].
Alder reactions, and ultimately,
Figure 22 illustrates cokedegradation
the typical formation (polyaromatics).
reactions of PET Process parameters are
during pyrolysis
essential
Polymers 2025, 17, x FOR PEER REVIEW to minimize
[411,452,453]. coke formation
At high temperatures, during
the C–O PET
bonds areand cellulosetopyrolysis
susceptible 51 of 104
breaking due through
to fast
pyrolysis
their weakand usingenergy.
bonding reactorsThewith a minimum
acidic (average)
groups attached residence
to benzene (C6H time [411,452,453].
6) are affected in
the subsequent stages. The primary pyrolysis products of PET are C6H6, CO2, and carbon
monoxide (CO), as shown in Figure 22. Although some TPA may be produced during
pyrolysis, a portion of it will quickly undergo secondary reactions. The formation of coke
during PET pyrolysis can be attributed to the presence of phenyl radical groups and sty-
rene (e.g., from contaminants). This leads to subsequent secondary reactions, such as car-
bonization, Diels–Alder reactions, and ultimately, coke formation (polyaromatics). Pro-
cess parameters are essential to minimize coke formation during PET and cellulose pyrol-
ysis through fast pyrolysis and using reactors with a minimum (average) residence time
[411,452,453].

Figure 22. The proposed mechanism of PET degradation at elevated temperatures [411,452,453].
Figure 22. The proposed mechanism of PET degradation at elevated temperatures [411,452,453].
It should be stressed that pyrolysis is not a suitable method for PET recycling, due to
the high production of gases (CO2 and CO) therein, and also for other polycondensation
polymers. Pyrolysis is a viable option in situations where techniques such as mechanical
recycling and solvolysis prove to be unresponsive. Studies have indicated that incorpo-
rating catalysts such as iron oxyhydroxide, rutile (titanium dioxide [TiO2])/SiO2, Zeolite
Socony Mobil–5 (ZSM-5), and sulfated zirconia into PET pyrolysis can effectively suppress
Polymers 2025, 17, 628 48 of 94

It should be stressed that pyrolysis is not a suitable method for PET recycling, due to
the high production of gases (CO2 and CO) therein, and also for other polycondensation
polymers. Pyrolysis is a viable option in situations where techniques such as mechanical
recycling and solvolysis prove to be unresponsive. Studies have indicated that incorpo-
rating catalysts such as iron oxyhydroxide, rutile (titanium dioxide [TiO2 ])/SiO2 , Zeolite
Socony Mobil–5 (ZSM-5), and sulfated zirconia into PET pyrolysis can effectively suppress
TPA formation [454]. Below, some key examples of pyrolysis-based research with textile
materials are given.
Molto et al. [452] applied a laboratory-scale batch horizontal tube reactor to pyrolyze
PET fibers within a temperature range of 650 ◦ C to 1050 ◦ C. The primary products were
mostly C6 H6 (2.42–30.09 wt%), CO2 (14.85–27.70 wt%), and CO (8.73–16.49 wt%), while
ethylene (0.39–3.88 wt%) and CH4 -ethane mix (1.71–5.70 wt%) were secondary products.
The pyrolysis process generated a diverse assortment of compounds, such as aromatics,
linear olefins and paraffins, acids, and phenols [452]. Moreover, the formation of organic
acids (e.g., TPA and benzoic acid [C6 H5 COOH]) as a process issue can cause corrosion and
line blockages [453]. During pyrolysis, PET goes through primary and secondary reactions,
leading to different products and by-products at high temperatures.
Kumagai et al. [454] conducted a study on the reactivity of PET pyrolysis products
with different types of metal oxides. They utilized a Tandem µ Reactor-GC/MS and carried
out PET pyrolysis at 450 ◦ C. The results showed that zinc oxide (ZnO), which has a high
base strength, effectively promoted the decarboxylation of the principal pyrolysis products
of C6 H5 COOH and TPA at a low temperature of 700 ◦ C, resulting in the production
of C6 H6 -rich aromatic hydrocarbons (88.8 area%). On the other hand, MgO, TiO2 , and
zirconium dioxide were found to have lower base strengths than ZnO; hence, a temperature
increase of around 50−70 ◦ C is required for decarboxylation. These findings provide
valuable insights into feedstock recycling and converting PET waste materials or mixed
plastics that contain PET into raw chemical materials through catalytic pyrolysis.
Diaz-Silvarrey et al. [455] pyrolyzed PET using a sulfated zirconia (SZ) catalyst at
different temperatures and catalyst/PET ratios. The findings indicate that both temperature
and the catalyst/PET ratio significantly affect the production of C6 H5 COOH, a widely
used precursor in the food and beverage industry. A high temperature (600 ◦ C) and the
absence of a catalyst resulted in a 16% increase in the recovery of C6 H5 COOH in the wax
product compared to other conditions. However, this process is energy-intensive due to the
endothermic nature of PET pyrolysis. The addition of the catalyst increased the amount of
light hydrocarbons (C1 –C4 ) produced, from 4 wt% without catalyst to 20 wt% at a 10 wt%
catalyst/PET ratio. Nevertheless, the catalyst deactivated due to coke deposition on the
catalyst surface and partially decomposed at high pyrolysis temperatures (>525 ◦ C). It was
thus suggested that PET catalytic pyrolysis using the SZ catalyst should be performed at
temperatures below 525 ◦ C, with catalyst loads below 10 wt% of PET, to obtain high yields
of C6 H5 COOH and a high value of gas products (i.e., a high proportion of hydrocarbons).
Jia et al. [434] performed catalytic pyrolysis of PET using ZSM-5 zeolite and nickel
chloride (NiCl2 ) as catalysts at various temperatures under a N2 atmosphere. The results
revealed a significant reduction in carboxyl and aliphatic hydroxyl groups in the waxy
residue upon zeolite utilization during pyrolysis. A 22% increase in aromatic hydroxyl
groups and a 42% decrease in carbonyl groups were observed under the catalyst/PET ratio
of 2/1, demonstrating enhanced deoxygenation effects with zeolite addition. Meanwhile,
the addition of ZSM-5 and NiCl2 reduced the waxy product yield while increasing the gas
yield. The use of ZSM-5 had a limited impact on the primary decomposition of PET but
promoted secondary volatile reactions, whereas NiCl2 enhanced primary decomposition
toward liquid products.
Polymers 2025, 17, 628 49 of 94

Sulfated zirconia has also been recognized as a promising catalyst for obtaining
C6 H5 COOH from PET. Diaz-Silvarrey et al. [455] reported the highest C6 H5 COOH yield
of 28 wt% at 600 ◦ C, using a catalyst/feed ratio of 1/10. Additionally, a Co-based catalyst
(Co/SiO2 ) could be employed to transform hazardous volatile compounds, such as C6 H6
derivatives and polycyclic aromatic hydrocarbons (PAHs), into syngas. Compared to
non-catalytic pyrolysis, CO2 -assisted catalytic pyrolysis of waste PET yielded over three
and eight times higher H2 and CO production, respectively. Furthermore, CO2 -assisted
catalytic pyrolysis suppressed carbon deposition on the Co-based catalyst [456].
Besides PET, other common types of plastics found in textiles, such as PE and PP,
have been identified as ideal sources for the production of light olefins, as previously
discussed [361,457]. However, it should be noted that the catalyst/feed ratio for converting
plastics into light olefins was relatively high. Optimizing the conversion of textile waste
into valuable bio-oil and gases, along with minimizing catalyst consumption and pyrolysis
time, is thus crucial.
Yousef et al. [458] examined the pyrolysis process of waste jeans, a substantial fraction
of textile waste, employing heavy metals present in textile dyes as self-catalysts to improve
conversion efficacy. A two-stage method—initially performing lab-scale experiments
utilizing TGA-FTIR and subsequently conducting pilot-scale assessments in a specially
designed pyrolysis reactor—was performed. The results revealed a successful conversion of
over 82% of the feedstock into liquid-gas products, with the untreated feedstock generating
a 20% higher bio-oil yield compared to the samples without heavy metals.
Furthermore, Phan et al. [459] focused on the pyrolysis of a textile sample made up of
mostly cotton, with a small amount of polyester (<5%). The study included experiments
at five temperatures, ranging from 350 ◦ C to 700 ◦ C, using a 150–200 g sample for each
test. To begin each test, the sample was placed in a fixed bed reactor at room temperature
and heated at a rate of 10 ◦ C·min−1 until the target temperature was reached, after which
it was maintained at that temperature for 2 h. The results showed that the percentage of
char decreased from 32% to 19% with rising temperature, while the liquid fraction reached
its highest yield of 47% at 600 ◦ C, and the gas yield increased with rising temperature.
Phenolic, furan, and anhydrosugar compounds were the predominant products in all
reactions, whereas the major gas products were CO2 , CO, CH4 , and H2 .
Zhang et al. [435] performed ex situ catalytic pyrolysis of waste mixed clothing using
hierarchical ZSM-5 and commercial CaO as catalysts. Pyrolysis in the temperature range of
450~750 ◦ C primarily resulted in levoglucosan formation. The use of HZSM, possessing
Brønsted/Lewis acid sites on microporous and mesoporous structures, contributed consid-
erably to the production of monocyclic and dicyclic chemicals. Moreover, CaO exhibited
strong deoxygenation capabilities, facilitating the transformation of the waste into low
oxygen-containing chemicals, such as ketones, aliphatic hydrocarbons, and aromatics. This
study underscored the potential of catalytic upgrading of waste mixed cloth into valuable
chemicals through catalytic pyrolysis over modified ZSM and CaO catalysts.
The valorization of waste teabags through catalytic pyrolysis, examining the effects
of CO2 and HZSM-11 on pyrolytic products, was investigated by Kim et al. [460]. In non-
catalytic pyrolysis, the carrier gas of CO2 increased the pyrolytic gas yields while reducing
the formation of C6 H6 , phenolics, and PAHs compared to N2 . The HZSM-11 catalyst further
enhanced CO2 conversion to CO, particularly in a CO2 environment. The synergistic use of
CO2 and HZSM-11 in waste teabag catalysis increased caprolactam production. However,
to ensure economic feasibility, a proper waste collection and treatment method, such as
separating waste teabags from food waste streams and drying at the source, is essential
prior to processing.
Polymers 2025, 17, 628 50 of 94

Table 5. Key contributions to pyrolysis and gasification for textile materials and waste.

