Environmental Chemistry Letters (2024) 22:1929–1987

https://doi.org/10.1007/s10311-024-01726-2

REVIEW ARTICLE

Textile production by additive manufacturing and textile waste

recycling: a review
Weiqiang Fan1 · Yongzhen Wang1 · Rulin Liu1 · Jing Zou1 · Xiang Yu1 · Yaming Liu1 · Chao Zhi1 · Jiaguang Meng1,2

Received: 6 July 2023 / Accepted: 3 March 2024 / Published online: 5 April 2024
© The Author(s), under exclusive licence to Springer Nature Switzerland AG 2024

Abstract
The rapid growth of textile industry and fast-fashion has led to the production of about 92 million ton of textile waste per
year. Nearly 85% of textile waste is disposed of by landfill and incineration, causing serious environmental pollution and
huge resource waste, calling for alternative textile production. Here we review the green production of textiles with focus on
additive manufacturing, 3- and 4-dimension printing, recycling textile waste, and synthetic and natural fibers. Additive manu-
facturing technologies, particularly 4-dimension printing, is flexible, green, and allows on-demand manufacturing, which
is one solution to the textile waste problem. 4-Dimension printing contributes to the development of intelligent materials,
and can create structures that deform in response to external stimuli. Textile waste contains high-quality, low-cost materials
that can be re-used and recycled. Applications include smart textiles, flexible electronics, soft robotics, human–computer
interaction, and wearable devices.

Keywords 3D printing · 4D printing · Textile materials · Textile waste recycling · Natural fiber · Chemical fiber

Abbreviations DLP Digital light printing

ABS Acrylonitrile butadiene styrene DMSO Dimethyl sulfoxide
Ag-NWs Silver nanowires DND Detonation nanodiamonds
AM Additive manufacturing EBL Electron beam lithography
[AMIM]Cl 1-Allyl-3-methylimidazolium chloride EGaIn Eutectic gallium-indium
[Bmim]OAc 1-Butyl-3-methylimidazolium acetate EMI Electromagnetic interference
[BMIM][Cl] 1-Butyl-3-methylimidazolium chloride EVM-GMA Ethylene vinyl acetate-glycidyl
CAD Computer-aided design methacrylate
CNCs Cellulose nanocrystals FDM Fused deposition molding
CNTs Carbon nanotubes FEA Finite element analysis
DBA Dibutyl adipate GBL ?-Butyrolactone
[DBNH]OAc 1,5-Diazabicyclo[4.3.0]non-5-enium GNP Graphene nanoplates
acetate GO Graphene oxide
DMAc/LiCl  N,N-Dimethylacetamide/Lithium hBN Hexagonal boron nitride
Chloride HEA Hydroxyethyl acrylate
DEs Dielectric elastomers HEMA Hydroxyethyl methacrylate
DEGDMA Di(ethylene glycol) dimethacrylate HPDE High-density polyethylene
DIW Direct ink writing IEM Ethyl isocyanate methacrylate
LCE Liquid crystal elastomers
ML Machine learning
* Yongzhen Wang
[email protected] [MMIM][DMP] 1-Methyl-3-methylimidazolium dime-
thyl phosphate
1
School of Textile Science and Engineering, Xi’an MCC Microcrystalline cellulose
Polytechnic University, Xi’an, Shaanxi, China NaOH Sodium hydroxide.
2
Key Laboratory of Functional Textile Material and Product, NASA National Aeronautics and Space
Ministry of Education, Xi’an Polytechnic University, Xi’an, Administration
Shaanxi, China

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1930 Environmental Chemistry Letters (2024) 22:1929–1987

NIPAM  N-Isopropyl acrylamide physical incinerators (Kerr and Landry 2021; Ecap 2019).
NIPAM  N-Isopropylacrylamide Large quantities of textile waste are improperly disposed of,
NMMO  N-Methylmorpholine-N-oxide polluting environment and posing a huge threat to human
PA Polyamide health (Asmatulu et al. 2022; Foundation 2021; Hamilton
PAA Polyacrylamide and Feit 2019; Nanda et al. 2021). Therefore, effective recy-
PAN Polyacrylonitrile cling and reuse of textile wastes are urgently needed. PET
PAN-VA Poly(acrylonitrile-co-vinylacetate) (polyethylene terephthalate) and cotton account for the larg-
PCL Polycaprolactone est proportion of textile fiber. PET fibers can be recycled
PCLA Poly(e-caprolactone-co- to extract pure monomers for reuse (Abdullah and Ahmad
lactide)-b-poly(ethylene 2013; Chen et al. 2019c; Guo et al. 2021; Liu et al. 2023b;
glycol)-b-poly(e-caprolactone-co-lactide Palme et al. 2017; Siddiqui et al. 2010; Zhang et al. 2022b).
PEG4A 4-Arm polyethylene glycol acrylate Cotton waste is increasingly used in value-added applica-
PCLDA Polycaprolactone diacrylate tions such as yarn, composite fillers, recycled cellulose fib-
PEEK Polyether ether ketone ers, functional materials, and biofuels through mechanical,
PET Polyethylene terephthalate chemical, and biological recycling (De Silva and Byrne
PET-G Polyethylene terephthalate glycol 2017; Ding et al. 2018; Haule et al. 2016; Liu et al. 2019;
PHBV Poly (3-hydroxybutyrate-co-3-hydroxy Lu et al. 2022b; Sun et al. 2021). Closed-loop recycling and
valerate) high value-added applications of textile waste can provide
PLA Polylactic acid a low-cost and high-quality materials source, creating value
PNIPA Poly(N-isopropylacrylamide) and mitigating significant environmental pressures and
PNIPAm Poly (N-isopropylacrylamide) economic costs. However, there is a scarcity of research on
POE-g-MAH Maleic anhydride grafted polyoctene closed-loop recycling of textile waste and its high value-
PP Polypropylene added applications.
PSPMA Potassium 3-sulfopropylmethacrylate Additive manufacturing (AM) technology has high pre-
PVC Polyvinyl chloride cision and customization flexibility, making it a promising
PµSL Projection microstereolithography approach to produce complex and sophisticated structures
PVA Poly (vinyl alcohol) (He et al. 2014; Hung et al. 2014; Mao et al. 2017). The
SDS Sodium dodecyl sulfate maturation of innovative materials design has driven the
SEBS Styrene-ethylene-butylene-styrene advancement of smart materials and the creation of a wide
SLA Stereo lithography appearance range of materials with advanced functions and properties.
SLS Selective laser melting Convergence of additive manufacturing technology and
SMPs Shape memory polymers smart materials gives rise to 4D printing technology (Tibbits
SMPU Shape memory polyurethane 2014). 4D printed structures can respond to external stimuli
TBAH Tetra butyl ammonium hydroxide and make corresponding deformations, with good flexibil-
TEMPO (2,2,6,6-Tetrame-thylpiperidin-1-yl) ity and promising applications in the fields of textiles, flex-
oxidanyl ible electronics, biomedical applications, tissue engineering
TPU Thermoplastic polyurethane materials, bionic structures, and so on (Beecroft 2019; Choi
et al. 2021; Flores Hernandez et al. 2021; Grain 2016; Guo
et al. 2022; Hernandez-Sosa et al. 2022; Kadumudi et al.
Introduction 2021; Le Duigou et al. 2019; Phan et al. 2022; Placone et al.
2017; Sommer et al. 2016; Sydney Gladman et al. (2016; Wu
The production and development of textile industry, often at et al. 2018; Zhang et al. 2019a). New opportunities and ideas
the cost of massive resource consumption and huge environ- for textile waste management and high value-added appli-
mental pollution, is not in line with the goal of sustainability cations are emerging benefiting from advances in additive
(Atugoda et al. 2022; Farhana et al. 2022; Muthu et al. 2012; manufacturing technology and material design.
Orasugh et al. 2018). With population growth and economic In recent years, there has been a growing interest in
development, textile production is constantly on the rise. additive manufacturing, such as 3D and 4D printing, for
In addition, the rise of fast fashion has increased per capita the production of functional textiles. Kumar et al. (2023)
textile consumption and shortened the life of textiles. As a explored the use of additive manufacturing to incorporate
result, the production of textile waste has increased dramati- embroidery elements onto plain fabrics, aiming to enhance
cally. Globally, more than 92 million tons of textile waste the market competitiveness of these fabrics. Manaia et al.
is generated annually, of which less than 20% is recycled (2023) reviewed the progress of 3D and 4D printing tech-
and reused, with the majority disposed of in landfills and nology in textile field and highlighted the utilization of
Environmental Chemistry Letters (2024) 22:1929–1987 1931

advanced computer-aided design techniques to create Based on the current situation of textile waste, advanced
exclusive and customized textiles. Compared to tradi- manufacturing technologies can promote the high-value
tional manufacture, additive manufacturing has advan- application and clean production of textile waste at a tech-
tages of clean production, material conservation, efficient nological level. The rapid development of AM technology,
design and preparation of complex structures, reduction flexible manufacturing methods, and customizable attributes
of production costs and wastage, and customizable and provide a new solution paradigm for the high-value appli-
flexible manufacturing to meet diversified needs (Gor- cation of textile waste. Here, we propose a combined tex-
rasi et al. 2020). Integrating textile waste recycling and tile waste and additive manufacturing strategy (Fig. 1). We
additive manufacturing technology can endow products review recent progress and analyze the advantages, oppor-
with exquisite details and excite creators (Vettese Forster tunities, and challenges, with a particular focus on the latest
2017). Renowned designer Iris van Herpen designed and developments of textile materials in 4D printing. Further-
produced dresses made of recyclable polyester using 3D more, the potential future directions and challenges of the
printing. The dresses have exquisite design details and combined textile waste-additive manufacturing strategy are
complex structures, greatly improving the quality and discussed.
design level of fashion products (Grain 2016). The emer-
gence of additive manufacturing technology has irrigated
new vigor for the design and manufacture of new textiles. Classification and advantages of textile
In addition to structural aspects, functional multi-material materials
printing can give textile waste strong properties and func-
tionality. Carrete et al. (2021) reported that cellulose from Textile materials usually exist in the form of fibers, which
waste denim can be functionalized and blended with recy- are twisted by bunching to form yarns (Hu et al. 2020a;
cled PET (polyethylene terephthalate) to increase the tough- Seguin and Crassous 2022). A variety of yarns could be
ness of printed PET structures. Stolz and Mülhaupt (2020) woven into various textiles by different arrangements or
mixed wastepaper-derived cellulose with PVA (polyvinyl textile processes. Textile fibers usually have a high aspect
alcohol) and printed structures with good dimensional sta- ratio, strong mechanical properties, and flexibility, meeting
bility, high Young’s modulus, and tensile strength. Further the needs of garment, domestic, medical, and many other
treatment endowed the printed structures with heat-humid- various technical fields (Denton and Daniels 2002). Nev-
ity-responsive shape memory properties and improved ertheless, different textile fibers have different properties,
mechanical properties, water resistance, and flame retar- which are closely related to the source, size, morphology,
dancy. Compared to virgin PET materials, recycled PET fiber structure, and aggregation mode, micro spatial con-
offers superior dimensional stability and mechanical prop- formation of polymer (Grishanov 2011). Textile fibers can
erties in additive manufacturing (Exconde et al. 2019; Fer- be divided into natural fibers and chemical fibers (Fig. 1).
rari et al. 2020). Some researchers have extracted and recy- Plant fibers are mainly composed of cellulose, such as cot-
cled materials from wastes, such as PA (polyamide) and PP ton, hemp, and so on (Sfiligoj Smole et al. 2013). Animal
(polypropylene), to improve composite performance through fibers mainly come from animal hair or secretions, such as
physical or chemical methods (Chong et al. 2020; Farina wool, silk, and some animal hair (Ho et al. 2012). Asbestos
et al. 2019; Maldonado-García et al. 2021; Morales et al. fibers are the main mineral fiber. For chemical fibers, syn-
2021; Zander et al. 2019a, b; Zhang et al. 2023a). Le Duigou thetic fibers and regenerated fibers are the most common.
et al. (2021) prepared a metamaterial wet-responsive actua- Furthermore, some metal fibers, carbon fibers, and glass
tor with tunable response rate and deformation curvature fibers are also used widely (Mather et al. 2015). Synthetic
by laminating continuous flax fibers into 4D-printed mate- fibers are mainly polyethylene terephthalate (PET), poly-
rial. The microscale arrangement of continuous flax fibers amide (PA), polyacrylonitrile (PAN), polypropylene (PP),
endowed 4D-printed actuator with controllable deforma- poly (vinyl alcohol) (PVA), polyvinyl chloride (PVC), and
tion. The application of multi-material design allows for the other materials polymerized by macromolecules (Harmsen
incorporation of intelligent properties in most textile materi- et al. 2021). Regenerated fibers are mainly formed by chemi-
als (Fan et al. 2023a). By integrating additive manufacturing, cal treatment of natural materials, for example, regenerated
smart products with complex structures and powerful prop- cellulose fiber and regenerated protein fiber (Chen 2015;
erties can be created. These advancements in technology and Sinclair 2015).
methods have the potential to revolutionize the utilization of Textile materials have mechanical stability, flexibility,
textile waste. In this paper, we hope to provide some inspira- comfort, and other performance advantages that are equally
tion for high value-added reuse of textile waste by summa- fascinating in the AM field. In detail, cellulose, being the
rizing and reviewing the related research and applying them primary constituent of plant fibers, cellulose molecular
in the additive manufacturing field. chains have a large number of reactive groups, and molecular
1932 Environmental Chemistry Letters (2024) 22:1929–1987