Pyrolysis T Catalysis T Cat/

Feed Carrier Gas Reactor Catalyst Product Yield Major Findings Ref.
(◦ C) (◦ C) Feed
Syngas:
700 The production of syngas from CO2 -assisted catalytic pyrolysis was seven times
CO2 600 Fixed bed Ni/SiO2 1 CO: 17.5 mol%
(10 ◦ C·min−1 ) larger than the inert atmosphere of N2 arising from increased CO formation
H2 : 11.9 mol% through the catalytic reaction of CO2 with pyrolytic products over the catalyst.
Polyamide
Syngas: CO2 also offered a great opportunity to suppress catalyst deactivation by
700 suppressing coke deposition or removing the coke deposited on
N2 600 Fixed bed Ni/SiO2 1 CO: 5.7 mol% the catalyst surface.
(10 ◦ C·min−1 )
H2 : 18.7 mol%
600 600 Benzoic acid: Increasing the catalyst/plastic ratio could increase the amount of other valuable
PET N2 Tubular Sulfated zirconia 0.1 [455]
(45 ◦ C·min−1 ) (45 ◦ C·min−1 ) 28.0 wt% products (e.g., light hydrocarbons [C1 –C3 ]) recovered in the gas.
Solid residual: 10.5
wt% ZSM-5 has little effect on the primary decomposition of PET, but it promotes the
N2 600 600 Tubular ZSM-5 6 secondary volatile reactions. The use of NiCl2 as a catalyst will greatly improve
PET [434]
Wax: 23 wt% the primary decomposition of PET to generate more liquid products.
N2 600 600 Tubular ZnCl2 1 Wax: 68.9 wt%
Spouted Light olefins (C2 ~C4 ): The low residence time in the catalytic reactor enhances the selectivity of light
HDPE N2 500 500 HZSM-5 8 [457]
bed + fixed bed 59 wt% olefins and attenuates the secondary reactions of coke formation.
Phosphorus-
modified and Light olefins (C2 ~C4 ):
LDPE 1 He 550 600 Micropyrolyzer 80
steam-treated 82.8 wt%
HZSM-5
Phosphorus-modified and steam-treated HZSM-5 showed almost no deactivation
23 wt% LLDPE 2 , Phosphorus- due to the lower coking propensity during 130 runs, with stable conversion to C5+
7.5 wt% LDPE, modified and Light olefins (C2 ~C4 ): aliphatics and high C2 –C4 olefin selectivity (~75%) using post-consumer [361]
He 550 600 Micropyrolyzer 80
29.5 wt% HDPE, steam-treated 78.8 wt% mixed polyolefins.
40 wt% PP HZSM-5
Phosphorus steamed Light olefins (C2 ~C4 ):
Mixed polyolefins He 550 600 Micropyrolyzer 80
HZSM-5 73.2 wt%
Oil: 37.5 wt%
800 800 Heavy metals in textile dyes were used as self-catalysts to accelerate the
Waste textiles N2 Fixed bed Al2 O3 - Gas: 44.7 wt% conversion process and decrease the pyrolysis time by 15% and to increase the [458]
(10 ◦ C·min−1 ) (10 ◦ C·min−1 )
bio-oil yield by ~20% compared to the textile samples treated without catalysts.
Char: 17.8 wt%

720 Gas: 80.9%

CO2 650 Tubular Co/SiO2 1 Catalytic pyrolysis over a Co-based catalyst with threefold- and eightfold-higher
(10 ◦ C·min−1 ) Char: 17.6%
Waste textiles (main production of H2 and CO, respectively, compared to non-catalytic pyrolysis. This [456]
component: PET) Gas: 73.9% process also suppressed catalyst deactivation, converting more than 80 wt% of
720 waste textile into syngas and CH4 .
N2 650 Tubular Co/SiO2 1
(10 ◦ C·min−1 ) Char: 19.1%
Polymers 2025, 17, 628 51 of 94

Table 5. Cont.

Pyrolysis T Catalysis T Cat/

Feed Carrier Gas Reactor Catalyst Product Yield Major Findings Ref.
(◦ C) (◦ C) Feed
He 650 650 Pyroprobe HZSM-5 6 Aromatics: 98.9% The utilization of HZSM with Brønsted/Lewis acid sites on microporous and
Waste mixed cloth
mesoporous structures significantly contributed to the production of
(cotton fibers, acrylic Anhydrosugars: [435]
He 650 - Pyroprobe - - monocyclic/dicyclic chemicals, mainly referring to monoaromatics and
fibers, and PET fibers) 45.7% naphthalene-based derivatives.
N2 550 550 Fixed bed Hbeta - BTEX: 49.4% The pore sizes of Hbeta and HY were larger than the kinetic diameters of the
N2 550 550 Fixed bed HY - BTEX: 35.2% branched hydrocarbons, allowing the thermally derived branched hydrocarbons
COVID-19 mask [461]
to diffuse inside the pores and thereby converting into the aromatic hydrocarbons
N2 550 550 Fixed bed HZSM-5 - BTEX: 21.1% over acid sites located mainly inside the pores.

COVID-19 mask 600 H2 : 55.1 mol% Pyrolysis over a Ni/SiO2 catalyst led to the substantial conversion of longer-chain
N2 600 Tubular Ni/SiO2 1 [462]
(PP, PE, polyamide) (10 ◦ C·min−1 ) CH4 : 18.2 mol% (≥C2 ) HCs into H2 and CH4 .
1 LDPE, low-density polyethylene; 2 LLDPE, linear low-density polyethylene.
Polymers 2025, 17, 628 52 of 94

More recently, Lee et al. [461] investigated the conversion of waste medical masks
(mainly PP and some polyamide), by-products of the COVID-19 pandemic, into value-
added chemicals, such as BTEX (C6 H6 , toluene, ethylbenzene, and xylene), via catalytic
fast pyrolysis using zeolite catalysts. The effect of zeolite properties on pyrolytic product
yields and composition was assessed using different catalysts (HBeta, HY, and HZSM-5).
The large-pore zeolite catalysts HBeta and HY exhibited 134% and 67% higher BTEX
concentrations than HZSM-5, respectively. The mesoporous structures of the catalysts
allowed the branched hydrocarbons formed during mask pyrolysis to diffuse within the
catalyst pores to convert into aromatic compounds. To recover more valuable gaseous
products, multistage catalytic pyrolysis over Ni/SiO2 was employed to enhance H2 and
CH4 formation by breaking the C–C and C–H bonds in long-chain hydrocarbons [462].
CO2 carrier gas acted as both a reaction medium and a soft oxidant, controlling the H2 /CO
ratio in the product gas. These pioneering investigations demonstrated the potential for
converting waste masks into valuable chemicals through catalytic pyrolysis.

3.5.4. Gasification
High plastic purity is necessary for both mechanical recycling and solvolysis, requiring
careful sorting of the textiles to be recycled. However, if textile sorting is difficult and
uneconomical, and none of the chemical processes are effective, gasification could provide
a viable alternative.
Gasification is a process whereby a carbon-rich feedstock reacts with a gasifying agent,
such as CO2 , steam, or air, to produce syngas at relatively high temperatures (exceeding
700 ◦ C) [463,464]. During gasification, the fuel is broken down into CO2 and H2 within the
temperature range of 550–1000 ◦ C by introducing the gasifying agent in sub-stoichiometric
quantities [465]. The process involves four stages: pyrolysis, oxidation, reduction, and
tar reforming. Partial oxidation occurs in the process, and the amount of oxygen used
is less than what is required for stoichiometric combustion. In the reduction stage, char
reacts with steam or CO2 to produce CO and H2 , while in the oxidation stage, char and
volatile compounds react with oxygen to create CO2 . The heat generated in the exothermic
oxidation reactions provides energy for the endothermic reducing reactions. In the tar
reforming step, tar reacts with steam to produce lighter hydrocarbons [466]. Important
contributions are included in Table 5 due to their complementarity with pyrolysis.
Supercritical water gasification technology has become a subject of widespread interest
for the clean utilization of fossil energy in recent years. By functioning as a solvent in its
supercritical state, nonpolar water can promote homogeneous reactions. Moreover, water
can act as a catalyst, boosting reaction rates due to the high ion production near critical
points and the formation of H2 atom radicals at high temperatures.
Supercritical water is also particularly tolerant of wet materials that have not under-
gone drying pretreatment, which can decrease polycondensation and coking. Utilizing
supercritical water to recycle textile waste is thus a promising prospect [467,468].
In what follows, some key examples of waste textile gasification are presented.
Wu et al. [469] investigated the catalytic pyrolysis and gasification of textile waste using
metal catalysts. The researchers examined the impact of metal catalysts on the gasification
rates of textile waste in the presence of CO2 using an atmospheric TGA system. The tem-
perature range of 300–500 ◦ C for the pyrolysis process of textiles was investigated, while
800–1000 ◦ C was maintained for char gasification. The results indicated that ZnO exhibited
the strongest catalytic effect on mixed textiles during the pyrolysis process, while Fe2 O3
had the highest catalytic effect during the char gasification process. Among the various
catalyst loadings tested, 5 wt% ZnO loaded char showed the most significant enhancement
of char pyrolysis reactivity.
Polymers 2025, 17, 628 53 of 94

Jeong et al. [470] performed gasification experiments on 10 types of plastic waste using
a two-stage gasifier with AC. The gases produced had low tar levels and could be used as
fuels in gas engines. Aliphatic plastics (polyolefins) produced lower tar content compared
to plastics with aromatic rings (PET and PU). Furthermore, the chemical structure of the
plastic material significantly affected the yield during gasification, with aromatic plastic
materials producing higher char yields. The heteroatoms in the plastic structure reduced
the char yield. Accordingly, PP had the highest H2 content (about 26 vol%).
Bai et al. [471] explored the impact of various operating conditions on the gasification
of PET microplastics and discussed the gasification pathway. They found that increasing
the reaction temperature and time promoted PET microplastic cracking, but the reaction
pressure did not significantly affect gasification. Seawater utilization was an effective route
for plastic gasification, and metal ions in seawater enhanced the process in different ways.
The gasification kinetics results showed that biphenyl formation was facilitated for PET
plastic and that its cracking was temperature-dependent, hindering gasification. The study
achieved 98% carbon conversion at 800 ◦ C and 23 MPa for 10 min.
Lee and Jung [436] investigated the gasification of polyamide through CO2 -assisted
catalytic pyrolysis using nickel (Ni)/SiO2 as a catalyst to enhance syngas (H2 and CO)
production. The research also identified caprolactam, the PA6 monomer, as a recover-
able product during pyrolysis, which has also been confirmed by other researchers [460].
Nonetheless, the separation of caprolactam from pyrolytic oil was complicated due to
its complex composition. The Ni-based catalyst facilitated the conversion of CO2 into
CO, promoting H2 production and pyrolytic oil degradation. The syngas yield from CO2 -
assisted catalytic pyrolysis was seven times higher than that in non-catalytic processes,
which was attributed to the increased CO formation via catalytic reactions. Additionally,
CO2 aided in mitigating catalyst deactivation by suppressing coke. This research suggests
that CO2 -assisted gasification presents an environmentally friendly approach to converting
GHG and plastic waste into value-added syngas while reducing harmful emissions.