Fig. 1  Textile production using textile waste and additive manufactur- permission of Springer Nature, Taylor & Francis, and ACS, from
ing. The production of textile waste has increased significantly due reference (Beecroft 2019; Cera et al. 2021; Sydney Gladman et al.
to the growing population and fast fashion economy. leading to seri- (2016; Hua et al. 2020; Vettese Forster 2017), and an image from
ous pollution and land occupation. Additive manufacturing offers the (Grain 2016)
potential and new insights for textile waste disposal. Reprinted with

chains are linked by hydrogen bonds (Ali et al. 2022a, b). and fiber reinforcements (Deopura and Padaki 2015; Zhang
The entanglement, alignment, and gelation of these chains et al. 2020). Polyacrylonitrile (PAN) fibers have a wool-like
in cellulose solutions or suspensions result in a shear thin- fluffiness, elasticity, and a degree of physicochemical sta-
ning behavior, thereby providing excellent print character- bility, attributed to strong polar acrylonitrile group (Gupta
istics (Wang et al. 2018; Yuan et al. 2022). Additionally, and Afshari 2018). The excellent solvent resistance, homo-
the utilization of plant fibers in fiber-reinforced composites geneous interconnection structure, and high porosity struc-
can effectively enhance both mechanical and biological ture have potential applications in printable encapsulation
properties (Koushki et al. 2020; Xiao et al. 2019; Zaki et al. materials (Kang et al. 2022). Melting the 3D-printed PAN
2021). Common animal fibers including wool and silk, have can turn it into a carbon material with excellent mechanical
good biocompatibility. In the field of AM, they are often and conductive properties (NREL 2016; Usselmann et al.
used for composite reinforcement, medical materials, and 2022). PP fibers have a relatively low density, high melting
porous structures (Choi et al. 2021; Röhl and Müssig 2022; point, strong mechanical properties, thermal stability, and
Sommer et al. 2016). Synthetic fibers occupy a high pro- low cost (Oliveira et al. 2017). Polypropylene (PP) can be
portion of textile fibers. Polyethylene terephthalate (PET) compounded with some compatibilizers, fillers, and other
fiber has good processability and economy, and the supra- components to realize stronger functional or mechanical
molecular force of molecular chains can form a temporary properties. Poly (vinyl alcohol) (PVA) fibers have good
physical cross-linked network to maintain the shape during flexibility, bio-affinity, degradability, and hydrophilicity,
the bonding process layer by layer (Jaffe et al. 2020; Jain making them very promising in bio-scaffolds, drug deliv-
et al. 2021). Polyamide (PA) fiber has high abrasion resist- ery, and complex structures. Polyvinyl chloride (PVC) fibers
ance and strength, but pure PA printing materials are prone are resistant to chemical corrosion and have good thermal
to warpage, distortion, and dimensional instability due to and electrical insulation performance (Hsissou et al. 2021;
stress accumulation during crystallization, which is why they Zhong et al. 2018). Pure PVC is difficult to use in AM due
are often blended with other polymers, inorganic materials, to poor thermal stability and rheology. This can be overcome
Environmental Chemistry Letters (2024) 22:1929–1987 1933

by modification treatment or adding fillers (Calafel et al. spinning speeds and reduced energy consumption have the
2020). Textile materials possess a remarkable amalgamation potential to significantly minimize environmental impact.
of properties, encompassing mechanical properties, biologi- Fabric dyeing and printing processes, along with pre- and
cal properties, cost-effectiveness, abundance in availability, post-treatment, often generate substantial amounts of dyeing
and flexibility. These properties are expected to offer valu- effluent. But the adoption of sustainable wet processes like
able insights into the advancement and synthesis of emerg- supercritical dyeing and water purification technology can
ing advanced materials in the foreseeable future. greatly reduce the generation of polluted water (Chandran
et al. 2023; Kim et al. 2019; Priya et al. 2023). Green tech-
nologies in the production process of the textile industry
Sustainable production and additive have enabled sustainability to be maximized in addition to
manufacturing the limitations of technical and economic conditions. Fig-
ure 2 illustrates the various remediation technologies avail-
Sustainable production technologies able in textile field. The key point for the proper disposal
of textile waste everywhere is the input of advanced green
The textile industry was once considered one of the most technology to enhance the added value of textile waste and
polluting industries in the world (Cao et al. 2023). It expand the application areas of textile waste products. The
involved the use of hazardous chemicals, depletion of unavoidable fact is that all textiles become waste eventually,
energy and petroleum resources, and water resources (Uddin and if not disposed of properly, they can cause serious sec-
2021). Textile industry also generated large quantities of ondary pollution. No single process route can significantly
contaminated water, hazardous emissions, microplastics, increase the recycling rate of multifarious textile wastes.
and solid wastes (Arora et al. 2017; Gjyli et al. 2020; Han
and He 2021; John and Mishra 2023; Kishor et al. 2021; Additive manufacturing
Matta 2010; Matta et al. 2018). Additionally, it required a
significant amount of land for the disposal of textile wastes Additive manufacturing (AM), also known as 3D print-
in landfills and contributed to large carbon emissions from ing, is a technology that allows for the creation of intricate
incineration. Noise pollution was also generated throughout structures by layering materials (He et al. 2014; Hung et al.
the entire process. Sustainable technologies in textile indus- 2014). This technology has revolutionized the traditional
try primarily focus on three aspects: the acquisition of textile manufacturing process of cutting and shaping, enabling
raw materials, textile production, and textile waste recycling. direct material-to-structure manufacturing. It offers several
The sustainability of textile raw materials is achieved by advantages, including simplicity, speed, and high-resolution
incorporating sustainable materials, such as biopolymer and capabilities (Mao et al. 2017; Schubert et al. 2014). Additive
regenerated fiber (Patti and Acierno 2022). On the other manufacturing allows the printing of a wide range of materi-
hand, manufacturing textiles involves using sustainable als, including metals, ceramics, polymers, and multi-mate-
technologies, including producing sustainable yarns, sus- rial composites, for applications in aerospace, medicine,
tainable wet-processing, and sustainable technologies in gar- automotive industry, textile industry, flexible robotics, bio-
ment manufacturing (Nayak et al. 2020; Panda et al. 2021; medical, and so on (Chatterjee and Ghosh 2020; Chen et al.
Utebay et al. 2023). However, the overall sustainability of 2021b; Duda and Raghavan 2016; Gul et al. 2018; Joshi and
the textile industry also depends on how to dispose of large Sheikh 2015; Liaw and Guvendiren 2017; Sarvankar and
quantities of post-consumer textiles effectively. Yewale 2019; Zhou et al. 2020). Moreover, 3D printing sup-
Textile production encompasses various stages including ports customization, and the direct forming of materials can
fiber production, yarn production, fabric production, pre- save raw materials (Peng 2016). Despite the advantages, 3D
treatment processes, fabric printing and dyeing, and post- printing has not been able to replace traditional manufactur-
treatment processes (Islam et al. 2021; Pensupa et al. 2018). ing, because of limitations in materials, structure size, and
For green processes in textiles, efforts have been made to cost (Attaran 2017).
focus on improving sustainability in fiber production, yarn Additive manufacturing starts with a digital model and
production, printing and dyeing, and post-treatment, also employs computer-aided design (CAD) software to trans-
reducing resource consumption, energy consumption, and form the digital model into a solid object. Before the fina-
pollutant emissions. For instance, alternative fibers like lization of 3D solid manufacturing, CAD software is uti-
bamboo fiber, banana fiber, or regenerated cellulose have lized to create a digital model of a predetermined entity.
been introduced in yarn production to decrease the reliance This model is then integrated with slicing software to direct
on cotton (Jawaid et al. 2022). Sustainable practices have the movement of the printer nozzle or platform, regulat-
also been implemented to enhance yarn durability. Addition- ing the deposition of the print head or the application of
ally, advancements in spinning technology such as increased pulsed lasers to solidify the material and finalize the printing
1934 Environmental Chemistry Letters (2024) 22:1929–1987

Fig. 2  Green technologies in the textile industry. Traditional technologies are focused on the textile production process, lacking the correspond-
ing technology to recycle textile waste

process (Chatterjee and Ghosh 2020). The transformation computational analysis methods, such as finite element
from a digital image to an additive manufacturing entity analysis and machine learning, are employed to analyze the
is achieved through the strategic addition of materials in entire design and manufacturing workflow (Gonabadi et al.
a 3D space. During this process, the CAD software sets 2022). These computational methods play an important role
various parameters such as print path, laser intensity, print in the development of additive manufacturing, supporting
temperature, interlayer parameters, and platform movement tasks such as design, process optimization, and field moni-
to regulate the voids, shape accuracy, surface quality, and toring and prediction (Goh et al. 2021). Future advancements
internal structure of the 3D entity. Additionally, computer
Environmental Chemistry Letters (2024) 22:1929–1987 1935

in this field are expected to significantly enhance the reli- 3D-printed structures, 4D-printed structures possess intel-
ability of additive manufacturing entities. ligent properties. These structures are capable of stimulus-
Forms of additive manufacturing can be categorized into responsive deformation through pre-programming, active
three main types: material extrusion, powder bed fusion, deformation, and precise control of the stresses within
and vat photopolymerization (Zhou et al. 2020). Material the structure (Wu et al. 2018). Common active and smart
extrusion includes technologies like fused deposition mold- materials used in 4D printing include shape memory poly-
ing (FDM) or fused filament fabrication (FFF) and direct mers, hydrogels, dielectric elastomers (DEs), liquid crys-
ink writing (DIW) (Daminabo et al. 2020). FDM involves tal elastomers (LCEs), and so on (Champeau et al. 2020;
depositing a thermoplastic filament, which is melted or Dong et al. 2020; Ge et al. 2016; López‐Valdeolivas et al.
semi-liquid, onto a printing platform to create a 3D solid 2018; Roach et al. 2018). 4D printing structures have been
layer-by-layer (Rahim et al. 2019). The most commonly widely used in medical field, biological tissue engineering,
used materials for FDM are thermoplastics or polymers intelligent wearable textiles, and flexible electronics (Bis-
with glass transition temperatures. Despite being the most was et al. 2021; Javaid and Haleem 2019; Kim et al. 2020b;
widely used additive manufacturing technology due to its Kuang et al. 2018; Shakibania et al. 2021; Zolfagharian et al.
low cost and simplicity, FDM has limitations such as poor 2020). The NASA morphing program integrates the study
interlayer adhesion, a narrow range of compatible materials, of smart materials, adaptive structures, microfluidics, bionic
and suboptimal mechanical properties in the vertical print- concepts, optimization, and control. Its research focuses
ing direction (Park et al. 2022). These factors hinder the on developing and evaluating advanced technologies and
widespread adoption and advancement of FDM technology. integrated component concepts to enable efficient, multi-
Direct ink writing is primarily used for printing soft materi- point adaptability of air and space vehicles (Mcgowan et al.
als or hydrogels. This technology requires precise control 2002). This unique characteristic opens up new possibilities
of ink viscoelasticity and shape retention after extrusion for advanced materials and design concepts, expanding the
(Saadi et al. 2022). DIW faces challenges in achieving strong dimensions of innovation.
connections between filaments due to incomplete curing. The research on 4D printing mainly consists of the con-
Although DIW is an important addition to additive manu- struction of theoretical models and the application of printed
facturing, further advancements are needed to overcome its solid models (Deng and Chen 2015; Raviv et al. 2014).
limitations (Champeau et al. 2020). Powder bed fusion tech- Reports between 2013 and 2016 mainly focus on theoreti-
nology mainly utilizes electron or laser beams to sinter or cal investigation analyzing intermolecular interaction, defor-
melt the material, and common techniques include selective mation mechanism, and product optimization. For example,
laser melting (SLS) (Singh et al. 2021b). Selective laser- Tibbits (2014) first demonstrated deformable 3D-printed
melting is a technology that employs a laser to selectively hydrogel triggered by water, attracting attention to 4D print-
melt a targeted area, allowing for layer-by-layer bonding ing. Ge et al. (2013) reasonably described the shape memory
and molding. Primarily used for processing metal powders behavior of anisotropic fibers through the nonlinear contin-
and polymers, this technique offers manufacturing flexibil- uum theory, and complex shapes including twisting, coiling,
ity. However, compared to other technologies, it does pose folding, and spatial curvature changes can be completed.
notable challenges when it comes to multi-material process- Raviv et al. (2014) proposed a “design-fabrication-simula-
ing (Zhou et al. 2020). Photopolymerization, also known as tion” workflow for self-evolving structures. Ge et al. (2014)
stereo lithography appearance (SLA) and digital light print- designed active origami self-assembly of printed active com-
ing (DLP), is a layer-by-layer manufacturing method that posites by controlling the folding angle of the hinge. Mao
utilizes specific light (Kadry et al. 2019). These technologies et al. (2015) fabricated a self-folding structure, predicting
are primarily employed for processing photopolymers, with deformation by finite element simulations. Sydney Gladman
molding being controlled by adjusting the intensity of the et al. (2016) developed a shear-induced cellulose hydrogel
light or the exposure area. They provide several advantages, material, completing the solution of inverse problems with
including high precision, excellent surface quality, and fast complex deformation. Bodaghi et al. (2016) printed a flex-
printing speeds. However, the presence of particles or fibers ible matrix based on two shape memory polymers (SMPs)
may decrease printing effectiveness. with different glass transition temperatures, achieving a self-
The development of novel technologies and materials has expanding/shrinking structure. However, the materials for
paved the way for the promotion of 3D printing (Fig. 3a). 4D printing at this stage are relatively limited, focusing on
One notable example is the emergence of 4D printing (Tib- active materials and heat-responsive shape memory materi-
bits 2014). This technology utilizes additive manufacturing als (Table 1). The main stimuli for smart material deforma-
to create intelligent structures that can deform and undergo tion are humidity or heat. The current researches primarily
functional changes in response to various stimulation, such focus on simple deformation and theory construction, which
as heat, water, electricity, magnetic fields, and light. Unlike provides a solid foundation for the future development of
1936 Environmental Chemistry Letters (2024) 22:1929–1987