3.5.5. Activated Carbon Production

The chemical structures of natural, semi-traditional, PET, and acrylic fibers make them
prone to intensifying secondary reactions (e.g., Diels–Alder reactions and carbonization).
In contrast to the pyrolysis approach, which necessitates fast pyrolysis and short residence
time to limit secondary reactions, AC production involves a slow pyrolysis process with an
extended residence time to enhance secondary mechanisms [472,473].
AC involves two methods: physical and chemical. Physical activation includes py-
rolysis and carbonization in a neutral medium, followed by physical activation in an
oxidizing atmosphere, such as steam and CO2 , at temperatures ranging from 800 ◦ C to
1100◦ C [474,475].
In chemical activation, the fiber or carbonized fiber is impregnated with a chemical
agent and activated at a lower temperature range (400–900 ◦ C) compared to the physical
method. Activating agents mainly react with weak structures in AC, such as defective
polyaromatics and functional groups, leading to increased pore formation. Activating
agents also create new functional groups on the surface of AC while neutralizing previous
ones [476]. Different acid, base, and salt activators, such as H3 PO4 [477], H2 SO4 [478],
zinc chloride (ZnCl2 ) [479], potassium carbonate (K2 CO3 ) [480], lanthanum ferrite [481],
NaOH [482], and potassium hydroxide [483], react with degradable parts of feedstock
before or after carbonization. Activators increase the activation rate and determine the
efficiency and application of AC to some extent by creating specific functional groups on
the surface. AC can also be produced in a single stage under an oxidizer atmosphere [484].
Polymers 2025, 17, 628 54 of 94

Fibrous AC has unique properties, such as distinctive pore structures, fast adsorption
rates, a large surface area, specific surface functional groups, and ease of regeneration.
Table 6 presents the review of ACs produced from different textile wastes, with key contri-
butions highlighted in what follows. For example, Xu et al. [485] synthesized AC with high
mesoporosity from waste PET by utilizing magnesium chloride (MgCl2 ) as an activator
and precursor based on a MgO template. The most significant surface area (1307 m2 ·g−1 )
and total pore volume (3.56 cm3 ·g−1 ) were achieved with a mixing ratio of 5:5, a pyrolysis
temperature of 900 ◦ C, and a duration of 1.5 h. The results indicated that MgCl2 hindered
the formation of tars through decarboxylic and dehydrogenation reactions, which led to the
favorable formation of an open pore structure. Moreover, MgCl2 catalyzed the secondary
reactions due to its Lewis acidity, which facilitated the formation of carbonaceous materials
during pyrolysis.
Furthermore, Silva et al. [486] employed a slow pyrolysis technique with H3 PO4 to
produce fibrous AC from denim fabric waste, which was applied as an efficient adsorbent.
H3 PO4 was utilized as a protective agent to maintain the fibrous morphology of the
precursor and introduce phosphorus-based functional groups onto the AC surface. The
AC exhibited a considerable surface area of 1582 m2 ·g−1 and mesoporous features. The
findings suggest that the adsorption process may involve chemisorption and can occur
through multilayer adsorption.
Rabbi and Dadashian [487] conducted research on how the degree of stabilization,
activation temperature, and activation stretching influence both the adsorption and me-
chanical properties of acrylic-based AC fibers. The ideal conditions for producing fibrous
AC with high iodine adsorption and tensile strength were determined to be a stabilization
degree of 56%, an activation temperature of 800 ◦ C, and 1% stretching. Under these condi-
tions, the experimental iodine adsorption and tensile strength values of the AC fibers were
approximately 865 mg·g−1 and 423 MPa, respectively. Brunauer–Emmett–Teller analysis of
the optimized sample revealed a surface area of 561 m2 ·g−1 with an average pore diameter
of 2.74 nm. Polyacrylics that incorporate vinyl chloride as a comonomer exhibit greater
stability than other types of polyacrylics. In addition, acrylic fibers have the potential to
produce carbon fibers at a low cost.

Table 6. Overview of the contributions of AC fibers produced from different textile wastes.

Activation Process Properties

Feed Reactor Heating Rate 1
BET Surface Micropore Micropore Volume Total Pore Volume Ref.
T (◦ C)
(◦ C·min−1 ) Area (m2 ·g−1 ) Area (m2 ·g−1 ) (cm3 ·g−1 ) (cm3 ·g−1 )
Waste cotton Tubular 750–900 5 1044–2562 - 0.41–1.14 0.41–1.35 [488]
Waste cotton Tubular 700 5 292 255 0.11 0.14 [489]
Aramid woven
Furnace 800–1200 300 109–248 - - - [490]
fabric waste
Hemp and flax Fixed bed 350–900 2 200–900 - 0.2–0.35 0.10–0.72 [491]
Acrylic waste Fixed bed 700, 800, 900 5 752 - 0.32 - [492]
Waste wool Tubular 1100 2 152 - - 0.15 [493]
PET waste Muffle furnace 900 10 230–1336 193–589 0.08–0.29 - [494]
PET waste Muffle furnace 900 10 171–951 98–480 0.04–0.20 0.15–1.68 [495]
PET waste Muffle furnace 900 10 171–1364 98–527 0.04–0.23 0.15–2.91 [496]
PET waste Pipe furnace 900 10 483–1307 24–323 0.01–0.12 1.53–3.56 [485]
PET waste Pipe furnace 650 10 382–1415 837–1071 0.32–0.43 1.45–2.10 [497]
Cotton wastes Pipe furnace 400–500 10 510–1855 274–440 0.13–0.20 - [498]
1 BET, Brunauer–Emmett–Teller analysis.
 Polymers
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628x FOR PEER REVIEW 60 of 104
55 of 94

3.5.6. Solvolysis
3.5.6. Solvolysis
Solvolysis is a process primarily employed for the depolymerization of polycondensa-
Solvolysis is a process primarily employed for the depolymerization of polyconden-
tion polymers [415,499,500]. For example, the solvolysis reactions of PET involve the use
sation polymers [415,499,500]. For example, the solvolysis reactions of PET involve the use
of various chemicals, such as CH3 OH (methanolysis) [501], EG (glycolysis) [502], water
of various chemicals, such as CH3OH (methanolysis) [501], EG (glycolysis) [502], water
(hydrolysis) [503], ammonia (NH3 ; ammonolysis) [504], and amines (aminolysis) [505],
(hydrolysis) [503], ammonia (NH3; ammonolysis) [504], and amines (aminolysis) [505], to
tofacilitate
facilitate the degradation of compounds. Note that, in complementary reductive de-
the degradation of compounds. Note that, in complementary reductive depoly-
polymerization, the solvent
merization, the solvent and material
and material used
used can can be different
be different and are generally
and are generally different
different from
from those used in other common methods. As the reaction still necessitates
those used in other common methods. As the reaction still necessitates solvent-based me- solvent-based
media, it has
dia, it has been
been classified
classified within
within solvolysis.
solvolysis.
Generally, the solvolysis process
Generally, the solvolysis process with withhigh
high monomer
monomer recovery
recovery is facilitated
is facilitated by low
by low
temperatures
temperatures and high pressures.
and high pressures.For
Forexample,
example, solvolysis
solvolysis is aispromising
a promising method
method for PET
for PET
fiber
fiberrecycling,
recycling, resulting
resulting ininhigh-quality
high-qualitymonomers
monomers without
without anyany toxic
toxic by-products
by-products [506].[506].
Figure23
Figure 23shows
shows the common
commontypestypesofofPET
PETsolvolysis.
solvolysis.

Figure23.
Figure 23. Examples
Examples of
of PET
PETdepolymerization
depolymerizationvia solvolysis.
via solvolysis.

In contrast,
In contrast, the
thecommonly
commonly reported methods
reported methodsfor solvolysis of polyamide,
for solvolysis such as such
of polyamide, hy- as
drolysis and
hydrolysis andaminolysis, require
aminolysis, requireharsh conditions,
harsh including
conditions, highhigh
including temperatures of 250
temperatures 250 ◦ C
of °C
toto300
300◦°C. Other methods,
C. Other methods, such
suchas asglycolysis
glycolysisoror
aminoglycolysis,
aminoglycolysis, have been
have lessless
been effective
effective
in regenerating polyamides. The presence of robust H 2 bonds in polyamide hampers de-
in regenerating polyamides. The presence of robust H2 bonds in polyamide hampers
polymerization, resulting
depolymerization, in in
resulting inferior performance
inferior performance compared
compared to polyesters. Hence,
to polyesters. therethere
Hence, is is
a need to develop new, efficient, and sustainable depolymerization methods for polyam-
a need to develop new, efficient, and sustainable depolymerization methods for polyamides
ides to improve their recycling [507].
to improve their recycling [507].
A high-level overview of the solvolysis methods for polyamide and PET is provided
A high-level overview of the solvolysis methods for polyamide and PET is pro-
in Table 7, followed by a more detailed discussion, including key examples of prior inves-
vided in Table 7, followed by a more detailed discussion, including key examples of
tigations.
prior investigations.
Polymers 2025, 17, 628 56 of 94

Table 7. An overview of common solvolysis processes.

Catalyst:
Polymer Method Agent Catalyst T (◦ C) t (min) Reactor P (atm) Yield % Ref.
Polymer
Di-n-butylamine 1:4 (mol%) 160 90 Three-necked flask 1 76.8 BHET [508]
Fe3 O4 -boosted 1 MWCNT 1:19 (wt%) 190 120 Stainless steel cylinder 1 100 BHET [509]
2 TBD:3 MSA 1:99 (wt%) 180 120 Schlenck flask 91.0 BHET [510]
4
1
POM:5 WZn3 1:2 (wt%) 190 40 Three-necked flask 84.5 BHET [511]
(Dimim)[FeCl4 ] 1:4 (wt%) 170 120 Three-necked flask 1 99.0 BHET [512]
6 [Ch][For] 1:19 (wt%) 180 180 84.5 BHET
Three-necked flask [513]
7 [Ch][OAC] 1:19 (wt%) 180 240 1 85.2 BHET
Glycolysis

EG MnO2 /holey GO nanosheets 1:10,000 (wt%) 200 10 Three-necked flask 100 BHET [514]
Acetaminde/ZnCl2
1:250 (wt%) 195 25 Three-necked flask 1 83.2 BHET [515]
DES@Zif-8
Orange peel ash 1:10 (wt%) 190 90 Two-necked flask 79.0 BHET [516]
Fe3 O4 @SiO2 @
3:20 (wt%) 180 1440 Round bottom flask 100 BHET [517]
(mim)[FeCl4 ] 1
PET
RZnO 1:100 (wt%) 196 120 50.0 BHET
Three-necked flask [518]
Co/RZnO 1:100 (wt%) 196 120 80.0 BHET
BLA 1:5 (wt%) 200 120 Autoclave 78.0 DMT [519]
Methanolysis

MeOH Modified ZnO 7:1000 (wt%) 170 15 Autoclave 1 95.0 DMT [520]
PIL-Zn2+ 1:50 (wt%) 170 60 Bottle reactor 90.3 DMT [521]
K2 CO3 1:5 (mol%) 25 1440 93.1 DMT
MeOH/CH2 Cl2 Round bottom flask 1 [501]
CH3 OK 1:5 (mol%) 25 1440 81.9 DMT
Marine water (metallic ions) 7:20 (wt%) 205 120 Stirred reactor 32.5 96.0 TPA
[522]
NaHCO3 + KHCO3 8:20 (wt%) 195 120 Stirred reactor 34.5 95.7 TPA
Hydrolysis

- - 230 30 Microwave 77.0 TPA

H2 O
- - 200 30 Microwave 12.0 TPA
~29 [523]
H+ @ZSM-5 1:2 (wt%) 230 30 Microwave 98.5 TPA
H+ @ZSM-5 1:2 (wt%) 200 30 Microwave 87.0 TPA
Polymers 2025, 17, 628 57 of 94

Table 7. Cont.