Fig. 3  Development timeline of 4D printing. a Publication status of ing, Springer Nature, PNAS, Elsevier and ACS from reference (Tib-
documents on 3D and 4D printing annually, extracted from Febru- bits 2014; Ge et al. 2014; Sydney Gladman et al. (2016; Huang et al.
ary 2024 Scopus database. b The 4D printing studies from 2013 to 2017; López‐Valdeolivas et al. 2018; Boley et al. 2019; Yang et al.
2016 were relatively simple in terms of response modes and driv- 2019; Ambulo et al. 2020; Zhao et al. 2021; Cui et al. 2022; Peng
ing processes. Starting from 2017, related studies have expanded et al. 2022; Deng et al. 2023; Xu et al. 2023); Reprinted from refer-
the range of materials, application functions, and application areas. ence (Mao et al. 2015; Bodaghi et al. 2016; Ge et al. 2016b; Ding
Recently, the world’s smallest 4D-printed heart and ejection device et al. 2017; Liu et al. 2018; Nishiguchi et al. 2020; Wang et al. 2024)
has been reported. Reprinted with permission of Wiley, IOP Publish- with open access creative commons CCBY license

4D printing. In this period, a relatively complete theoretical 2014; Sydney Gladman et al. 2016). However, the functions
analysis of the design-fabrication-deformation process or and applications of 4D printed materials are limited, still
structure prediction has been covered (Bodaghi et al. 2016; with challenges in fabricating high-precision and micro- and
Deng and Chen 2015; Ge et al. 2014, 2016; Raviv et al. nanoscale 4D printed devices (Fig. 3b). The integration of
Table 1  4D printing, including material components, printing technique, response material, and demonstrated applications
Material components Printing technique Stimulus responsive compo- Stimulus Proposed application Ref
nents

Hydrophilic polymer Fused depositionmolding Hydrophilic polymer Water Shipping and manufacturing Tibbits (2014)
(FDM) sectors
Shape memory polymer fib- FDM and ultraviolet photopo- Shape memory polymer Temperature Self-folding and opening box Ge et al. (2013)
ers + elastomeric matrix lymerization
Water-expandable and rigid FDM Expanding material Water _ Raviv et al. (2014)
materials
Printed active composites Multi-jet FDM printers and Mismatched strains between Temperature Self-assembling box and pyra- Ge et al. (2014)
(PAC) ultraviolet light polymeriza- layers of PAC laminates mid and origami airplanes
tion
Polystyrene film and cured Assembled additive manufac- Pre-strained polystyrene film Temperature Self-folding structures Deng and Chen (2015)
resin turing
Environmental Chemistry Letters (2024) 22:1929–1987

A rigid plastic and a rubbery FDM and ultraviolet photopo- Thermal response shape Temperature Packaging of solar cells and Mao et al. (2015)
material lymerization memory effect in compos- space structures, deployable
ites biomedical devices, and
self-assembling robots and
airbags
A family of photo-curable High resolution projection Shape memory effect of Temperature Biomedical devices deploy- Ge et al. (2016b)
methacrylate based copoly- microstereolithography methacrylates able aerospace structures,
mer networks, di(ethylene (PμSL) shopping bags, and shape
glycol) dimethacrylate changing photovoltaic solar
(DEGDMA) as crosslinkers cells
Clay, N,N-dimethylacrylamide Direct inkwriting (DIW) Cellulose fibrils Water Tissue engineering, biomedi- Sydney Gladman et al. (2016)
or N-isopropylacrylamide, cal devices, soft robotics and
cellulose fibrils, photoini- beyond
tiator, enzyme/glucose and
deionized water
Shape memory polymers fiber Ink jet light curing Shape memory polymers Temperature Meta-material lattice and Bodaghi et al. (2016)
and flexible beams with dif- tubular grippers and stents
ferent arrangements with both self-expanding
and self-shrinking features
Composite consisting of a Ink jet light curing Shape memory polymers Temperature Medical technology, aero- Ding et al. (2017)
glassy shape memory poly- space, and consumer product
mer and an elastomer
Hydroxyethyl acrylate (HEA), Digital printing process, Hydrophilic swelling of com- Water Multilayer structures Huang et al. (2017)
hydrox yethyl methacrylate posite hydrogels
(HEMA), potassium
3-sulfopropylmethacrylate
(PSPMA), and polycaprol-
actone diacrylate (PCLDA),
irgacure 819 as photoinitia-
tor
1937
Table 1  (continued)
1938

Material components Printing technique Stimulus responsive compo- Stimulus Proposed application Ref
nents

Liquid crystalline elastomer DIW Thermal response of LCE (Includes Joule heat from A box able to reversibly open Roach et al. (2018)
ink, soft elastomer resin, and active hinge reversible electrical conductivity) and close, a soft robotic
glassy polymer resin bending gripper used for pick and
place, and a hand
Liquid crystalline elastomer DIW and ultraviolet curing Thermal response of LCE Temperature Polarization monitoring, López‐Valdeolivas et al. (2018)
(LCE) and irgacure 369 as active hinge reversible polarimetry, or temperature-
photoinitiator bending steered light transmission
devices
Elastomeric DIW Structural design and pro- Temperature Autonomous morphing struc- Liu et al. (2018)
poly(dimethylsiloxane) gramming of preset strains tures, aerospace propulsion
matrix nanocomposites components, space explora-
tion, electronic devices, and
high-temperature microelec-
tromechanical systems
Poly(dimethylsiloxane) DIW Mismatched thermal expan- Temperature Tunable antennae, dynamic Boley et al. (2019)
matrix, an elastomeric ther- sion of double-layer ribs optics, soft robotics, and
moset and glass fibers deployable systems
Polyurethane hydrogels and FDM Water-absorbing and swelling Temperature Tessellated waterbomb ori- Baker et al. (2019)
polyurethane elastomers properties of polyurethane gami pattern
hydrogels
Silver nanowires (Ag-NWs) FDM Electrically controlled local- Temperature and electricity Robots, temperature sensors, Shao et al. (2020)
and poly lactic acid (PLA) ized temperature deforma- biomedicine, folded wings
tion of composite materials of deformable aircraft
Poly (N-isopropylacrylamide) Multiphoton lithography Light-responsive soft material Light-induced braking An adaptive micro-opto- Nishiguchi et al. (2020)
(PNIPAm) (MPL) mechanical system for a
tunable switching system, a
microfluidic device to mix,
sort, and circulate fluids,
an artificial muscle, and a
micro-swimmer
Liquid crystal elastomer DLP Liquid metal photothermal Light, heat, and electricity Artificial muscle Ambulo et al. (2020)
matrix and dispersed low response switch, LCE ther-
eutectic gallium-indium mal response deformation
(EGaIn) droplet composites
An asymmetric bilayer DIW Double-layer mismatched Temperature/water Automated robotics, and Zhao et al. (2021)
poly(N-isopropylacryla- construction responds to smart biomedical devices
mide)/polyacrylamide heat and moisture-induced
(PNIPA/PAA) structure deformation
Liquid crystal elastomer DIW _ Temperature Soft robotics, smart structures, Peng et al. (2022)
active metamaterials, and
smart wearable devices
Environmental Chemistry Letters (2024) 22:1929–1987
 Environmental Chemistry Letters (2024) 22:1929–1987 1939

customizable 3D printing technology with smart materials

deformation methods, functional properties of materials, and applications. Moreover, 4D printing technology is witnessing a trend of multidisciplinary integration and development, leading to
the emergence of numerous new technologies, theories, and innovative applications that further accelerate its progress. However, it is important to note that 4D printing is still in its early stages
Since the concept of 4D printing was proposed, the technology has continued to evolve, expanding in various aspects such as theoretical research, preparation techniques, stimulus-responsive
achieved milestone progress, promoting the development of
4D printing.

Wang et al. (2023a, b)

Since 2017, 4D printing has been expanded in depth

Deng et al. (2023)

and dimension, making excellent improvements on the
Cui et al. (2022)

Li et al. (2023)
application deficiencies faced by traditional 4D printing
(Fig. 3b). In 2017, Ding et al. (2017) provided a signifi-
cant simplification in the design of high-resolution 3D pro-
Ref

grammable multi-material structures. Huang et al. (2017)

ing and garbage cleaning at reported a material and method that can address the slow

Remotely responsive human-

production of 4D printed multilayer structures, using digi-
Aerospace satellite launch-
Biomedicine, bionic struc-
robotics, and electronics
Biomedical applications,

tal light brief exposures to achieve ultra-fast printing of

tures, and soft robotics

hydrogel and SMPs. Liu et al. (2018) developed a layered

Proposed application

elastomer-derived ceramic, to achieve structures with excel-

space stations

lent mechanical properties in addition to high resolution.

oid robot

This research makes an important advancement in the high

precision and intelligence of 4D structures. In the same
year, research related to liquid crystal elastomers (LCEs)
4D printing was beginning to emerge (López‐Valdeolivas
light, humidity, or electric-

Temperature and near-infra-

External force, temperature,

et al. 2018; Roach et al. 2018). Boley et al. (2019) solved

the problem of simple deformation of thin structural sheets
Temperature or laser

by precisely controlling the coefficient of thermal expansion

and elastic modulus of a composite structure. After 2020,
4D printing has moved toward the integration of multidis-
Temperature

of development, and there is a need for future research to explore pioneering and revolutionary advancements
red light

ciplinary technologies. Sun et al. (2022) obtained datasets

Stimulus

for predicting deformation outcomes by building machine-

ity

learning models of recurrent neural networks, and finite

element simulations. Zhao et al. (2021) designed a bionic
memory effect in polymers
Stimulus responsive compo-

NIPAM has a reversible low

Glass transition temperature

memory effect in compos-

critical solvation tempera-

breathing hydrogel actuator with unpaired bilayer structure,

softening of composites

Thermal response shape

Thermal response shape

realizing reversible shape change and oxygen-evolving. Cui

ture phase transition

et al. (2022) introduced dynamic thiocarbamate bonds in

methacrylate, giving the material excellent self-healing and
self-repairing properties. In the same year, Peng et al. (2022)
combined digital light processing techniques with direct ink
nents

ites

writing to form 3D spatial liquid crystal elastomers lattice

soft actuators with tunable stability. Recently, research on
4D printing growth and de-growth of reversible seeds, bio-
FDM and near-infrared light

mimetic 4D printing catapult, and 4D printing intelligent

Femtosecond laser direct

micromachines have been reported (Fig. 3b) (Deng et al.

2023; Li et al. 2023; Xu et al. 2023). The processing size and
Printing technique

fast response at micro- and nano-scale have become possible

(Hu et al. 2020c; Nishiguchi et al. 2020), and advantageous
writing

4D printed structures continue to be discovered (Ambulo

FDM
DLP

et al. 2020; Cui et al. 2022; Liu et al. 2021a; Shao et al.
2020; Wang et al. 2023b). In Fig. 3a, the number of reports
contain dynamic oxime-car-
bamate bonds and hydrogen
containing electrically con-

on innovative 4D printing research is steadily increasing,

Multi-material composite

and innovative applications of 4D printing research will be

N-isopropylacrylamide
Carbon nanotube-doped

Polyurethane polymers
(NIPAM) composite

carried out in many areas in the future.

Material components
Table 1  (continued)

ductive materials

4D printing has seen significant advancements in recent

Polythiourethane

years (Table 1). These advancements include the expansion

of 4D materials such as hydrogel, liquid crystal elastomer,
bonds

liquid metal, and ceramics. Each material has unique advan-

tages that cater to a wider range of practical applications.
1940 Environmental Chemistry Letters (2024) 22:1929–1987

Unlike previous 4D materials, the new 4D materials can the favorable biological properties of cellulose, it holds great
respond to multiple factors simultaneously. Moreover, the potential for applications in biomedical materials, hydrogels,
processing dimension of 4D printing has been expanded, and composites (Fig. 4c3–c5). Cellulose plays a crucial role
allowing for the manufacturing of high-precision, micro- in the advancement of high-performance, degradable, and
nano-scale devices. This is particularly valuable in scenar- cost-effective advanced materials.
ios that require high precision. These technologies enable The lightweight and robust nature of the all-cellulose
diverse programming and complex deformations beyond printed structure is attributed to the anisotropic arrangement
simple bending, stretching, or shape reversion. The applica- of cellulose molecules. Additionally, this printed structure
tion of 4D printing is continuously advancing in biomedi- exhibits the unique property of transitioning between rigidity
cine, textiles, flexible electronics, bionic devices, aerospace, and flexibility in wet and dry conditions. The all-cellulose
and other fields. In the future, 4D printing technology will printed honeycomb structure holds great potential for vari-
continue to be driven and meet the specific needs of various ous applications in the field of thermal insulation materials
industries. The rapid and advanced development of additive (Fig. 4d) (Jiang et al. 2021a). The cotton cellulose-ionic liq-
manufacturing, with its manufacturing flexibility, a wide uid solution can be used to prepare antifreeze hydrogels with
range of applications, and environmentally sustainable pro- good frost resistance, electrical conductivity, and thermal
duction characteristics, also presents new opportunities for reversibility (Zhang et al. 2019b). By adjusting the orderly
the treatment of textile waste. arrangement of cellulose nanocrystals (CNCs), Li et al.
(2021a) used cellulose-based inks to print patterns that are
transparent under natural light, rainbow-colored under polar-
Textile materials in additive manufacturing ized light, and have anti-counterfeiting functions (Fig. 4e).
Molecular chains of cellulose are intertwined with each
Textile materials are an important part of the additive manu- other, causing blocking and worsening printing conditions
facturing material system and play a pivotal role in practi- when cellulose microfiber concentration is too high. Cel-
cal applications. Natural fibers can be used in engineering lulose inks with self-supporting networks can be prepared
materials, tissue engineering, and bio-scaffolds owing to by optimizing the content of dissolved cellulose and cel-
their good mechanical properties, anisotropic orientation, lulose microfibers. And the high-resolution structure was
bio-affinity, and biodegradability. Meantime, natural fibers printed by further optimizing the process (Fig. 4f) (Yuan
can be used as high-quality fillers to reinforce composites. et al. 2022). By incorporating microcrystalline cellulose
Synthetic fibers are mainly used by various processes or (MCC) into alginate, a hydrogel scaffold with excellent
compounding for additive manufacturing. In this part, we mechanical and printable characteristics can be printed.
present a comprehensive summary of the current status, Moreover, this preparation does not include any substances
methods, and prospects for the application of natural and that could be detrimental to cell growth (Hernandez-Sosa
synthetic fibers in 3D and 4D printing. et al. 2022). Amphiphilic copolymer incorporated into cel-
lulose nanocrystal hydrogel can give it printing performance.
Natural fiber in additive manufacturing The synergistic effect of internal hydrogen bonds and drugs
can control drug release for breast cancer treatment. The
3D printing field 3D-printed hydrogel exhibited controllable biodegradation
(Fig. 4g) (Phan et al. 2022). 3D printing has a natural advan-
Plant fiber: Plant fibers are widely used due to their wide tage in the medical field due to its customizability combined
range of sources and excellent properties, and their main with good bio-affinity of cellulose. Guo et al. (2022) utilized
component is cellulose (Fig. 4a). Trees, cotton and bacte- epichlorohydrin to pre-cross-link cellulose. This process
rial cellulose are the main sources of cellulose, which is resulted in the formation of printable cellulose materials
developed as a 3D printing material through solubiliza- with remarkable mechanical properties, attributed to the
tion and decomposition pre-processing (Fig. 4b). Cellulose presence of loose chemical cross-linking sites and hydro-
molecules consist of a distributed chain of reactive groups, gen bonding between cellulose molecules. The researchers
with numerous hydrogen bonding connections between the successfully employed a printed bilayer cellulose scaffold
chains (Fig. 4b). This unique molecular structure gives cel- for repairing osteochondral defects. Furthermore, implanting
lulose strong material compatibility properties and func- the scaffold into a rabbit femur for 8 weeks demonstrated its
tional editing capabilities. Cellulose-based inks can achieve effective osteochondral repair properties (Fig. 4h). Above
an anisotropic arrangement by adjusting the microscopic cellulose, 3D printing examples are manufactured by DIW
size, viscosity, and shear induction of the ink (Fig. 4c1). (Guo et al. 2022; Hernandez-Sosa et al. 2022; Jiang et al.
The printed cellulose structure is freeze-dried, resulting in a 2021a; Li et al. 2021a; Phan et al. 2022; Yuan et al. 2022;
three-dimensional network pore structure (Fig. 4c2). Due to Zhang et al. 2019b).
Environmental Chemistry Letters (2024) 22:1929–1987 1941

Fig. 4  The 3D printing process of cellulose and its applications. permission of Elsevier from the reference (Jiang et al. 2021a), c2
This figure outlines the main sources of cellulose (a), the prepara- reprinted from the reference (Hu et al. 2020b) with open access crea-
tion process of raw materials for 3D printing (b), the various forms tive commons CCBY license, c3 reprinted with permission of Else-
of application of cellulose materials (c), and their practical applica- vier from the reference (Yuan et al. 2022). The figure also delves into
tions (d–h). Cellulose, sourced from a variety of origins, possesses the relevant applications of 3D-printed cellulose structures, as shown
unique molecular hydrogen bonding connections that naturally lend in (d–h). d Reprinted with permission of Elsevier from the reference
themselves to create materials with robust mechanical properties (c1), (Jiang et al. 2021a). e Reprinted with permission of RSC from the
a three-dimensional network structure (c2), and biomaterial applica- reference (Li et al. 2021a). f Reprinted with permission of Elsevier
tions (c3). Moreover, the distribution of cellulose molecular chains from the reference (Yuan et al. 2022). g Reprinted with permission of
containing numerous reactive groups plays a crucial role in the devel- ACS from the reference (Phan et al. 2022). h Reprinted with permis-
opment of composites (c4), and hydrogels (c5). c1 Reprinted with sion of ACS from the reference (Guo et al. 2022)

Cellulose can also be printed using fused deposition mod- and the resulting viscous cellulose solution was extruded
eling (FDM) methods. It was dissolved in dimethyl sulfox- using an FDM 3D printer. The air-cured structures were
ide (DMSO) and tetra butyl ammonium hydroxide (TBAH), then subjected to solvent exchange in deionized water and
1942 Environmental Chemistry Letters (2024) 22:1929–1987

treated with a cross-linking agent to enhance their mechani- affinity, mechanical properties, and controlled rheological
cal properties, including a compressive strength of 96 kPa properties (Brodin et al. 2022; Ranjit et al. 2022). Keratin
and a swelling property of 28 g/g. The macroscopic and can give composites excellent biocompatible properties,
microscopic images of the 3D-printed cellulose scaffolds, such as PLA/keratin and PCL/keratin composites (Fig. 5a).
showcase the porous structure that facilitates water storage PLA can be enhanced by NaOH-modified keratin. Unmodi-
(Hu et al. 2020b). Cellulose can be blended with the polymer fied keratin increased the thermal conductivity of the PLA
matrix to enhance interface binding and improve printing composites by 155%, and cell adhesion and proliferation
characteristics. The high performance, functionality, and experiments on the composites showed improved cell growth
bio-affinity of cellulose-based 3D printed structures have (Flores Hernandez et al. 2021). Choi et al. (2021) developed
been demonstrated to have potential for future applications a new skin substitute using human hair keratin to promote
in advanced materials manufacturing. Therefore, cellulosic the growth of human dermis and epidermis. The research-
materials were previously regarded as a promising alterna- ers implanted these scaffolds in mice and observed that the
tive to petroleum-based materials (Li et al. 2021b). scars in the PCL/keratin group healed more quickly and
Hemp fibers were mainly used to reinforce composites effectively, resulting in a smoother surface compared to the
in the additive manufacturing field. It was reported that pure PCL scaffolds. This process provides a possibility for
preloading the printed structure and adding flax fiber can repairing defects in skin dermis and epidermis. Placone et al.
significantly improve the tensile strength and stiffness of (2017) fabricated a 3D-printed keratin scaffold derived from
polylactic acid (PLA) (Hinchcliffe et al. 2016). Continuous human hair, prepared a photosensitized solution containing
bleached textile flax yarn/PA6 composites with strong tensile an initiator-catalyst-inhibitor, and then UV-lithographed it.
properties can be printed through the production of molten This keratin hydrogel has high-resolution (Fig. 5b1), com-
silk (Terekhina et al. 2022). Mirzaee and Kim (2022) used pressible, and dynamic mechanical properties. The hydro-
printed graphene as a conductive component to produce a gel exhibits excellent biophilicity and has a porous structure
fully 3D-printed antenna made of biofila and flax filaments, with multiple honeycombs (Fig. 5b2). The cell culture ability
which exhibited excellent electromagnetic and degradation of the printed keratin hydrogel was evaluated by cytotoxicity
characteristics. The printing filament prepared by graft- analysis and medium uptake capacity (Fig. 5b3), indicating
ing fluorescent groups with pH perception onto selectively that the hydrogel is well suited for cell culture, beneficial
milled flax scraps can obtain higher open porosity for fluid for cell growth and migration, drug or growth factor deliv-
penetration with pH sensors through 3D printing technology ery. Based on this hydrogel, a 3D-printed hydrogel scaffold
(Mayer Laigle et al. 2021). for treating burns has been reported. The keratin scaffold
Based on its mechanical, rheological, optical, and thermal can promote effective healing of complex burn wounds
stability properties, cellulose has a wide range of applica- by absorbing and releasing a collagen synthesis inhibi-
tions in 3D printing. Adjusting the concentration of cellu- tor (Navarro et al. 2020). Wool keratin reacted with ethyl
lose, adding fillers, and optimizing process conditions are all isocyanate methacrylate (IEM) to obtain keratin gel with
effective measures for improving the printing properties of photolithographic properties (Fig. 5c). The printable keratin
cellulose-based inks. Anisotropic alignment by shear induc- patterns have micron-level high resolution. Such hydrogels
tion, which significantly improves mechanical properties, are potentially valuable in tissue engineering, bioassays, and
has been successfully achieved in some 3D printing studies. drug delivery (Zeng et al. 2020). In flexible sensors field, a
Cellulose, primarily derived from plants, offers excellent humidity sensor prepared by dispersing moisture-sensitive
properties without increasing cytotoxicity and holds great materials onto a wool keratin porous substrate and printing
potential in the production of biomedical materials (Pan- on a silk fibroin matrix can be used for respiratory detec-
dey 2021). By subjecting cellulose to various modification tion (Ma et al. 2021). Keratin applications are focused on
processes, its material functionality and properties can be biomass composites, tissue engineering, flexible sensing
tailored. Moreover, cellulose serves as a high-quality filler devices, and biomedicine.
that enhances bonding and improves the performance of Silk’s main ingredient is silk fibroin (SF) composed of
composite materials. Additionally, cellulose is widely avail- amino acids, supporting various cross-linking mechanisms,
able and renewable, making it an attractive alternative to mainly used in tissue engineering, flexible electronics, bio-
petroleum-based polymers due to its easy availability, low materials, and so on (Lu et al. 2022a; Mu et al. 2020). In
cost, degradability, and environmental benefits. In conclu- flexible electronics field, the incorporation of functional fill-
sion, cellulose plays a strategic role and holds significant ers into silk proteins can give special functions to printed
application value in advancing the development of green structures. Zhang et al. (2019a) used carbon nanotubes as the
advanced materials. conductive core and SF as the outer edge sheath (Fig. 5d1).
Animal fiber: Wool has a high purity of keratin content. This core-sheathed fiber was directly printed using a special
Keratin is widely used in biomaterials field due to its good print nozzle and applied to friction nanogenerator textile
Environmental Chemistry Letters (2024) 22:1929–1987 1943