Catalyst:
Polymer Method Agent Catalyst T (◦ C) t (min) Reactor P (atm) Yield % Ref.
Polymer
Hexyl-amine - - 180 30 Microwave 64.0 8 DHTA
Ethanol-amine - - 200 10 Microwave 91.0 9 BHTA
[524]
82.0 10 BFTA
Aminolysis

Furfuryl-amine - - 200 60 Microwave 1

Allyl-amine - - 280 15 Microwave 61.0 11 DAA
Isophorenediamine Zn(OAc)2 1:10 (wt%) 200 240 Four-necked flask 90.0 TPA [525]
Ethanol-amine 12 mHpb 5:32 (wt%) 190 3 Three-necked flask 1 100 13 BHETA [526]
Ethanol-amine TBD 7:192 (wt%) 120 120 Schlenk flask 1 93.0 TPA [527]

Reductive de- H2 Ruthenium(II) PNN pincer 2:100 (mol%) 160 2880 Schlenk tube 54.4 >99 TPA, EG [528]
polymerization Et3 SiH B(C6 F5 )3 2:100 (mol%) 25 180 Stirred reactor 91.0 BDM-SI [529]
H2 CoMo@NC 3:10 (wt%) 260 1200 Sealed tube 1 91.0 TPA [530]
Hydrogenolysis
Pd/Hf/PET:
H2 Hf-(OTf)4 : Pd/C 180 1440 Schlenk flask 1 95–98 TPA [531]
1:6:400
14 IL - - 280 60 Microwave 0 caprolactam
IL - - 300 60 Microwave 36 caprolactam
IL 15 DMAP 1:10 (wt%) 300 60 Microwave 55 caprolactam [532]
1
PA6
IL DMAP 1:10 (wt%) 300 30 Microwave 24 caprolactam
IL DMAP 1:10 (wt%) 310 60 Microwave 54 caprolactam
Acid hydrolysis HCl - - 80 120 Round bottom flask 1 72.2 16 DBHMD [533]
1 2 3 4 5
MWCNT, multiwall carbon nanotube; TBD, 1,5,7-triazabicyclo[4.4.0]dec-5-ene; MSA, methanesulfonic acid; POM, polyoxometalates; WZn3 , Na12 [WZn3 (H2 O)2 (ZnW9 O34 )2 ];
6 [Ch][For], choline formate; 7 [Ch][OAC], choline acetate; 8 DHTA, dihexylterephthalamide; 9 BHTA, bis(2-hydroxyethyl)terephthalamide; 10 BFTA, bis(furan-2-
ylmethyl)terephthalamide; 11 DAA, diallylterephthalamide; 12 mHpb, methyl 4-(2,3,4,6,7,8-hexahydro-1H-pyrimido [1,2-a]pyrimidine-1-carbonyl) benzoate; 13 BHETA, bis(2-
hydroxyethyl) terephthalamide; 14 IL, hydrophilic ionic liquids [emim][BF4 ]; 15 DMAP, N,N-dimethylaminopyridine; 16 DBHMD, dibenzoyl derivative of hexamethylenediamine.
Polymers 2025, 17, 628 58 of 94

Glycolysis
Glycolysis is the most cost-effective and commercially viable process for the chemical
recycling of PET bottles. It uses excess glycol, commonly EG, to produce BHET (Figure 23a)
and its oligomers for a 180–240◦ C temperature range and considering a suitable pressure
to maintain EG in the liquid state. The mechanism of glycolysis consists of several steps.
Glycol first diffuses into the polymer and swells it. The diffused glycol then reacts with an
ester bond in the chain. The swelling increases the diffusion rate as well as the reaction rate
of glycolysis. The reaction rate increases with the polymer surface area. Hence, it is better
to make the PET chip smaller through grinding, cutting, etc. BHET is generally purified by
melt filtration under pressure and treated with AC to remove impurities and color [414].
The limited efficiency of the non-catalytic glycolysis of PET has prompted increased in-
terest in utilizing catalysts for this process. Thus, various metal salts and organocatalysts have
been used to enhance the reaction rate. Currently, the most frequently utilized catalysts for
PET degradation are multiphase catalysts made of metal oxides (e.g., ZnO, manganese oxide,
cobalt oxide, and zinc manganese oxide) and homogeneous catalysts made of metal acetates
(e.g., zince [Zn], Mn, and Co), ILs ([Bmim][Cl], [Bmim][AlCl4 ], and [Deim][Zn(OAc)3 ]), while
zinc acetate exhibits more activity for PET depolymerization [521].
Wang et al. [534] demonstrated that 1,3-dimethylimidazolium-2-carboxylate can
serve as an organocatalyst for PET glycolysis. Using a mass ratio of 50/5/0.75 for
EG/PET/catalyst and 20 mol% of 1,3-dimethylimidazolium-2-carboxylate relative to the
monomer, post-consumer PET was depolymerized completely within 1 h at 185 ◦ C. Upon
cooling, the reaction mixture yielded up to 60% BHET as a crystalline precipitate. Com-
pared to the basic IL (i.e., 1,3-dimethylimidazolium acetate), zwitterionic carbonate (i.e., 1,3-
dimethylimidazolium-2-carboxylate) proved to be a much more effective catalyst. PET
degradation was initiated more quickly at lower temperatures, leading to complete PET
degradation within 1 h using 1,3-dimethylimidazolium-2-carboxylate. In contrast, with
1,3-dimethylimidazolium acetate, only around 35% degradation was achieved after 1 h,
and up to 3 h were necessary to achieve a similar degree of depolymerization.
Typically, the glycolysis approach is utilized to recycle top-notch PET bottles and
fibers. As a preliminary measure, partial glycolysis can be implemented, which involves
the use of EG molecules to break down PET molecules into oligomers with a reduced
average molar mass. This process of glycolysis between PET bottles and EG is commonly
carried out through reactive extrusion. The resulting low-molar-mass oligomers can be
utilized as raw material for subsequent steps, such as methanolysis or hydrolysis, or for the
repolymerization process [535]. Furthermore, during glycolysis, the undesired by-product
diethylene glycol, which is a dimer of EG, is produced, posing challenges in the separation
and purification of the intended product.
The recycling challenges associated with specific fiber blends, such as polycotton, elas-
tane with polyester, and elastane with cotton, differ from those associated with other fibers
and textiles. Polycotton, a blend of polyester and cotton, presents significant difficulties due
to its combination of natural and synthetic fibers, complicating the separation and recycling
processes. Methods such as dissolution or glycolysis are often required to separate the
polyester from the cotton, but these processes tend to be both energy-intensive and costly,
and they must be selective to one of the fibers. Likewise, blends that include elastane with
polyester or cotton introduce additional challenges because elastane’s elasticity complicates
mechanical recycling, often leading to downcycling or disposal in landfills [59,536–538].
To overcome the aforementioned challenges, solutions such as selective dissolution or
solvolysis, which targets specific fibers within a blend, or enzymatic methods that break
down natural fibers while leaving synthetic ones intact can be considered. The selective
removal of one of the fibers or blends can then precede mechanical recycling or chemical
Polymers 2025, 17, 628 59 of 94

recycling techniques. Additionally, recycling could involve techniques such as thermal or

chemical processes in which separation can occur after depolymerization [228,289,536].

Hydrolysis
Hydrolysis of PET chains produces hydroxyl and carboxylic end groups. A water
molecule attacks the chain and causes its scission, creating a carboxylic end group. Al-
though hydrolysis has been actively studied, it is still not a commercially viable option.
One major obstacle is the purification problem of recycled TPA. It is difficult to purify TPA
from the reaction mixture due to its low solubility and vapor pressure. Some impurities in
PET waste that are not soluble in hydrous agents are not separated by transcrystallization
using CH3 COOH/H2 O [539].
The depolymerization process involves using water to break down PET chains into
TPA and EG, which can then be used in TPA-based PET synthesis plants. This process can
be carried out under neutral, acidic, or basic conditions, as shown in Figure 23b.
Hydrolysis of PET with water or steam under high pressure and temperature can
produce TPA and EG at a neutral pH. The hydrolysis rate is higher in a molten state
than in a solid state. Metal salts, such as zinc acetate and sodium acetate, can catalyze
hydrolysis reactions. Neutral hydrolysis does not produce undesirable liquid effluents
and is not corrosive. However, PET impurities require intensive purification for pure TPA.
Purification can be achieved through filtration, crystallization, extraction, or distillation of
TPA and EG [535].
Several contributions have described a process for the acidic hydrolysis of PET using
concentrated H2 SO4 at atmospheric pressure and temperatures ranging from 25 ◦ C to
100 ◦ C. The resulting hydrolysis product is then neutralized with NaOH, leading to the
formation of the corresponding TPA sodium salt (Na2 SO4 ), which is water-soluble. In the
final stage of the process, the resulting solution is acidified again to reprecipitate TPA with
99% purity. This process requires the separation of large amounts of concentrated H2 SO4
and the purification of EG containing H2 SO4 , which significantly increases the cost of the
process [50,540,541].
Ügdüler et al. [542] investigated the aqueous alkaline hydrolysis of pure PET and
post-consumer PET waste to obtain EG and TPA. They found that PET depolymerization
had the highest yield at 80 ◦ C, with a particle size lower than 500 µm and after 20 min in a
solution containing 40:60 vol% H2 O:EtOH and 5 wt% NaOH. They also found that the PET
conversion rate decreased with an increase in particle size, with the highest conversion rate
obtained from monolayer PET films at the smallest particle size. The proposed alkaline
hydrolysis process is promising for the chemical recycling of complex PET plastic waste,
but the parameters need to be adjusted for environmental sustainability.
Furthermore, polycotton, a popular material used in hospital and hotel service textiles,
such as sheets and towels, is a blend of cotton and PET. Recycling cotton-based textiles
is a challenge due to their common blending with PET in various ratios, resulting in a
structured blend that can hinder enzymes’ access to cotton. Compared to unblended cotton,
blended cotton has greater crystallinity and polymerization because it has a higher average
molar mass and intermolecular and intramolecular bonds [543].
Palme et al. [544] specifically examined a simple lab-scale method to hydrolyze PET in
polycotton waste. The process involved the use of 5–15 wt% NaOH in water at temperatures
ranging from 70 ◦ C to 90 ◦ C, which degraded PET to TPA and EG. The process generated
three output streams: cotton, TPA, and filtrate containing EG and process chemicals. PET
hydrolysis could be achieved in a 10% NaOH solution at 90 ◦ C in just 40 min with the
addition of a phase-transfer catalyst (benzyltributylammonium chloride). The yield of
cotton cellulose was high, up to 97%, depending on the duration of the sample treatment.
Polymers 2025, 17, 628 60 of 94

While the phase-transfer catalyst was not necessary for separation, longer treatment times
were required, resulting in more cellulose degradation.
The use of acidic or basic conditions for hydrolysis can lead to corrosion and pollution
issues. Additionally, the formation of TPA and acidic catalysts can promote the production
of diethylene glycol [545]. Despite ongoing research, hydrolysis is currently not a feasible
option for commercial use due to the difficulty of purifying recycled TPA. Purification of
TPA from the reaction mixture is challenging due to its low solubility and vapor pressure.
Moreover, the use of CH3 COOH and H2 O for transcrystallization may not effectively
separate impurities in PET waste that are insoluble in aqueous agents.
The reduction in the degree of polymerization of cellulose by breaking down its
β-1,4-glycosidic bonds is known as cotton depolymerization. Various methods can be
employed for depolymerizing cotton fibers, such as hydrolysis, enzymolysis, and fermen-
tation. Hydrolysis is affected by several factors, such as the heating source, the type of
solvent (acid, base, or neutral), and the process’s duration. Cotton is transformed into
glucose and solid fiber residues through the hydrolysis process. This process depolymerizes
cellulose completely into its monomer, glucose, which can be used to create other chemicals,
such as EtOH, organic acids, cellulose nanocrystal (CNC), and microcrystalline cellulose
(MCC) [546].
Sanchis-Sebastiá [547] conducted a two-step acid hydrolysis process on cotton waste
to extract glucose. The first step involved dissolving textile waste in a concentrated H2 SO4
solution at a concentration of 60–80 wt% and a temperature of 30 ◦ C for 1 h. The second
step used a dilute H2 SO4 solution at a concentration of 5 wt% and a temperature of 121 ◦ C
for 1 h in an autoclave to fully break down the cotton and form glucose. After these steps,
the mixture was vacuum filtered to obtain liquid and solid fractions for further analysis.
The two-step approach resulted in a high glucose yield of around 80–90%, which could not
be achieved using concentrated or dilute H2 SO4 alone.
CNC and MCC possess distinct mechanical, optical, and thermal characteristics that
render them appealing for a diverse range of applications in industries such as biomed-
ical engineering, electronics, and packaging. CNC can be obtained through different
methods, including the use of a H2 SO4 /HCl aqueous solution, 60 wt% H2 SO4 , and 2,2,6,6-
tetramethylpiperidine 1-oxy (TEMPO) oxidation. CNC has been produced from bleached
white cotton fabric and indigo-dyed denim fabric via 60 wt% H2 SO4 or TEMPO oxidation.
Acid hydrolysis produced CNC yields of 40% and 38% for bleached cotton and denim
fabrics, respectively, whereas oxidation generated greater yields of 73% and 79% [548]. Acid
hydrolysis and oxidation were also used to extract CNC from cotton fabric, with yields of
90% and 60%, respectively. MCC was obtained with phosphotungstic acid at 140 ◦ C for 6 h,
achieving a high yield of 83.4% [548].
Kamimura et al. [532] developed a new technique for depolymerizing PA6 into capro-
lactam using hydrophilic ILs [emim][BF4 ]. The process was significantly enhanced with the
addition of catalytic quantities of N,N-dimethylaminopyridine [DMAP]. Under microwave
radiation at 300 ◦ C, PA6 was effectively depolymerized in hydrophilic ILs, with complete
conversion within 1 h. As a result of this reaction, by utilizing a catalyst (10 wt%), the
recovery rate of [emim][BF4 ] was found to vary from 82% to 89%, while the recovery rate
of caprolactam as a PA6 monomer was observed to be between 54% and 62%. Similarly,
Kamimura and Yamamoto [549] employed DMAP and various IL solvents to depolymerize
PA6 at a temperature of 300 ◦ C. Among the solvents used, N-methyl-N-propylpiperidinium-
bis(trifluoromethanesulfonyl)imide exhibited the most favorable outcome, with 86% capro-
lactam retrieval.
Polymers 2025, 17, 628 61 of 94

Methanolysis
PET methanolysis offers several benefits, including obtaining N,N-dimethyltryptamine
(DMT) of identical quality to virgin DMT, simple purification of DMT, and facile recovery
of EG and CH3 OH. This technique exhibits a relatively high tolerance of contaminants,
allowing it to process low-quality feedstocks [519].
In the methanolysis process of PET, CH3 OH can be utilized in three different states:
liquid, superheated vapor, and supercritical fluid. The process of PET methanolysis involves
breaking down PET chains by reacting them with CH3 OH under a high temperature
(180–280 ◦ C) and pressure (20–40 atm). Transesterification catalysts (e.g., zinc acetate,
cobalt acetate, magnesium acetate, and lead dioxide) are commonly utilized to facilitate the
reaction. The yield of DMT typically falls between 80% and 85% [550,551]. Alternatively,
superheated CH3 OH vapor can be used instead of liquid CH3 OH to react with oligomers
or crude BHET (obtained through glycolysis) by passing the CH3 OH vapor through the
glycolysis product. The production of DMT increases with higher CH3 OH feeding rates
and reaches its maximum output at a reaction temperature of 250–260 ◦ C and 3–6 atm
reaction pressure. This vapor methanolysis method has proven successful in processing
PET waste [552].
More recently, the use of supercritical CH3 OH at temperatures exceeding 300 ◦ C
and pressures above 80 atm has also been applied to PET methanolysis [519,540]. Using
supercritical CH3 OH, Liu et al. [553] were able to depolymerize PET into monomer DMT
rapidly and completely. The influence of the MeOH-to-PET mass ratio on the response
surface was found to be less significant than that of the reaction temperature and time
within the studied range of experimental conditions. The optimal operating conditions for
methanolysis were determined to be 112 min, 298 ◦ C, and a mass ratio of 6/1 MeOH/PET.
The results showed that PET could be quickly and completely decomposed to its monomer
DMT under supercritical CH3 OH conditions. The degree of depolymerization and selec-
tivity for DMT increased with higher CH3 OH/PET ratios and reaction temperatures. The
experimental conditions based on the optimal values led to a high DMT yield of 99.8%,
which was in good agreement with the predicted value.
Numerous catalysts have been employed to hasten PET depolymerization, and their
effectiveness with regard to the depolymerization rate, environmental impact, by-products,
and process expenses has been evaluated. Ongoing research is exploring a range of catalysts
for this purpose. For instance, Jiang et al. [521] employed a poly(IL))-Zn2+ (PIL) catalyst to
carry out the methanolysis of PET in an efficient and eco-friendly manner. The findings
suggest that the reaction temperature is a crucial aspect that affects the process. Under
conditions in which the CH3 OH to PET mass ratio was 3:1 and the quantity of PIL-Zn2+ was
2% of the PET mass, complete PET conversion and 89% DMT yield were attainable through
methanolysis at 170 ◦ C for 60 min. The PIL-Zn2+ catalyst was reused six times without
significant performance degradation, implying that poly(IL) may replace conventional
compounds in the industrial application of PET catalytic methanolysis.
Tang et al. [554] utilized MgO/crystalline sodium Y (NaY) catalysts to perform PET
methanolysis. The 21%MgO/NaY catalyst displayed notable catalytic activity in this pro-
cess. For a CH3 OH-to-PET mass ratio of 6, a catalyst dosage of 4 wt%, a temperature of
200 ◦ C, and a reaction time of 30 min, the yield of DMT and the conversion of PET reached
91% and 99%, respectively. The excellent catalytic performance of the 21%MgO/NaY
catalyst was attributed to its robust basic sites, large pore size, and high specific surface
area. Furthermore, the catalyst alkalinity was found to positively affect PET conversion
and DMT yield. Remarkably, the catalyst retained its high catalytic activity even after
undergoing six repeated cycles. These results demonstrate that the 21%MgO/NaY catalyst
has numerous benefits, such as high efficacy, simple recovery, reusability, and robustness.
Polymers 2025, 17, 628 62 of 94

After regeneration, the catalyst’s activity returned to the level of activity of the unused cata-
lyst. Therefore, utilizing 21%MgO/NaY as a catalyst for PET methanolysis is a promising
approach for chemical recycling of PET.

Aminolysis
PET aminolysis involves the recycling of PET by reacting it with various primary amine
solutions, including methylamine, allylamine, ethanolamine, ethylamine, and hydrazine,
in aqueous form (Figure 23d). This reaction leads to the formation of the diamides of TPA
and EG.
Amines, being organic bases, cause faster depolymerization compared to alcohols.
Catalysts and pre-catalysts (e.g., ILs) utilized in other solvolysis procedures can also
exhibit effectiveness in this context. However, this process has not yet been upscaled to an
industrial scale, which makes it less feasible to use economically. The temperature range
for this process is between 20 ◦ C and 100 ◦ C. Meanwhile, using various types of amines in
the aminolysis process can lead to the production of other products, such as a hydrogel
adsorbent [555] or a high-temperature cross-linking agent for unsaturated polyesters [556].
Notably, using deep eutectic solvents synthesized with choline chloride.x ZnCl2 and
choline chloride.2 CH4 N2 O as catalysts, Musale and Shukla [557] employed aminolysis
by ethanolamine and diethanolamine to depolymerize PET waste. Reaction parameters,
including the time of aminolysis, the catalyst concentration, and the PET/amine ratio, were
optimized. The pure products obtained were TPA, N1 ,N1 ,N4 ,N4 -tetrakis(2-hydroxyethyl)-
terephthalamide, and bis(2-hydroxyethylene) terephthalamide (BHETA), which were ob-
tained in yields of 83, 82, and 95%, respectively.

Ammonolysis
The degradation of PET through ammonolysis involves the attack of anhydrous NH3
on PET in an EG medium at temperatures between 70 ◦ C and 180 ◦ C under pressure,
producing terephthalamide and EG. EG is used in the reaction atmosphere to facilitate
heat and reaction exchanges and acts as a partial PET solvent. The process can lead to a
high-purity product with a yield of about 90% [558].
Ammonolysis, which involves the use of NH3 to depolymerize PET, has not been
as extensively researched as other chemical recycling methods. This is because the prof-
itability of the process depends on the economic potential of the resulting degradation
products [559].
Furthermore, ammonolysis is a slower process than aminolysis and usually necessi-
tates the use of a catalyst to increase the depolymerization rate. Catalysts, such as zinc
acetate or ammonium quaternary salt, can reduce the reaction time and yield a terephthala-
mide that can be used as an epoxy hardener or intermediate in other applications [539].