Fig. 5  Application areas and preparation processes for 3D-printed ing the important role of 3D printing technology in advancing the
animal fibers are diverse and promising. Animal fibers, known for diverse application areas of customizable biomedical devices, tissue
their excellent properties and biocompatibility, are being developed engineering scaffolds, and flexible electronics. b Reprinted with per-
as advanced materials in various fields. These fibers, derived from mission of Springer Nature from the reference (Placone et al. 2017).
animal hair and insect secretions, are utilized in the development d Reprinted with permission of Elsevier from the reference (Zhang
of biopolymers (a), tissue-engineered scaffolds (b), protein micro- et al. 2019a). e Reprinted with permission of Wiley from the refer-
structures (c), flexible electronics (d), human–computer interaction ence (Kadumudi et al. 2021). f Reprinted from the reference (Qin
devices (e), and nanorobotics (f) (Scale bar, 20um). The figure offers et al. 2021) with open access creative commons CCBY license
the common application mechanisms of animal fibers, highlight-

with circuit arrangement. The textile could harvest biome- material can be applied in gloves for gesture recognition and
chanical energy from body movement and achieve a power translation (Fig. 5e2), demonstrating promising applications
density of up to 18 mW/m2 (Fig. 5d2). Silk fibroin and in human–computer interaction, flexible electronics, and so
reduced graphene oxide can form bio-material. The presence on (Kadumudi et al. 2021). The material properties and
of sacrificial and hierarchical hydrogen bonds gave the mate- multi-material compatibility characteristics of SF provide
rial a strong mechanical toughness, self-healing properties a viable solution for the development of flexible electronics.
and electrical conductivity. The composite supports variety Apart from flexible electronics, SF’s 3D structures are
of production methods, such as 3D printing (Fig. 5e1). This most commonly used in the biomedical field. Fibrous cells
1944 Environmental Chemistry Letters (2024) 22:1929–1987

can be embedded in the mixture of SF and 4-arm polyethyl- The multi-size morphology and material distribution of spi-
ene glycol acrylate (PEG4A), the surface of mixture was cul- der silk layers can be controlled by adjustable high-energy
tured to form keratinocytes. The resulting hydrogel bio-ink electrons. The laminar structure of radial lines and spiral
has good printing characteristics under digital visible light. lines gives rise to different functions of selective adhesion.
The printed objects were induced at an air–liquid interface The original molecules of this structure can be precisely
to produce a keratin layer for artificial skin. SF provided modified and then cultured, allowing cells to adhere and
elasticity to the artificial skin, forming a thicker keratin layer grow in a bilayer structure. 3D EBL provided support for
compared to pure PEG4A (Kwak et al. 2019). Sangkert et al. the functionalization and activation of other fillers to design
(2021) prepared a 3D-printed bio-scaffold resembling a bone biological dye-driven nanofishes (Fig. 5f2). Nanofishes can
extracellular matrix by combining alginate, polyvinyl alco- be activated by near-infrared and triggered by temperature
hol, SF, and cultured bone cells on the bio-scaffold. The and pH for controllable payload release and device lifetime.
scaffold with SF formed a porous cross-section structure 3D electron EBL of spider silk offers new approaches in the
and lower swelling property, thus being conducive to cell fields of nanorobotics, bionics, molecular devices, and so on.
adhesion and proliferation. SF solutions can be compat- Incorporating additive manufacturing technology in nat-
ible with nanoparticles, drugs, enzymes, and antibodies to ural fibers can derive a variety of advanced applications,
provide different functions. Tao et al. (2015) developed a as shown in Fig. 6. Cellulose exhibits favorable printing
customized inkjet print library based on a SF solution for- properties due to its gel-like characteristics and anisotropic
mulation. The ink was printed using a piezoelectric inkjet arrangement. Direct ink writing printing (DIW) is a com-
process to control ink deposition. The printed sensors can monly used technique for cellulose printing. The printing
change color from blue to red at a bacterial concentration conditions can be adjusted by controlling the viscosity. How-
of approximately 1­ 02 CFU m ­ L−1. The process eliminates ever, cellulose-based ink often encounters challenges such
the destruction of high-temperature extrusion on biological as low interlayer adhesion and poor mechanical properties.
compounds. Silk polymorphism and other fillers allow the Nevertheless, these issues are gradually being addressed and
customizable additional functions, micro or nano-scale, and improved as the innovative materials design process matures
specific pore structures, combining with different processes. and evolves. Cellulose can also be printed by FDM, usu-
Aqueous 3D microprinting solution containing regenerated ally incorporated into polymers with a glass transition tem-
silk fibroin and immunoglobulin can use multiphoton lithog- perature, as a high-performance organic filler to improve
raphy technology to print structures with good shape fidelity mechanical properties, thermal stability, extrusion, biocom-
and biological functional properties (Dickerson et al. 2017). patibility, and biodegradability. Cellulose composites can be
Organic particles with different particle sizes can be used modified by adding functional fillers and making chemical
as sacrificial materials to form nano-porous structures with modifications, allowing for easy customization of function-
specific morphology, and open porosity can be achieved by ality and properties. Moreover, cellulose can be obtained
ultrasonic treatment. 3D-printed silk protein porous struc- from various sources such as plants, trees, and cotton, which
tures have highly viable applications in insulation materi- makes it both cost-effective and environmentally sustainable.
als and tissue engineering (Sommer et al. 2016). In short, Recent research has focused on the application of cellulose
SF brings together a host of excellent properties such as in advanced areas like hydrogel printing, optical applica-
mechanical properties, flexibility, multi-material compatibil- tions, biomaterials, solar steam collection, small-scale
ity and biological properties. It plays an important role in the energy absorption devices, sensors, and human–computer
fields of textiles, tissue engineering, flexible electronics, and interaction (Balcerowski et al. 2023; Groetsch et al. 2023;
functional materials. Guo et al. 2023; Maity et al. 2023; Zhu et al. 2023).
Spider silk is a strong natural material with super tough- The excellent biocompatibility of animal fibers makes
ness and adhesion, used in military body armor and special them highly attractive in biomaterial research. This allows
protective shields. Qin et al. (2021) fabricated 3D structures animal fibers to be used in wound healing, bone tissue
with nanoscale shape fidelity using a developed electron repair, artificial skin, and in combination with advanced
beam lithography (EBL) technique. Spider silk proteins AM technology to meet the specific customization needs
obtained by genetic recombination can be used as a resist of patients (Fig. 6). The incorporation of photoinitiators,
with excellent mechanical strength and structural complex- catalysts, and cross-linking agents into keratin or silk pro-
ity. Figure 5f1 shows the natural spinning process of spider teins enables the development of lithography inks, which
silk, and the crystallization of spider silk protein nanofibers presents a valuable approach for printing high-precision,
formed during electron spinning is highly dependent on the micro- and nanoscale devices. The utilization of animal
writing direction. Furthermore, it offered greater advantages fibers in the fabrication of hydrogels or composites is
than silk for achieving nanoscale high-precision patterns due attributed to their favorable biological properties and the
to the well-defined molecular weight of artificial spider silk. creation of porous structures that promote cell adhesion
Environmental Chemistry Letters (2024) 22:1929–1987 1945

Fig. 6  Molecular structure of the main components of natural fib- interaction devices. The utilization of 3D-printed animal fibers pri-
ers, the main forms in which natural fibers exist, and the application marily focuses on biomaterial development, including artificial skin,
areas of natural fibers. Cellulosic materials offer various advantages bone repair, wound healing, functional fibers, hydrogels, flexible sen-
in creating structures such as anisotropic structures, hydrogels, porous sors, fluorescent materials, and porous materials conducive to cell
structures, and structural colors. Furthermore, 3D-printed cellulose- growth. It is evident that the potential applications of natural fibers
based composites show promise in applications related to fresh water are yet to be fully realized, and future emphasis will be placed on
harvesting, friction generators, flexible sensors, and human–computer innovative applications involving animal fibers

and proliferation. Moreover, the addition of functional fill- innovative application techniques, and the development of
ers like carbon nanotubes and reduced graphene oxide into advanced materials. In conclusion, natural fibers hold sig-
animal fibers can enhance mechanical properties while nificant research potential and value, playing a crucial role
introducing desirable characteristics such as self-healing in promoting the development of new materials.
or electrical conductivity. There is enormous potential
for expansion in flexible electronics, human–computer 4D printing
interaction, and functional textiles based on animal fib-
ers. Table 2 shows the different types of printed natural Cellulose and animal proteins possess the inherent ability
fiber, printing formulations, printing techniques, related to sense deformations caused by environmental factors.
mechanisms, functions, and applications. Animal fiber is As material design technology continues to advance and
also a widely used functional filler, mainly in polymers, manufacturing techniques become more sophisticated, the
to improve mechanical properties, thermal properties, and utilization of these ingredients in the field of smart materi-
biocompatibility. als is gaining prominence. The distinctive material advan-
Natural fibers offer a renewable and versatile source of tages offered by cellulose and animal protein, such as their
materials that exhibit exceptional performance and compat- mechanical properties, biocompatibility, and material com-
ibility for the advancement of advanced materials. However, patibility, contribute to the exceptional performance and
current researches indicate that the full potential of natural innovative applications of 4D printing. This section aims
fiber materials is yet to be fully explored. In the future, there to review the research progress, current status, and future
will be further advancements in incorporating natural fibers development trends of natural fibers in the realm of 4D
into engineering materials, biomaterials, textile materials, printing.
and flexible electronic devices. This will involve advance- Plant fiber: Cellulose has the potential to be developed
ments in natural fiber extraction and recycling technology, as a 4D-printed smart material due to its ability to absorb
Table 2  Natural fiber printing formulations, printing techniques, related mechanisms, functions, and applications
1946

Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Cellulose Filter paper is dissolved and Direct ink writing (DIW) _ 16.6 MPa compressive Biomedical, environmental, Jiang et al. (2021a, b)
dispersed in NaOH/urea Young’s modulus and heat and structural engineering
insulation areas
Cellulose, ­ZnCl2, ­CaCl2 and _ Metal cations form revers- Hydrogels have good Low-temperature flexible Zhang et al. (2019a, b, c)
glycerol ible ionic coordination stretch, toughness, flex- equipment
bonds with hydroxyl ibility, and electrical
groups on the cellulose conductivity at − 70 °C
molecular chain
Ink formulated with cellulose DIW DC 5700 is grafted by a Bright iridescent colors in Preparation of optical anti- Li et al. (2021a)
nanocrystals continuously hydroxyl condensation polarized light counterfeiting patterns
modified with organosilane coupling reaction with
and polyoxyethylene ether electrostatic interaction
between polyoxyethylene
ether and cellulose
Pulp-based cellulose dissolved DIW _ Excellent thixotropy and Biomedical, decorative, Yuan et al. (2022)
in NaOH/urea with different instantaneous self-support energy-related products
crosslinkers ability
Alginate and microcrystalline DIW CaCl2 as a cross-linking Cell adhesion and bioactiv- Bone tissue Hernandez-Sosa et al. (2022)
cellulose agent ity
Cellulose soluble in LiOH/ DIW Epichlorohydrin as a cross- Possesses cartilage repair Personalized tissue engi- Guo et al. (2022)
urea, bioactive glasses linking agent properties neering scaffolds
Cellulose nanocrystal and DIW CNC physically enhanced Controlled release of drugs Stimuli-responsive Phan et al. (2022)
poly(ε-caprolactone-co- PCLA syringeable drug delivery
lactide)-b-poly(ethylene depot, controlled protein
glycol)-b-poly(ε- delivery, 3D printing, and
caprolactone-co-lactide cancer therapy
(PCLA)
A mixed solution of cellulose, Fused deposition Deionized water solvent Water absorption of 28 g/g, Cellulose hydrogel scaf- Hu et al. (2020b)
dimethyl sulfoxide (DMSO), molding (FDM) exchange is print pattern compressive strength of folds
and tetrabutyl ammonium molding 96 kPa
hydroxide (TBAH)
Cellulose acetate/ethyl acetate DIW The aqueous layer formed Oil–water separation Highly efficient oil–water Koh et al. (2019)
solution by the pre-wetting of the separation applications
printed cellulose web
insulates the cellulose and
oil from van der Waals
interactions
Flax fragments grafted with FDM Covalent reaction of amino- Fluorescent emission Sensors depending on the Mayer Laigle et al. (2021)
fluorescent groups and com- fluorescein with free fluorophore used
plexed with poly-(butylene hydroxyl groups of flax
terephthalate) fibers
Environmental Chemistry Letters (2024) 22:1929–1987
Table 2  (continued)
Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Continuous flax fiber bundle FDM _ Strong tensile strength, Natural Fiber Composites Hinchcliffe et al. (2016)
composite PLA stiffness, and flexural
strength, stiffness
Poly(vinyl acetate) modified FDM _ Strong interlaminar adhe- Functional materials such Wu et al. (2022)
cellulose nanocrystal, poly- sion and toughness as shape memory, and
L-lactic acid, and polyether- electrical and thermal
based polyurethane conductivity
Cellulose dehydrated and FDM _ Good mechanical properties 3D bioprinting Li et al. (2018)
freeze-dried after dissolving
in N-methylmorpholine-
N-oxide (NMMO)
Regenerated cellulose and FDM _ High storage modulus Furniture or building com- Gauss et al. (2022)
PLA ponents for biomedical
Environmental Chemistry Letters (2024) 22:1929–1987

and dentistry applications

Carboxymethylated cellulose DIW Carboxymethyl cellulose of Excellent shear-thinning Tissue engineering Radeke et al. (2023)
micro-fibrillated cellulose properties
Hydroxypropyl Cellulose DIW Crosslinking of glutaralde- The twisting behavior of High-quality light filters, Balcerowski et al. (2023)
hyde with hydroxypropyl the ink can be changed polarizers, and mono-
cellulose by printing conditions to chromators for optical
show different structural applications
colors
Poly(acrylamide-co-acrylic Digital light printing Sodium dodecyl sulfate Excellent conductivity (0.83 Flexible strain sensor for Guo et al. (2023)
acid)D/cellulose nanofiber (DLP) (SDS) as photoinitiator S/m) human motion monitoring
Cellulose nanocrystal, elasto- FDM _ CNC has self-generated pie- Biomedical device develop- Maity et al. (2023)
meric thermoset polymers zoelectric properties for ment and human–machine
mechanical to electrical- interface
energy conversion
Carboxymethyl cellulose/hBN DIW _ When mechanical strain A flexoelectric energy Jayakumar et al. (2023)
is applied, a charge state harvester
fluctuation and spontane-
ous polarization in the
hBN/CMC matrix are
seen
Cellulose nanocrystal, Two-photon polymeriza- _ Non-cytotoxic microscale Small-scale energy absorp- Groetsch et al. (2023)
methacrylate resist, and tion printed structures tion devices
γ-butyrolactone (GBL)
TOCNF ((2,2,6,6-tetrame- DIW TOCNF has carboxyl and Excellent EMI shielding Complex geometries with Erfanian et al. (2023)
thylpiperidin-1-yl) oxidanyl hydroxyl groups that effectiveness tuned compressibility and
(TEMPO)-oxidized cellulose form a large number of electrical conductivity
nanofibrils) and electrochem- hydrogen bonds with EGO
ically synthesized graphene functional groups
oxide (EGO)
1947
Table 2  (continued)
1948

Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Bilayer structure formed by DIW _ Highly absorbent properties Solar-driven atmospheric Zhu et al. (2023)
cellulose nanofibers /LiCl prevent salt leakage at the water harvesting
and cellulose nanocrystal/ same time
carbon nanotube
Cellulose nanofibers and PLA FDM In situ polymerization reac- Excellent thermo-mechani- Bio-composites Gauss and Pickering (2023)
tion of L-propanediolate cal stability
Keratins Keratin/PLA FDM NaOH slightly erodes Favorable for cell growth Bio-composites from waste Flores Hernandez et al.
keratin sources (2021)
Polycaprolactone (PCL)/ FDM and electro-spun _ Favor cell adhesion and Skin repair applications Choi et al. (2021)
keratin electrostatically spun proliferation
scaffolds and 3D printed
polymer scaffolds
Alpha and gamma keratin and DLP Oxidation of keratin by Favor cell adhesion and Tissue engineering and Placone et al. (2017)
initiator-catalyst-inhibitor peroxyacetic acid proliferation regenerative medicine
Wool keratin (WK) and 2-iso- Direct-write photolithog- UV cross-linking reactions High-fidelity, high-resolu- Tissue engineering, bio- Zeng et al. (2020)
cyanate ethyl methacrylate raphy of WK and IEMs tion photoresist logical array, and drug
(IEM) delivery
Lignin and keratin FDM Cross-linking reactions Mechanical response to Functional material Grigsby et al. (2020)
between keratin and lignin water stimulation
Keratin and initiator-catalyst- DLP _ Release of drugs Repair of skin tissue after Navarro et al. (2020)
inhibitor burns
Silk-wool-tannic acid DIW The synergistic effect of Increases wound healing Skin wound healing field Jafari et al. (2023)
hydrophobic and hydrogen
bonding of polyphenols
with proteins is the main
mechanism of gelation
Wool keratin (WK), silk Screen printing _ Excellent structural stability Textile anti-counterfeiting Zeng et al. (2023b)
fibroin (SF), and Au–Ag and high fluo­rescence
nanoclusters (NCs) intensity
Silk Carbon nanotubes (CNTs) as Coaxial extruder printer Partial dissolution of silk Converting the mechanical Energy-management Zhang et al. (2019a)
a conductive core and silk by formic acid/CaCl2 dis- energy of human motion systems, flexible sensors,
fibroin as a dielectric sheath solution into electrical energy electric antennas, and
other functional circuits
Silk proteins and graphene DIW The introduction of phe- High mechanical toughness, Cyborganics, bionics, soft Kadumudi et al. (2021)
oxide nolic gum promotes the electrical conductivity robotics, human–machine
formation of sacrificial Young’s modulus, and interfaces, 3D-printed
and hierarchical hydrogen self-healing properties electronics, and flexible
bonds bioelectronics
Environmental Chemistry Letters (2024) 22:1929–1987
Table 2  (continued)
Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Silk and gold nanoparticles Inkjet printing _ The addition of nanoparti- A custom library of inkjet- Tao et al. (2015)
cles, enzymes, antibiot- printable, functional “silk
ics, growth factors, and inks” for use in sensing,
antibodies gives the ink a therapeutics, and regen-
different function erative medicine
Silk protein solution, photoini- Multi-photon lithography Multi-photon lithography Microlithography structure Microreactors containing Dickerson et al. (2017)
tiator crosslinking after printing printing enzyme cascades for use
in fuel cells or diagnostic
devices
Silk protein inks and poly- DIW Chloroform dissolved sacri- The printed structure has a Insulation, tissue-engi- Sommer et al. (2016)
caprolactone as sacrificial ficial material hierarchical pore structure neered supports
agents
Silk sericin (SS), silk fibroin Volumetric additive Photocrosslinking reactions Reversible volume change, Shape-memory materials, Xie et al. (2023)
Environmental Chemistry Letters (2024) 22:1929–1987

(SF), and ruthenium (II) manufacturing between SS, SF, and adjustable mechanical 4D printing, soft robotics,
hexahydrate (Ru)/sodium RuSPS properties, and biocom- and drug delivery
persulfate (SPS) (Ru-SPS) patible properties
Silk proteins (SF) and 4-arm DLP The cross-linking reaction Favorable for cell prolifera- Biomedical and biotechnol- Kwak et al. (2019)
polyethylene glycol acrylate of 4-arm PEG precursors tion ogy fields
(PEG 4A) under visible light
Alginate/PVA and silk fibroin DIW _ Favorable cell adhesion and Maxillofacial surgery Sangkert et al. (2021)
(SF) proliferation
Silk powder and PVA Binder Jetting The hydroxyl group of PVA High compression modulus Load-bearing biomedical Zhang et al. (2021)
reacts with the cross-link- applications
ing agent glutaraldehyde
to form acetal bonds
Fluorescent silk fibroin (FSF) DLP Covalent binding of FSF Fluorescent properties and Biomedical field Lee et al. (2022)
and glycidyl methacrylate and GMA excellent biocompatibility
(GMA)
Polycaprolactone and Silk FDM _ Favorable cell adhesion and Pre-clinical and clinical Bojedla et al. (2023)
fibroin microfibers proliferation studies for craniofacial
reconstructive
Silk fibroin, polyvinyl alcohol, DIW _ Good mechanical proper- Implantable devices and Indrakumar et al. (2023)
and methylcellulose ties, fatigue resistance, sensors
and shape recovery
properties
Synthetic peptides to deg- Extrusion-based bioprint- Covalent attachment of Excellent biocompatibility Wound dressings and bio- Ceccarini et al. (2023)
ummed silk fibers ing synthetic peptides to and moisture-sensing based nonvolatile sensor
degummed silk fibers capabilities
1949
 1950 Environmental Chemistry Letters (2024) 22:1929–1987

moisture and expand. The response of cellulose-based mate-

tures, and potential application areas. The abundance of reactive groups in cellulose allows for easy modification through physicochemical processes to customize the properties and functionality
The figure showcases the utilization of natural fibers in 3D printing technology, covering material formulations, printing techniques, related mechanisms, functional properties of printed struc-

combined with additive manufacturing technologies for precise fabrication and customization, animal fibers offer valuable insights for creating applications with diverse scales and unique require-
of composites. Animal fibers, known for their biocompatibility, are gaining attention in various fields like biomedicine, tissue engineering, flexible electronics, and wearable technology. When

ments. In summary, the exceptional performance and wide availability of natural fibers play a crucial role in advancing the development of environmentally friendly and sustainable materials
rials or structures to ambient moisture is influenced by the
Zhang et al. (2023c) difference in moisture levels and the rational distribution of
cellulose. These factors have led to the emergence of numer-
Qin et al. (2021) ous promising applications. Sydney Gladman et al. (2016)
investigated shear-induced cellulose alignment through the
DIW technique. The hydrogels exhibited distinct anisotropic
stiffness and swelling strain in both the printing direction
Ref

and laterally (Fig. 7a). By employing different lattice angle

designs (Fig. 7b), the printed hydrogel could be deformed
devices, nanoscale robot-
Biomimetics, molecular

into a predetermined bionic petal structure, enabling it to

Proposed application

respond to changes in humidity (Fig. 7c, d). This research

Biomedical fields

offers valuable insights into the 4D printing of cellulose

smart structures for solving inverse problems. The hygro-
scopic expansion property of cellulose is a crucial principle
for achieving humidity sensing. This principle drives the
ics

humidity difference between the upper and lower layers of

the cellulose film structure, similar to the active and passive
Favorable cell proliferation

High-resolution and com-

layers in cellulose composite materials (Fig. 7e, f). This form

plex printed structures

of cellulose-based materials is commonly used to facilitate

humidity control. Inspired by the stimulated deformation
of pine cones, a composite ink was prepared by doping
adhesion

cellulose pulp fibers among carboxymethyl cellulose. The

Function

content of cellulose and filler was adjusted and the inks had
different peak viscosity yield stresses to optimize the best
ink formulation. Figure 7g shows reversible deformation of
Methacrylation of AFS by

the 3D-printed composite hydrogel between hydration and

methacrylic anhydride

dehydration (Mulakkal et al. 2018).

Related mechanisms

Similarly, a 4D printed biomimetic water-responsive scale

material was developed, derived from a composite of cellu-
lose and acrylonitrile butadiene styrene (ABS) (Fig. 7h). The
bilayer structure deforms differently in response to humidity
by adding different constraints in the transverse and longi-
_

tudinal directions (Correa et al. 2020). Non-uniform stress

distribution in the upper and lower layers plays a crucial
Spider silk Genetically engineered recom- Electron beam lithog-

role in enabling self-deformation in 3D printed structures, as

Printing techniques

illustrated in Fig. 7i. Gu et al. (2023) developed a cellulose

nanofiber reinforced polycaprolactone (PCL)/polybutylene
terephthalate (PBAT) thermo-responsive shape memory pol-
raphy

ymer composite. Cellulose nanofibers were incorporated to

DLP

improve interfacial bonding and mechanical properties of the

composite. Drawing inspiration from plant climbing mecha-
Antheraea pernyi silk fibroin

binant spider silk proteins

nisms, these composites were utilized in the design of 4D

printed soft grippers (Fig. 7j). The primary concept behind
Fiber type Printing formulations

the grippers’ self-deformation involved leveraging 3D print-

ing technology to control stress distribution in the upper and
lower layers. Remarkably, the gripper demonstrated the abil-
ity to lift weights to 30 times its weight. Cellulose can also
Table 2  (continued)

be mixed with other shape memory polymers in addition to

being smart hydrogel. A more uniform porous structure can
be formed by introducing nano-cellulose into shape memory
polyurethane (SMPU) (Fig. 7k). The introduction of cel-
lulose significantly improved the shape fixation ratio, the
Environmental Chemistry Letters (2024) 22:1929–1987 1951

Fig. 7  The self-deformation mechanisms of 4D printed cellulose deformation of 4D-printed bilayer structures with active and passive
structures and their potential applications. The hygroscopic swelling layer arrangements. g, h Photographs showing the physical deforma-
property of cellulose plays a key role in achieving moisture-stimu- tion of these structures. Reprinted from the reference (Mulakkal et al.
lated deformation, while cellulose is often utilized as a filler in shape 2018) with open access creative commons CCBY license. Reprinted
memory polymers to enable thermo-responsive deformation. The fig- with permission of Royal Society from the reference (Correa et al.
ure presented illustrates various common 4D-printed cellulose struc- 2020). i, j Self-deforming structures with inhomogeneous stress dis-
tures, their deformation mechanisms, and their related applications. tribution structures and their deformation processes. Reprinted with
(a–d) Smart response principle and smart bionic petal model of 4D permission of Elsevier from the reference (Gu et al. 2023). k, l Defor-
printed cellulose hydrogel. Reprinted with permission of Springer mation mechanisms of cellulose-reinforced shape memory polymers
Nature from the reference (Sydney Gladman et al. (2016). e, f The and their deformation processes. Reprinted with permission of Else-
mechanisms of bending expansion caused by asymmetric humid- vier from the reference (Zhou et al. 2022b)
ity distribution in 4D-printed cellulose and the humidity-stimulated

shape recovery ratio, and mechanical properties of SMPU. the development of smart biomaterials and smart textiles
The glass transition temperature (Tg) of polyurethane var- (Zhou et al. 2022b). Research on 4D-printed cellulose-based
ies with cellulose content, with the lowest Tg close to the materials is still in its early stages, with a current focus on
human body temperature (Fig. 7l), which was important for cellulose hydrogels and biocomposites. However, these
1952 Environmental Chemistry Letters (2024) 22:1929–1987