Hydrogenolysis
In terms of a circular economy, heterogeneous catalysts that are durable and recyclable
are better suited for the hydrogenolysis-based recycling of PET [530,531,560]. Unlike
reductive depolymerization, which is a hydrogenative recycling type, hydrogenolysis does
not require expensive high-pressure equipment. This feature makes it a safer and more
convenient option.
For example, Kratish et al. [561] applied a heterogeneous carbon/molybdenum dioxide
catalyst for PET hydrogenolysis. This catalyst exhibited remarkable selectivity because
its molybdenum (Mo) sites could selectively activate and cleave ester groups. However,
it had low efficiency in PET hydrogenolysis due to its poor ability to activate H2 . More
recently, Ye et al. [562] employed ruthenium (Ru)/TiO2 to hydrogenolyze the C–C and C–O
bonds of PET, converting it into a series of aromatics. Ru/TiO2 possesses an exceptional H2
Polymers 2025, 17, 628 63 of 94

activation capacity, enabling it to hydrogenolyze PET. The most efficient catalyst for the
conversion of PET to BTX (77%) was the one with a Ru size of ~1.1 nm and a coordination
number of ca. 5.0, which had dominant edge/corner sites. Larger-sized Ru catalysts
produced more ring hydrogenation and subsequent ring-opening products.
Zeolitic imidazole frameworks (ZIFs) have also shown potential as a support for metal
catalysts in recent years. Multimetallic ZIFs and their derivatives may exhibit superior
catalytic performance compared to their monometallic counterparts, and they have been
shown to be an effective method for creating bimetallic and multimetallic catalysts.
Note that under solvent-free and atmospheric H2 pressure conditions, Wu et al. [530]
developed a new and effective heterogeneous bimetallic catalyst (CoMo@NC) for PET
hydrogenolysis. The catalyst was prepared through pyrolysis of the Mo@ZIF-CoZn precat-
alyst in a special procedure. In the optimum range of process parameters (catalyst/PET: 0.3,
H2 : 1 atm, 260 ◦ C, 10 h), TPA was obtained with a high yield (91%). This catalytic approach
offers numerous benefits, such as high monomer yields, the absence of a need for reagents
or solvents, the use of atmospheric H2 , low cost, and being a reusable catalyst. The Mo
sites in the bimetallic catalyst primarily and effectively catalyze β-scission, while the Co
sites activate H2 and catalyze the hydrogenolysis process. The coordination between the
two metals substantially enhances catalytic efficiency.
Kratish and Marks [531] applied a combination of homogeneous (hafnium trifluo-
romethanesulfonate [Hf-(OTf)4 ]) and heterogeneous (palladium on carbon [Pd/C]) cata-
lysts as a tandem catalytic system to catalyze selective PET hydrogenolysis without the
need for solvents. Under a 1 atm pressure of H2 and optimum ranges of parameters
(PET/Hf/Pd: 400/6/1, 180 ◦ C, 24 h), PET hydrogenolysis resulted in high yields and
selective formation of the corresponding monomers (TPA).
Recently, Kumar et al. [563] reported the first experience of hydrogenative depoly-
merization of conventional polyamide using a green and sustainable approach based on
hydrogenation in the presence of a Ru pincer catalyst at 150 ◦ C and 70 bar H2 . They also
demonstrated the hydrogenation of PU to produce diol, diamine, and CH3 OH using the
same catalytic conditions.
The hydrogenation process is definitely a promising process and has high potential,
but the long reaction time is still challenging. It is necessary to shorten the reaction time for
the recycling process to become economically competitive. Using an extruder to quickly
melt the plastic, increasing the H2 pressure, and using more active catalysts can be effective
in this field.

Reductive Depolymerization
Reductive depolymerization has emerged as a promising alternative approach for the
utilization of polycondensation plastics in recent years. It has gained popularity because it
enables plastic waste to be converted into value-added products that cannot be obtained
using other recycling techniques. Catalysts play a crucial role in this process and must
possess high activity, low cost, and stability in the presence of air, moisture, organic
compounds, and metallic contaminants [564].
Silanes have been employed as reducing agents in the reduction of PET waste into
smaller units in the presence of various organic and organometallic catalysts. PET waste was
subjected to reductive depolymerization using B(C6 F5 )3 (2 mol%) and Et3 SiH (4.3 equiv.)
at ambient temperature, which resulted in the formation of two disilylethers: BDM(1,4-
benzenedimethanol)-Si and EG-Si, with yields of 85% and 72%, respectively. Upon hydrol-
ysis of these disilylethers using tetrabutylammonium fluoride trihydrate (TBAF·3H2 O),
1,4-benzenedimethanol and EG were obtained quantitatively (Figure 23f) [529].
 Polymers 2025, 17, x FOR PEER REVIEW 69 of 104
Polymers 2025,
Polymers 17,17,
2025, 628x FOR PEER REVIEW 64 of 94
69 of 104

Different organometallic catalysts have been employed to develop various instances

Different
of hydrogenative organometallic
Different organometallic
depolymerization catalysts
catalysts have
of have
PET been
been
waste. employed
employed
Krall to develop
to [528]
et al. develop various
various
applied instances
instances
Ru(II) PNN
of hydrogenative
of hydrogenative
pincer depolymerization
complexes depolymerization of PET waste.
of PET waste.
(Figure 24) in a controlled Krall
Krall
catalytic et al. [528] applied
et al. [528] applied
hydrogenation Ru(II) PNNPNN
Ru(II)
depolymerization
pincer
pincer complexes
techniquecomplexes (Figure24)
(Figure
to depolymerize 24)ininTo
PET. aacontrolled
controlled
overcome catalytic
catalytic
the hydrogenation
hydrogenation
low solubility depolymerization
of PET,depolymerization
a mixture of ani-
technique
technique
sole to depolymerize PET. To
to depolymerize(THF) (50:50)
and tetrahydrofuran overcome
overcome the low solubility
the lowtosolubility
was utilized hydrogenate of PET,
of PET, a mixture
thisapolymer.
mixture of Aofani-
anisole
Ru
and
soletetrahydrofuran
complex (THF)
tetrahydrofuran
and was considered (50:50)
a(THF) was
(50:50)
catalyst utilized to hydrogenate
was utilized
at a concentration 2 mol%,this
toofhydrogenate polymer.
thiswith
along A Ru
polymer.
54.4 Acomplex
atm Ru
of
complex
H
was2 at 160 was
°C for
considered considered
catalyst aatof
a duration catalyst
a48 at a process
h. This concentration
concentration of resulted
2 mol%, ofin2 outstanding
mol%,
along withalong with
atm 54.4
of Hatm
54.4conversion 2 of ◦ C
rates,
at 160
H2 aatduration
1601,4-benzenedimethanol
yielding
for °C forofa duration
48 h. This of 48 h. This
and
process EG.process resulted
resulted in outstanding
in outstanding conversion
conversion rates,rates,
yielding
yielding 1,4-benzenedimethanol
1,4-benzenedimethanol and EG.and EG.

Figure 24. Catalytic

Figure Catalytichydrogenation
hydrogenationofofPET
PETviavia
Ru(II) PNN
Ru(II) pincer
PNN complexes
pincer [528].
complexes [528].
Figure 24. Catalytic hydrogenation of PET via Ru(II) PNN pincer complexes [528].
The method
methodofof regeneration
regenerationis applicable to various
is applicable types oftypes
to various plastics,
of including PVC,
plastics, including
PVC, and allows for dechlorination, as presented in Figure 25. Monsigny etPVC,
and The
allows method
for of regeneration
dechlorination, as is applicable
presented in to various
Figure 25. types
Monsignyof plastics,
et al. including
[565] specifically
al. [565]
and allows
applied
specifically for dechlorination,
an iridium
applied catalyst for as
an iridium presented
thecatalyst in the
Figure
dechlorination
for of 25. Monsigny
PVC at 110 °Cof
dechlorination et PVC
for al.
72[565]
h,at specifically
resulting
110 ◦ C in
fora 72 h,
applied aniniridium
conversion
resulting rate catalyst for
of approximately
a conversion theof
rate dechlorination
42%. Nevertheless,
approximately of PVC
42%.at 110
challenges °C foras72
such
Nevertheless, h, resulting
insufficient in asuch
mon-
challenges
conversion
omer rate
retrieval, of approximately
purification 42%.
complexities, Nevertheless,
stringent challenges
conditions, andsuch
the as
need
as insufficient monomer retrieval, purification complexities, stringent conditions, and insufficient
for mon-
hazardous
omer retrieval,
solvents purificationagents
and degradation complexities,
impede stringent conditions,of
the implementation and the needdepolymeriza-
reductive for hazardous
the need for hazardous solvents and degradation agents impede the implementation of
solvents and degradation agents impede the implementation of reductive depolymeriza-
tion.
reductive depolymerization.
tion.

Figure Reductivedechlorination
Figure 25. Reductive dechlorinationofof PVC
PVC to to
PEPE with
with thethe iridium
iridium catalyst/Et
catalyst/Et 3SiH 3 SiH [565].
[565].
Figure 25. Reductive dechlorination of PVC to PE with the iridium catalyst/Et3SiH [565].
Furthermore,
Furthermore, this thisapproach
approachfrequently
frequently necessitates
necessitates highhigh
H2 H 2 pressures,
pressures, problematic
problematic
organicFurthermore,
solvents, this
and approach
additives. In frequently
addition, necessitates
Ru-based high
homogeneous
organic solvents, and additives. In addition, Ru-based homogeneous catalysts H 2 pressures,
catalystsproblematic
are air-sen-
are air-
organic
sitive,
sensitive, solvents,
costly, and
andand
costly, additives.
challenging to In
challenging addition,
separate
to andRu-based
separate reuse homogeneous
[528].
and reuse [528]. catalysts are air-sen-
sitive, costly, andcan
Polyamides
Polyamides challenging
can also to separate and
alsobebedepolymerized
depolymerized reuse
using [528].
reductive
using reductive depolymerization,
depolymerization, which has has
which
the Polyamides
benefit of not can also
generatingbe depolymerized
stoichiometric using
waste, reductive
as with depolymerization,
traditional reducing
the benefit of not generating stoichiometric waste, as with traditional reducing agents. which
agents. has
In In
the benefit
this
this field, of not generating
field, proficient
proficient Ru
Rupincer stoichiometric
pincer catalysts have
catalysts waste,
have been as discovered
with traditional
discovered
been reducingamides
to hydrogenate
to hydrogenate agents. In by
by
amides
this field,
cleaving proficient
C–N bonds, Ru pincer
producing catalysts
amines have
and been
alcohols discovered
[566]. to
Other hydrogenate
homogeneous
cleaving C–N bonds, producing amines and alcohols [566]. Other homogeneous catalysts amides by
catalysts
cleavingon C–N bonds,
and producing amines
beenand alcohols
for [566].
based
based on RU, Fe,
RU, Fe, andMn Mnhave
havealso
also reported
been reported thisOther
this purpose.
for homogeneous catalysts
purpose.
based on RU, Fe, and Mn have also been reported for this purpose.
4. Technology Assessment of Textile Fiber Recycling
Assessing the recycling of textile fibers, whether single or blended, presents numerous
challenges. The suitable recycling method varies based on the fiber type, chemical structure,
and purity, among other factors [60]. In the initial stage, mechanical recycling is preferred
Polymers 2025, 17, 628 65 of 94