materials face several challenges, including limited innova- moisture-absorbing and swelling properties of cellulose,
tive application scenarios, inadequate humidity responsive- 4D-printed flexible actuators, and bionic devices find
ness for large-size structures, and complex programming. extensive applications in smart buildings and smart tex-
Animal fiber: In 4D printing field, animal fibers have the tiles. Additionally, protein-based animal fibers also exhibit
most applications in the biomedical field due to their unique deformation in response to humidity, and 4D printed
mechanical properties and good bio-affinity (Fig. 8a). De structures derived from these fibers demonstrate excellent
Maria et al. (2021) designed a printed core–shell coiled bio-functional and mechanical properties, making them
structure with graphene nanosheet-modified regenerated advantageous in smart textiles, tissue engineering, and
silk as the core and poly (3-hydroxybutyrate-co-3-hydroxy medical fields. Overall, natural fibers offer the potential
valerate) (PHBV) as the shell. Illustration of the core-sheath for metamaterials and advanced smart materials due to
structure and FTIR spectra of relevant components are their multifunctionality, positive biological effects, and
shown in Fig. 8b. The 4D-printed tendrils can respond to mechanical properties.
temperature and moisture stimuli, resulting in self-twisting
and reversible stretching. Finally, the 4D-printed tendril-like Synthetic fiber in additive manufacturing
structure was used for the retraction integration of the intes-
tinal prosthesis flap structure (Fig. 8c). Its main working Synthetic fibers are produced through the polymerization
principle is based on the fact that the nucleus and the sheath of polymer compounds, which are commonly derived from
have opposite coefficients of thermal expansion (Fig. 8d). petroleum products. These fibers have high glass transition
Wool keratin can self-assemble into a nematic phase induced temperatures and can melt at high temperatures, making
by shear stress, obtaining the native hierarchical organiza- them ideal for utilization in additive manufacturing pro-
tion of protein (Fig. 8e). The strong shear-thinning proper- cesses, particularly fused deposition modeling. Synthetic
ties of protein hydrogels can be processed into delicate struc- fibers frequently have broad applications due to their high
tures. Keratin fiber bundles exhibit wet-responsive shape strength-to-weight ratio, corrosion resistance, low cost, and
memory behavior and the permanent shape of the printed good processing (Al Rashid and Koҫ 2021). The develop-
structure can be changed (Fig. 8f). A detailed record of the ment of synthetic fibers in additive manufacturing is ham-
wet-responsive shape memory process was shown in Fig. 8g, pered by printability and material properties, which can
demonstrating 3D-printed keratin architectures can quickly be typically improved by the addition of fillers or chemi-
recover from coiled tube shape to star-shaped pattern after cal modifications (Yilmaz et al. 2021). Researches in the
water stimulation (Cera et al. 2021). Silk fibroin hydrogel additive manufacturing field regarding synthetic fibers has
can be used to develop DLP printing materials by adding primarily concentrated on the development and production
photocurable agents. Printed bilayer bioproducts are subject of composite materials. By physicochemical processes, syn-
to deformation when stimulated by the culture environment thetic fiber composites demonstrate robust properties and
(Fig. 8h), and their possible deformation can be predicted by functionalities that cater to a wide range of applications.
finite element analysis. After blending two types of growth This section will focus on discussing several commonly used
cells into the printed tracheal structure and implanting it into synthetic fibers in the realm of additive manufacturing.
the damaged trachea of rabbits for 8 weeks, the implanted
trachea formed epithelium and cartilage; Fig. 8i showed the
implanted trachea and the fusion of the 4D printed trachea 3D printing field
and the native trachea at different times. After 4 weeks, the
scaffold surface completely covered the epithelial mucosa, Polyethylene terephthalate (PET) occupies a high propor-
the airways were open and the stenosis appeared stable tion of textile fibers and has received widespread attention
for up to 8 weeks (Kim et al. 2020b). The response of 4D in AM. Polyethylene terephthalate glycol (PETG) has high
printed animal fiber composites to temperature or humid- thermal stability and excellent thermal degradation resist-
ity combined with good biocompatibility makes them very ance and can be employed to manufacture components
promising for biomedical applications. with high rigidity and thermoplastic 3D printing materials
Natural fibers have the potential to be designed as intel- (Grigore et al. 2020). Carbon fiber (CF) is often used as a
ligent materials through physical or chemical processes, reinforcing filler in PET (Kichloo et al. 2021; Mansour et al.
filler modification, and advanced manufacturing technol- 2018; Vijayakumar et al. 2022). Vijayakumar et al. (2022)
ogy. The emergence of 4D printing has opened up new reported a study on the incorporation of shell walls in the
opportunities and possibilities for these fibers, particu- planar-type hexagonal lattice structure of PETG/CF com-
larly in the biomedical field. Plant systems composed of posites (Fig. 9a). The researchers optimized the compressive
natural fibers possess the ability to respond to moisture strength and printing parameters, and analyzed the key pro-
spontaneously and undergo deformation. By utilizing the cess parameters that affect both the compressive strength and
Environmental Chemistry Letters (2024) 22:1929–1987 1953

Fig. 8  Deformation mechanisms and applications of 4D printed ani- tin secondary structure during the transition from α-helix to β-sheet
mal fiber materials are explored in this study. The unique combina- under strain, and the wet-responsive shape memory mechanism of
tion of strong comprehensive properties and biocompatibility in ani- wool keratin. g The diagram also depicts the shape memory process
mal fibers shows promising potential for applications in biomedicine, of the intact wool keratin 3D printed structure. Reprinted with per-
flexible wearables, and tissue engineering using 4D printing technol- mission of Springer Nature from the reference (Cera et al. 2021). Silk
ogy (a). The figure illustrates the mechanism and application of stim- protein hydrogel bilayer structures were prepared using digital light
ulus-responsive deformation achieved by 4D-printed animal fibers. processing. h The bilayer hydrogel structures exhibited deformation
This research sheds light on the significance of animal fibers and 4D in aqueous solution as a result of anisotropic volume changes. When
printing technology in the development of metamaterials and regen- a bilayer hydrogel structure simulating a trachea was implanted into
erative materials for tissue repair. b–d 4D printed core-sheath ten- damaged rabbit trachea, the implant integrated well with the host tra-
dril structures, actuator applications, and their working mechanisms. chea naturally (i). Reprinted with permission of Elsevier from the ref-
Reprinted with permission of Wiley from the reference (De Maria erence (Kim et al. 2020b)
et al. 2021). e, f Schematic illustration of the rearrangement of kera-

dimensional errors. They found that a nozzle temperature of as a thermal barrier, preventing the polymer from volatil-
220 °C, a layer height of 0.1 mm, a filler density of 100%, izing at high temperatures. Additionally, the well-bonded
and a printing speed of 20 mm/s resulted in higher compres- interface between the graphene and polymer contributes to
sive strength. Additionally, previous studies have demon- a significant improvement in the thermal stability of PETG
strated that CF/PETG composites exhibit improved friction (Bedi et al. 2023). The addition of sepiolite to PETG led to
properties compared to pure PETG (Kichloo et al. 2021). To a 35.4% enhancement in the tensile properties of the com-
enhance the thermodynamic properties of PETG, graphene posites compared to PETG fibers (Kim et al. 2020a). This
was doped into it, resulting in a composite that remained improvement can be attributed to the anisotropic arrange-
undamaged even at 400 °C. The presence of graphene acts ment of sepiolite along the printing direction, as well as the
1954 Environmental Chemistry Letters (2024) 22:1929–1987

synergistic effect between the nanostructure and the poly- their mechanical properties. Selective laser sintering (SLS)
mer, resulting in a substantial increase in the performance of technology could be used to print PA powder into 3D flex-
the composite material. PET composites based on new fillers ible weft knitted structures with stretching and flexibility
suitable for 3D printing are gaining attention. of traditional knitted fabrics (Beecroft 2019). Gong et al.
In addition, PET can be compounded to give it functional (2021) fabricated a flexible honeycomb absorber made of
properties. Layered transparent electromagnetic interfer- a novel carbon fiber/PA/carbonyl iron composite. The high
ence (EMI) shielding patterns can be achieved using nano- flexibility of absorber allowed it with excellent microwave
silver wires and PETG through laser marking and transfer absorption capability even at large bending angles. The syn-
printing. The resulting three-layer composite shielding film ergistic enhancement of continuous carbon and kevlar fibers
exhibits a light transmittance of 67.8% at 10 GHz, along could obtain high strength and good ductility for PA matrix
with a shielding effectiveness of 44 dB. Moreover, the EMI composites (Wang et al. 2021a). Physical blending with
shielding devices offer the advantage of customization, novel fillers offers process simplicity and excellent overall
allowing for structural adjustments to both the shielding performance compared to printable PA chemical modifica-
capability and light transmittance of the device (Gu et al. tion processes.
2020). Chatham et al. (2019) investigated the enhancement Polyacrylonitrile (PAN) showed advantages in viscos-
of composite properties by blending PETG with other poly- ity control, conductivity, high performance, and precursor
mers. They successfully prepared a semi-crystalline blend candidates in the AM field. The viscosity, conductivity,
of PETG, PP, and polypropylene grafted with maleic anhy- and performance advantages of PAN make it a viscosity
dride. This blend exhibited good printability and potential regulator for printable electrolytes in solar-sensitized bat-
for application in high-modulus and heat-resistant materials. teries. Increasing PAN concentration improved printing
Additionally, physical blends of glycol-modified PET and performance but reduced battery performance, which can
thermoplastic polyurethane (TPU) were found to possess be compensated for by introducing titanium dioxide ­(TiO2)
good biocompatibility, excellent printability, and impressive or titanium carbide (TiC) nanofillers. The cell efficiency was
mechanical properties. These blends hold promise for appli- above 96% after testing for 500 h (Venkatesan et al. 2015). A
cation in idiosyncratic maxillofacial prosthetics (Katschnig nanofiltration membrane could be prepared by inkjet print-
et al. 2020). PET has high thermodynamic and low cost that ing nanoscale graphene oxide on modified PAN substrate.
provide insights for the exploitation of new composites. This nanofiltration membrane has an order of magnitude
Polyamide (PA) is a highly effective engineering ther- higher water permeability than conventional polymeric
moplastic known for its exceptional performance in various nanofiltration membranes, with filtration efficiency of up to
applications (Jia et al. 2017). However, during the process of 95% for small molecule organics (Fathizadeh et al. 2017).
3D printing, PA is susceptible to stress accumulation, which Kang et al. (2022) reported a methylammonium lead bro-
often results in warpage of the printed structure. To over- mide/PAN optoelectronic composite material prepared by an
come this challenge, it is crucial to address interlayer stress electrohydrodynamic injection process. The printed pattern
accumulation. The mixture of maleic anhydride grafted has high resolution, approximately 10 μm, tunable nanomor-
poly (ethylene 1-octene) and rigid polystyrene prevented the phology, high crystallinity, light transmittance over 95%,
orderly arrangement of molecular chains during PA6 crystal- and underwater stability for 20 days (Fig. 9c). An intrinsic
lization, reducing its shrinkage stress, and thus producing a PAN-copolymer plasticizer could avoid unnecessary thermal
PA6 filament with good toughness and printing performance carbonization systems by reducing its melting temperature.
(Fig. 9b) (Jia et al. 2017). The use of short fibers to rein- This method allowed the 3D-printed PAN-copolymer com-
force PA significantly enhances the overall performance of ponent to be thermally carbonized and realized mold-free
the printed substrate. To illustrate, basalt fibers combined rapid prototyping of carbon materials. An open mesh carbon
with a low melting point PA (L-PA) to create printed sub- electrode was printed for supercapacitors, with a maximum
strate, exhibited excellent printing properties. Compared capacitance of 387 Mf ­cm−2 and a thickness of only 1.5 mm
to pure L-PA, the composites demonstrated substantial (Usselmann et al. 2022). Liu et al. (2023a) reported a high-
improvements in tensile modulus, tensile strength, and spe- performance 3D-printed solar evaporator made of PAN and
cific energy absorption per unit volume, with increases of carbon nanotubes, with light absorption up to 98.3% and
176.6%, 142.0%, and 172.2%, respectively, without com- excellent photovoltaic water harvesting properties. On the
promising ductility. This enhancement can be attributed to side, even in highly concentrated saline water, the evapora-
the shearing of basalt fibers into fine short fibers and their tor still has a high evaporation rate and good self-cleaning
proper dispersion within the matrix during the extrusion performance. PAN has promising applications in carbon
process (Hua et al. 2023). In addition, Chen et al. (2021a) material applications, printable electrolytes, and photother-
reported that carbon fiber addition could effectively improve mal materials.
Young’s modulus of 3D-printed PA composites, enhancing
Environmental Chemistry Letters (2024) 22:1929–1987 1955

Fig. 9  Synthetic fibers play a crucial role in the 3D printing mate- nium lead tribromide/polyacrylonitrile (MAPbBr3/PAN) composite
rial system. Due to the specific requirements and limitations of pure and corresponding scanning electron microscopy images. Reprinted
synthetic fibers, current research focuses on developing high-per- with permission of ACS from the reference (Kang et al. 2022). d 3D
formance functional materials through physical filler composites or printed PP composite fixing plate (Kabiri et al. 2021). e Photos, drug
chemical modifications. The figure illustrates the application advan- release mechanism, and drug release performance of 3D printed chi-
tages of various synthetic fibers and outlines typical material prepa- tosan/poly(vinyl alcohol) hydrogels. Reprinted with permission of
ration processes or applications. a Schematic representation of poly- Wiley from the reference (Liu et al. 2021b). f Photos, scanning elec-
ethylene terephthalate glycol/carbon fiber composites with hexagonal tron microscopy images, and stress relaxation experiments of FDM
lattice structure. Reprinted with permission of Springer Nature from printed polyvinyl chloride/ diisopropyl phthalate structure. Reprinted
the reference (Vijayakumar et al. 2022). b 3D printed nylon 6 com- from the reference (Calafel et al. 2020) with open access creative
posites with different formulations. Reprinted with permission of commons CCBY license
Wiley from the reference (Jia et al. 2017). c 3D printed methylammo-
1956 Environmental Chemistry Letters (2024) 22:1929–1987