after reuse whenever feasible, particularly in cases of high purity [289,567]. Second, alterna-
tive methods, such as dissolution, are often applicable to natural polymers. However, when
it comes to synthetic plastics, dissolution typically demands significant energy and solvent
usage [194,287,359,365]. If other methods are not viable, chemical recycling techniques,
such as pyrolysis for polyolefins and solvolysis for fibers (e.g., polyester and polyamide),
can be employed [441,499,538]. For blended fibers, such as those combining polyester and
natural fibers, a combined dissolution-solvolysis approach can effectively dissolve natural
fibers and facilitate the depolymerization of polyester fibers [536].
Table 8 provides an overview of the various methods utilized in the industry to recycle
different types of fibers.

Table 8. Technology assessment of closed-material-loop end-of-life options for different fiber types.

Fiber Type
Blends
Closed-loop end-of-life option Natural fibers Synthetic fibers
elastane + cotton/polyamide/PET
Reuse If textiles or fibers are reusable, they are a more suitable option than the other alternatives [189].
Good option, but needs high
Good option, but shortens fiber Elastane makes this
Fiber recycling purity and shortens fiber
length [60,270,310] incompatible [312,315].
length [289,567,568]
Polymer recycling (re-extrusion)
- Good option [322,325,326] -
via melting
Good option for removing
additives and contaminants in
Polymer recycling (re-extrusion) Good option for separating
Good option [287,365] polymers, but high energy
via dissolution cotton [40,364]
consumption; under
research [194,359,362]
Selectivity elastane vs. PET
Good option for pure PET and
Monomer recycling via solvolysis - needed (complicated but
polyamide [499,500,515,532,533]
possible) [59,536,538]
Good option for
Monomer recycling via pyrolysis - -
polyolefins [434,437,438,441]
Monomer recycling via
Good option [419,421,426,428] - -
biological processes
Monomer recycling When options are limited due to low purity and high degree of contamination, gasification can be a
via gasification suitable alternative [467,469–471].
Combination of
- - Good option [289,536]
dissolution + solvolysis
Combination of biological
- - Good option [66,536]
processes + solvolysis

5. Life Cycle Assessment

As explained above, nowadays, the end-of-life treatment of textiles, both synthetic and
natural, mainly involves disposal in landfills and incineration, with a small proportion be-
ing recycled using conventional methods, such as mechanical and chemical recycling [569].
Moreover, the most widespread mechanical recycling option often requires downcycling
because the loss of textile quality is inevitable. The increase in textile waste is additionally a
global problem driven by fast-changing trends, increasing population numbers, and rising
purchasing power, particularly in developing countries.
Complementary to the further development of mechanical recycling methods, chem-
ical recycling is thus likely necessary to close the recycling loop [542]. However, the
energy intensity of certain processes, as well as reactant consumption, raises the question
of whether such a recycling pathway has a lower impact than state-of-the-art processes.
An additional question is how to select a preferable technology from among many con-
Polymers 2025, 17, 628 66 of 94

cepts. In this context, LCA has become a standard [570] method for estimating the overall
environmental footprint of a process.
Shen et al. [571], for instance, focused on the chemical recycling of PET through
methanolysis to produce DMT and EG. This reaction occurred in the presence of catalysts,
such as Zn, Co, or Mg acetates or lead dioxide, at a pressure of 2–4 MPa and a temperature of
180–280 ◦ C. DMT was recovered from the reaction mix through precipitation, centrifugation,
and crystallization. The recycled polymer was then converted into fiber via the spinning
and finishing processes. The authors considered cradle-to-gate LCA and used a cut-off
approach to define the cradle of the recycled polymer as the collection and transportation
of PET waste. Three cases—low, high, and average recycled PET—were considered. The
low case assumes zero PET loss and 100% recovery of EG, the high case assumes 10% PET
loss and no EG recovery, and the average case assumes 5% PET loss and 50% EG recovery.
The net CH3 OH input was assumed to be zero for the low case, 10% for the high case, and
5% for the average case. The resulting carbon footprint, estimated with the global warming
potential (GWP) 100a model [572], is 2.71, 3.08, and 3.44 kg of CO2 equivalent per kg of
treated PET, respectively.
Ügdüler et al. [542] applied a two-step aqueous alkaline hydrolysis approach for
PET recycling. Mass and energy balance simulations were conducted using Aspen Plus
software, while LCA was performed using open LCA. The hydrolysis process was carried
out under mild conditions, yielding approximately 95% of the PET monomers, EG, and
TPA in less than 20 min. The purity of these monomers was confirmed through various
characterization techniques. The study revealed that the degradation rate is inversely
proportional to the particle size and that the decomposition yield is affected by factors such
as the thickness and presence of multilayers in PET samples. The researchers performed
LCA under system boundaries similar to those in a previous work [571]. Various solid
feed/alkaline solution (S/L) ratios were tested, and the results revealed that keeping the
S/L ratio at a minimum of 0.04 g mL−1 decreases the process’s carbon footprint below
virgin production levels.
The LCA results demonstrated that the hydrolysis process has the potential to yield
environmental savings in terms of carbon emissions compared to incineration, a common
practice for complex PET waste streams, such as PET trays and films. The energy con-
sumption during solvent and product recovery constitutes the largest share (>55%) of GHG
emissions (Table 9). The study concluded that industrial optimization of the hydrolysis
process can result in significant environmental benefits in terms of reduced carbon emis-
sions. Furthermore, the process has the potential to recycle other polymers from multilayer
structures, such as PE, from PET trays. Moreover, the successful removal of various colors,
including carbon black, from the hydrolysate demonstrates the versatility of this method,
paving the way for increased recycling rates of PET trays and films, which have historically
been challenging to recycle due to their complex compositions and poor collection rates.

Table 9. Results of the LCA work presented in Ügdüler et al. [542].

S/L Ratio Estimated GHG Emissions [kg CO2 eq/kg of Recycled PET]
0.02 5.6
0.03 3.9
0.04 3.0
0.05 2.4

In the case of natural fibers, such as cotton, open-loop chemical recycling is prevalent
over closed-loop recycling. In this framework, Paunonen et al. [573] investigated the
cellulose carbamate (CCA) process as a compelling alternative for producing man-made
Polymers 2025, 17, 628 67 of 94

fibers. It is compatible with traditional viscose spinning processes, allowing existing mills
to easily adopt it. In the CCA process, dissolving pulp is combined with CH4 N2 O at high
temperatures, causing CH4 N2 O to break down into isocyanic acid (HNCO) and NH3 . The
highly reactive HNCO then forms carbamates with cellulose hydroxyl groups. These newly
created carbamate groups enhance the solubility of cellulose in aqueous NaOH, enabling
the dissolved CCA to be transformed into textile fibers within an acidic coagulation bath.
The authors assume that the properties of such fibers are comparable to those of traditional
viscose fibers; hence, the cut-off cradle-to-gate system boundary was selected.
In greater detail, it includes sorting discarded cotton textiles, transportation, and the
CCA process itself, from shredding the cotton textile to CCA fiber spinning and bailing.
Two scenarios were considered: one with a standalone CCA factory and one integrated
with a pulp mill setup. The standalone facility has shown a significantly higher carbon
footprint than typical viscose production from wood pulp. In contrast, the integrated
scenario has proven to be able to reduce GHG by up to 40% below the reference value.
Besides GHG reduction, the CCA process consumes significantly less water, only 31 L per
kg of produced fiber (integrated case), whereas a conventional viscose factory consumes
445 L, and cotton growing and processing consume up to 4342 L.
To fairly compare the described processes, the cradle-to-gate carbon footprints of
recycled fibers have also been benchmarked against corresponding virgin fiber production
with state-of-the-art processes. The impacts of the latter have been quantified, for instance,
with the SimaPro package and the ecoinvent 3.8 database, using the GWP
Polymers 2025, 17, x FOR PEER REVIEW
100 impact
73 of 104
assessment method. Interestingly, this baseline approach (Figure 26) is consistent with the
values disseminated in the literature [573].

6 6
5.5
kg CO2 eq per kg of fiber

5
4.54
4
3.51 3.44
3 3.12
2.71
2.4
2 1.9

1 1.15

0
v-PET r-PET, r-PET, v-Cotton v-Viscose r-Viscose,
methanolysis hydrolysis CCA

Figure 26. Carbon footprint ranges of state-of-the-art virgin and recycled fiber production.
Figure 26. Carbon footprint ranges of state-of-the-art virgin and recycled fiber production. v-PET =
v-PET = virgin PET; r-PET = recycled PET via methanolysis pathway [571]; r-PET, hydrolysis = PET
virgin PET; r-PET = recycled PET via methanolysis pathway [571]; r-PET, hydrolysis = PET recycled
recycled via the alkaline hydrolysis pathway [542]; v-Cotton and v-Viscose = virgin fibers; r-Viscose,
via the alkaline hydrolysis pathway [542]; v-Cotton and v-Viscose = virgin fibers; r-Viscose, CCA =
CCA = cellulose carbamate fiber derived from waste cotton [573].
cellulose carbamate fiber derived from waste cotton [573].

Since the typical end-of-life scenario for polymer waste, particularly in Belgium, is
6. Eco-Design
incineration [574], it is necessary to include its impact in the comparison because the benefit
To address
of recycling is a the environmental
substitute process challenges associated
for both virgin with
material textile waste,
production it is crucial
and waste end-of-life
not
treatment. Hence, the baseline carbon footprint is expressed in Figure 26recycling
only to develop commercially feasible collection, sorting, pretreatment, and as a range, in
processes
which thebut also limit
lower to change
is thehow textile products
contribution of the are designed process
production in the first place.
alone, andBythe
im-upper
plementing certain design principles, the need for recycling as an end-of-pipe solution for
boundary includes waste treatment as well.
textile waste can be reduced, and the efficiency of end-of-life processes can be enhanced.
These principles, commonly called “eco-design”, focus on making textiles easier to recy-
6. Eco-Design
cle, extending product lifecycles, and reducing waste at the source. “Design for recycling”
To address the environmental challenges associated with textile waste, it is crucial
is a subset of eco-design concerned with facilitating recycling processes [575].
not only to develop
The first commercially
eco-design principle isfeasible collection,
designing sorting,
for longevity, pretreatment,
which emphasizes and recycling
using
high-quality fibers, reinforcing weak points (e.g., seams), and incorporating repairable,
replaceable, or modular features (e.g., attached via zippers), thus creating durable and
easily customizable products. For garments specifically, it is also important to both design
the aesthetics to be timeless rather than what is encouraged by fast fashion trends [576]
Polymers 2025, 17, 628 68 of 94

processes but also to change how textile products are designed in the first place. By
implementing certain design principles, the need for recycling as an end-of-pipe solution
for textile waste can be reduced, and the efficiency of end-of-life processes can be enhanced.
These principles, commonly called “eco-design”, focus on making textiles easier to recycle,
extending product lifecycles, and reducing waste at the source. “Design for recycling” is a
subset of eco-design concerned with facilitating recycling processes [575].
The first eco-design principle is designing for longevity, which emphasizes using
high-quality fibers, reinforcing weak points (e.g., seams), and incorporating repairable,
replaceable, or modular features (e.g., attached via zippers), thus creating durable and
easily customizable products. For garments specifically, it is also important to both design
the aesthetics to be timeless rather than what is encouraged by fast fashion trends [576] and
to encourage modularity and adaptability, such as by allowing consumers to change their
clothing by attaching or detaching sleeves, hoods, etc. This approach extends the lifespan
of textile products, thus reducing waste generation, the overall demand for replacement
products, and the associated environmental impact. Extending a garment’s life by just three
months, for example, has been found to reduce its carbon, water, and waste footprints by
5–10% each [577].
A second eco-design principle is related to material selection, as the environmental
impact of a virgin product and its recyclability are directly tied to the material. For instance,
using renewable, biodegradable, and recycled materials ensures that textiles have a lower
environmental impact and are likely to be recovered at the end of their lives. Organic
cotton, TencelTM , and recycled polyester are favored for their lower energy requirements
and recyclability. Purposefully using mono-materials (textiles made from a single type
of fiber) is also crucial because it simplifies the recycling process, removing the need for
separation and sorting of mixed textiles, which is challenging and resource-intensive.
Mono-materials thus allow for streamlined recycling processes that yield higher-quality
secondary raw materials [578].
A third eco-design principle concerns additives in textile products. While products
without any additives would be the easiest to recycle, they are necessary for the product’s
function (e.g., dyes in clothing) and may increase its lifespan. Hence, this principle may
contradict the design-for-longevity principle. For example, applying durable press finishes
or hydrophobic finishes to garments may reduce their need for care and maintenance, thus
reducing the environmental impact of such processes (e.g., laundering) and extending the
garments’ lifespans (washing clothes is detrimental to their lifespans). However, many of
these finishing compounds (e.g., fluorocarbon-based hydrophobic finishes) interfere with
recycling processes and are difficult to remove, thus remaining in the recycled product and
lowering its quality. Colorants have a less ambiguous nature and should be chosen to be
easily removable from textile waste with a common treatment process [262].
A fourth eco-design principle is design for disassembly. Garments incorporating
multiple components, such as buttons, zippers, and linings, can slow the recycling process
down. Designing textiles with fewer fasteners or using fasteners that can be easily removed
or recycled alongside the fabric significantly improves recyclability [312]. A recent example
is the manufacture of textile articles with special stitching threads that can be disintegrated
at the end of the product’s life cycle without damaging the rest of the product. This means
no cutting occurs, so the textile pieces maintain their maximum size (i.e., allowing high-
quality mechanical recycling). The downsides are that the system is limited to stitched
goods and that identifying the thread at the end of an article’s life cycle may be challeng-
ing [194,269]. To date, two companies offer these yarns: Resortecs and Wear2. The Resortecs
threads can be broken down by applying heat (between 150 ◦ C and 190 ◦ C) [579], while
Polymers 2025, 17, 628 69 of 94

the Wear2 threads contain metallic particles and can thus be disintegrated by applying
microwaves [580].
Before disassembly can take place, textile waste needs to be collected and sorted.
Hence, a fifth eco-design principle is design for identification. If a waste product can be
fully identified with a simple system at the end of its life cycle, that information can be
used to sort it into the correct waste category without any external analysis. Concepts such
as RFID tags and photonic crystals, are excellent examples of this principle [208,209].
A final example of a design principle concerns efficient production techniques. Reduc-
ing the amount of water, energy, and chemicals required during manufacturing can lead to
significant environmental savings. For example, techniques such as cold dyeing and digital
printing reduce energy and water use compared to traditional methods [581].
While not a principle of product design, it is important to note that exploring new
business models that can disrupt traditional linear consumption patterns is vital to the
industry’s sustainability. Companies can implement take-back schemes, such as collecting
and repurposing old products or adopting rental and leasing services, particularly for items
typically used infrequently, such as formal wear. These models not only reduce waste but
also create new revenue streams and customer engagement opportunities [582,583].
Addressing the aforementioned eco-design principles and business models collec-
tively can drive significant progress toward a more sustainable textile industry. A holistic,
integrated approach mitigates environmental impacts and fosters a more responsible and
resilient industry capable of adapting to the growing demand for sustainability from
consumers and regulators alike.
Several manufacturers are leading the integration of recycling processes in textile
production. REPREVE® produces performance fibers from recycled plastic bottles and
textile waste, while Evrnu® develops engineered fibers from discarded clothing. Vivify
Textiles specializes in sustainable fabrics made from recycled materials like PET plastic
and textile waste. Additionally, Pure Waste Textiles creates fabrics using 100% recycled
materials sourced from garment factory waste. These companies exemplify the growing
trend toward sustainable practices in the textile industry [584,585].

7. Conclusions and Perspectives

This review has underscored the escalating environmental burden of textile waste,
which is rapidly growing in volume, diversity, and complexity. To address this, a shift
toward more efficient and sustainable end-of-life technologies is essential. In this work
we have explored both existing and emerging methods for textile waste collection, sort-
ing, and recycling, identifying key advancements while highlighting areas that require
further development.
Automated collection systems, powered by smart tags and sensor networks, are emerg-
ing as a game-changer in textile waste management. These systems improve efficiency in
tracking and sorting, yet they require refinement to reduce costs and ensure widespread
adoption. The success of these systems will hinge on enhanced infrastructure, active partic-
ipation from consumers and producers, and supportive policies such as extended producer
responsibility (EPR) legislation.
For sorting, advanced technologies like near-infrared (NIR) and hyperspectral imaging
(HSI) stand at the forefront, enabling precise fiber separation based on chemical composi-
tion. However, challenges remain, particularly with complex or multilayered textiles that
these technologies struggle to analyze. Future development should focus on tackling the
increasing complexity of blended fabrics and integrating hybrid sorting technologies that
combine spectroscopic methods with AI-based detection.
Polymers 2025, 17, 628 70 of 94

Pretreatment is another critical area, especially removing non-textile components,

colorants, and finishing compounds, which interfere with recycling processes. While auto-
mated disassembly technologies are promising, they are still in the early stages and need
significant speed, accuracy, and cost-efficiency improvements to become viable. Similarly,
scalable and cost-effective methods for removing colorants and finishes are urgently needed
to improve the quality of recycled fibers.
Recycling technologies are broadly categorized into mechanical and chemical methods.
Mechanical recycling, while cost-effective and environmentally favorable, is limited by
its inability to maintain fiber quality over repeated cycles, especially for blended fabrics.
Polymer recycling, which involves melting or dissolving waste polymers, offers higher-
quality outputs but is more resource-intensive. Chemical recycling methods like solvolysis
and pyrolysis hold the potential for producing virgin-quality monomers, particularly for
synthetic fibers, while biological recycling shows promise for natural fibers. However,
these methods face significant scalability challenges due to high energy consumption and
operational costs.
Looking ahead, the future of textile recycling depends on the integration of advanced
sorting technologies, scalable pretreatment solutions, and efficient recycling processes. In-
novations such as automated disassembly, engineered enzymes for biolysis, and improved
chemical recycling techniques will be pivotal in closing the material loop. Reducing energy
inputs, optimizing processes, and developing solvent recovery systems will be key to
making chemical recycling more viable on a larger scale.
Beyond technological advancements, collaboration between policymakers, industry
leaders, and researchers is crucial to driving change. Policies that incentivize eco-design
and encourage EPR will be vital, as will industry cooperation to standardize recycling
processes and adopt innovative technologies. Consumer engagement will also play a
central role, both in reducing waste generation and participating in textile recycling efforts.
In conclusion, while significant strides have been made in end-of-life technologies
for textiles, much work remains to overcome the current challenges. By combining ad-
vanced sorting, pretreatment, and recycling technologies with strong policy support and
industry collaboration, the textile sector can move toward a sustainable, closed-loop
future—one that minimizes waste, maximizes material recovery, and significantly reduces
its environmental footprint.

Author Contributions: Writing (review and editing), writing (original draft), conceptualization,
visualization, and data curation, M.S.A.-A.; writing (review and editing), writing (original draft),
conceptualization, visualization, and data curation, B.T.; writing (review and editing), data curation,
and visualization, B.G.; writing (review and editing) and data curation, O.M.; writing (review and
editing) and data curation, Y.W.; writing (review and editing) and data curation, S.R.; writing (review
and editing) and data curation, R.K.; writing (review and editing) and data curation, B.B.; writing
(review and editing) and supervision, K.D.C.; writing (review and editing) and supervision, S.D.M.;
writing (review and editing) and supervision, D.R.D.; project administration, writing (review and
editing), supervision, and funding acquisition, K.M.V.G. All authors have read and agreed to the
published version of the manuscript.

Funding: Kevin M. Van Geem and Dagmar R. D’hooge acknowledge the Vlaio Moonshot program
via the Core2 program. We acknowledge the financial support provided by the C-PlaNeT (Circular
Plastics Network for Training) project from the EU in the framework of the Horizon 2020 research
and innovation program (Marie Skłodowska-Curie Grant Agreement No. 859885) and the European
Research Council Grant OPTIMA (Process Intensification and Innovation in Olefin Production
through Multiscale Analysis and Design) under grant agreement ID 818607. The research also
received funding from the Flemish Research Foundation (FWO), i.e., the project CIRCA G065324N
Polymers 2025, 17, 628 71 of 94

and the European Union under the HO2020-REA action, call H2020-SC5-2018-2, i.e., the project React
ID 820869.

Conflicts of Interest: Author Mehrdad Seifali Abbas-Abadi was employed by Synpet Technology.
The remaining authors declare that the research was conducted in the absence of any commercial or
financial relationships that could be construed as a potential conflict of interest.

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