Polypropylene (PP) is a widespread thermoplastic mate- improved the printing property of the hydrogel and endowed
rial, and composite or adding functional fillers can endow it with antibacterial capacity, while PVA provided mechani-
printable PP composites with various properties. For exam- cal properties and reduced swelling properties. In addition,
ple, composites from laminating bamboo fibers, poly(lactic the loaded antitumor drugs into hydrogel scaffolds can be
acid) (PLA), and PP with appropriate amount of compatibi- released continuously, and release amount is related to pH
lizer have unique colors and strength, making them potential of release environment (Fig. 9e).
alternative consumables for 3D printing (Long et al. 2019). Similarly, (Goyanes et al. 2016) developed a 3D-printed
In addition, glass fiber-reinforced PP composites could be drug delivery capsule made of water-soluble PVA and can be
used as bone-healing fixation plates owing to their excel- used in drug delivery. PVA-based materials are well suited
lent bending strength. This 3D-printed composite fixation for cell growth and proliferation and play an important role
plate can provide the support necessary for bone healing in tissue engineering and biomedicine. PVA is also used in
and sufficient movement between fracture blocks, showing the development of functional materials. Li et al. (2020)
more advantages in load-bearing capacity and reduced stress utilized cellulose acetate and nanoscale silicon dioxide
shielding compared to metal fixation plates (Fig. 9d) (Kabiri ­(SiO2) to create a printed PVA composite mesh. This mesh
et al. 2021). Silicon dioxide ­(SiO2) could also serve as a exhibited superhydrophobic and submerged superhydropho-
reinforcing agent for PP and its content affects the mechani- bic properties. Notably, the mesh demonstrated exceptional
cal properties, rheological properties, and microstructure of mechanical stability and achieved an impressive oil–water
composites. When the concentration was 1–2% by weight, separation efficiency of up to 99%. Cellulose nanocrystals
the mechanical properties were significantly improved with- as fillers can significantly raise the stiffness, dimensional
out affecting printing performance. When the concentration stability, thermal performance, and biodegradability of PVA
increased to 4% by weight, the printing performance was (Cataldi et al. 2018). A composite material composed of
compromised (Vidakis et al. 2021). Mainly through intro- graphene nanosheets and PVA with electromagnetic interfer-
ducing fillers, the overall performance of PP-based printed ence shielding ability was prepared through FDM printing.
composite materials can be improved to enhance the com- The structure of PVA/graphene nanoplates (GNP) printed at
petition in the future. 200 °C is optimal. The incorporation of GPN brings good
Poly (vinyl alcohol) (PVA) has been widely used in bio- printing performance and hydrophobicity. Besides, electro-
materials and drug delivery based on its excellent biocom- magnetic interference shielding ability of PVA/GPN com-
patibility and degradability. The flexibility, hydrophilicity, posite is related to the content and thickness of GNP parts
semipermeability, and chemical stability of PVA can pro- (Yang et al. 2020). In conclusion, PVA is a polymer with
vide nutrient delivery capacity necessary for cell growth excellent comprehensive properties and has a promising
and proliferation. FDM-printed PVA filament can serve as application in future additive manufacturing field.
a drug-loading device (Berger et al. 2023; Matijašić et al. Generally speaking, polyvinyl chloride (PVC) materi-
2019; Xu et al. 2019). Hexagonal boron nitride (hBN) and als have good toughness and chemical stability. However,
bacterial cellulose were used as fillers to prepare PVA com- the material properties and thermal stability of PVC limit
posite bone tissue scaffolds. hBN improved the mechanical its application in AM, which can be overcome by filler,
properties and thermal conductivity, and the porous struc- modification, or composite. Calafel et al. (2018) prepared a
ture formed by bacterial cellulose upgraded the adhesion self-plasticized PVC by using single electron transfer-degen-
between cells and materials (Aki et al. 2020). The problem erative chain transfer living radical polymerization technol-
of weak interfacial bonding between polyether ether ketone ogy. The self-plasticized PVC has a lower glass transition
(PEEK) and PVA was solved by introducing amphiphilic temperature compared to pure PVC, which was conducive
graphene oxide (GO). π–π bonds were formed between to interlayer extrusion and adhesion in additive manufactur-
GO and PEEK, and strong molecular hydrogen bonds were ing. The incorporation of diisopropyl phthalate into PVC
formed with PVA, which effectively improved the poor significantly improved the printability, providing a flexible
interfacial bonding. A composite scaffold with good bio- and ductile 3D printing formulation. The stress relaxation
mechanical properties, hydrophilic and biodegradable was experiments of different samples at 180 °C showed that the
printed and applied to bone regeneration (Feng et al. 2020). concentration of diisopropyl phthalate is proportional to the
The incorporation of gelatin into PVA can print composite printing characteristics. The printing temperature was con-
scaffolds with sufficient mechanical strength, strong cell pro- sidered optimal at 210 °C, and the printed structure exhib-
liferation, and differentiation ability, showing high applica- ited better mechanical properties compared to the printed
tion prospects in the field of tissue regeneration. Moreover, structure at 190 °C. It can be seen in Fig. 9f, that printed
chitosan (CS) can be incorporated into PVA to form a dual layer bonding is good at the micro level (Calafel et al. 2020).
network hydrogel (Kim et al. 2018). Liu et al. (2021b) pre- Lewenstam et al. (2019) mixed a composition containing
pared a 3D-printed CS/PVA hydrogel scaffold (Fig. 9e). CS dicalcium chloride (KCl) with PVC and deposited it on a
Environmental Chemistry Letters (2024) 22:1929–1987 1957

3D printed acrylonitrile butadiene styrene (ABS) substrate through fillers, such as solar fresh water harvesting appli-
equipped with silver/silver chloride (Ag/AgCl) electrical cations developed by doping carbon nanotubes into PAN
contacts using 3D printing technology to form a reference (Fig. 10). PVA is highly regarded for its biocompatibility and
electrode or electrically active part, with excellent potential excellent processing properties. Some crosslinking agents,
stability and acid–base titration performance. Ethylene-vinyl such as glutaraldehyde, have allowed PVA composites to
acetate-glycidyl methacrylate (EVM-GMA) can be used as a meet printing requirements without losing their biological
plasticizer to construct special structures of poly(lactic acid) properties (Fig. 10). Physical bonds established by PVA with
and PVC, improving phase morphology, advanced printing, molecular chains containing oxygen-containing functional
and mechanical properties (Lyu et al. 2020). The excellent groups enhance the structural and thermal stability of com-
toughness and chemical stability of PVC materials will pro- posites, such as detonation nanodiamonds. In addition, the
vide ideas for the development of new flexible materials. incorporation of fillers such as cellulose, graphene, cellulose
The emergence of new types of fillers, such as graphene, acetate, ­SiO2, chitosan, and gelatin enables PVA-based com-
carbon fiber, and Kevlar, has contributed to the power- posites to meet the requirements of applications such as bone
ful properties of certain synthetic fibers. Fiber-reinforced repair, tissue regeneration, wound healing, oil–water separa-
printed composite filaments commonly use PET, PA, and tion, and bioprinting (Fig. 10). Polyvinyl chloride (PVC) is
PP as base materials, and by blending and optimizing the known for its good toughness and chemical stability, but its
manufacturing process, notable enhancements in compos- limited thermal stability restricts its application in additive
ite properties can be achieved. These cost-effective and manufacturing. However, the incorporation of fillers such as
straightforward methods hold great promise for the future diisopropyl phthalate (DINP) and butyl acrylic can greatly
application of 3D printing materials (Fig. 10). Nano-silver enhance the thermal stability of PVC (Fig. 10). Addition-
wires and PET can be used to make EMI devices, but they ally, the plasticizer dibutyl adipate (DBA) can be used to
are more expensive compared to other fillers. Graphene dissolve PVC in tetrahydrofuran (THF), enabling the flex-
is effective in enhancing the thermal properties of PETG, ible production of composites with added functionality. In
addressing the poor stability at high temperatures. The summary, synthetic fiber composites often involve fillers,
hydrogen bonding between sepiolite and PETG molecular modifications, pretreatments, and composites to ensure good
chains plays a crucial role in enhancing interlayer adhesion, printability, excellent function, and advanced properties.
and the use of micro-scale sepiolite can improve the ten- Table 3 provides a comprehensive review of the composite
sile properties of the material along the printing direction. process, associated mechanisms, performance enhancement,
Despite these advancements, PET printed materials still have and related applications of synthetic fiber. Synthetic fiber
weaknesses in interlayer adhesion, printability, toughness, printing materials have immense potential for applications in
and cost-effectiveness. PA has excellent overall properties textiles, tissue engineering, engineering materials, medical
but printed products often experience warpage. Maleic anhy- materials, and flexible electronics. The combination of AM
dride is commonly employed to enhance the printability of technology with the exceptional properties of synthetic fiber
PA (Fig. 10). The utilization of maleic anhydride grafted composites will enable sophisticated and future-oriented
polyoctene (POE-g-MAH) has proven effective in improving applications.
the interfacial bonding between PA and other polymers. Fur-
thermore, high-performance fibers like CF and Kevlar can 4D printing
be utilized as reinforcing fillers for PA, resulting in printed
structures that possess both high strength and good ductil- Synthetic fibers possess the capability to be engineered as
ity. Polypropylene has a wide range of applications in AM 4D printed materials. By strategically arranging the distribu-
field, particularly in the research on composites and related tion of molecular soft and hard segments or crystalline and
properties achieved through fillers or other polymers blend- amorphous domains, synthetic fibers can serve as vital con-
ing. These new fillers, such as carbon fibers, glass fibers, stituents of shape memory polymers. Apart from exhibiting
carbon black, ­SiO2, and plant fibers, play a crucial role in shape memory effects, synthetic fibers can also be rendered
improving the mechanical properties, printability, and func- 4D-printed structures by adapting to thermal expansion and
tionality (Fig. 10). deformation in response to moisture stimulation. These 4D
Some synthetic fibers have special functionality based printed synthetic fiber materials, characterized by their light-
on their unique molecular structure. PAN as a precursor of weight nature, exceptional shape fixation and recovery rates,
carbon materials has a wide range of applications. offering as well as high performance, hold immense potential for
a significant solution for the cost-effective and sustainable diverse applications in the future.
manufacturing of carbon fibers. PAN is a potential electro- PET can be applied in 4D printing mainly through physic-
lyte that would be promising in applications related to flexi- ochemical processes that give it a shape memory effect. Mul-
ble batteries. PAN can be endowed with additional functions tifunctional co-polyesters are prepared by introducing three
1958 Environmental Chemistry Letters (2024) 22:1929–1987

Fig. 10  Molecular structure of synthetic fiber and associated syn- Reprinted with permission of ACS, Elsevier, and Wiley, from the ref-
thetic process. Common compounding processes, fillers, modification erence (Gong et al. 2021; Kim et al. 2020a; Usselmann et al. 2022;
methods, and some reaction mechanisms for various synthetic fibers. Zeng et al. 2023a)

monomer-side phenylacetylene-phenylamine units and phe- enhanced tensile strength. It is worth noting that C≡N bonds
nylacetylene groups into PET, resulting in π–π stacking and can be generated during combustion, giving PET composite
synergistic crosslinking units. The existence of π–π stacking materials excellent flame retardancy (Fig. 11a), which can be
was regarded as a reversible network, endowing the mate- used in fire alarm systems. The mechanical properties show
rial with a shape memory effect and self-healing properties a marked improvement compared to traditional shape mem-
(Fig. 11a, b). Moreover, strong molecular chain interactions ory polymers (Chen et al. 2019a). Physical aging technology
Environmental Chemistry Letters (2024) 22:1929–1987 1959

endowed polyethylene terephthalate glycol (PETG) with printed structure using swelling polyurethane elastomer and
self-deformation and shape memory properties. The pre- heat-shrinking shape-memory PVC and ensured the defor-
strain of interlayer functional gradients was optimized by mation diversity by adjusting printing thickness and angle.
adjusting printing parameters (print speed, temperature) and The bilayer structure depicted in Fig. 11g undergoes bend-
programming conditions, thereby improving the self-defor- ing deformation under water and thermal stimuli. By con-
mation and shape memory behavior of 4D printed PETG. trolling the filling angle, this structure exhibits a complex
PET can be also melted and blended with other polymers to deformation pattern, as illustrated in Fig. 11h. There are two
improve shape memory effect, for example, the shape recov- primary methods for polymers to achieve electrically stimu-
ery can be increased by mixing PA filaments into rigid PET lated response deformation. One involves the deformation
(Aberoumand et al. 2022). The design of PET as a smart of polymer gel caused by electric Maxwell stress when sub-
material incorporating other functional properties will sig- jected to an electric field, as depicted in Fig. 11iI. The other
nificantly increase its application value. method involves incorporating a suitable amount of elec-
In addition to the shape memory properties obtained by tro-thermal fillers into shape memory polymers to achieve
modification, PA is itself capable of deforming in response electrically stimulated response deformation, as illustrated
to moisture stimulation. An intelligent textile has been devel- in Fig. 11iII.Wang et al. (2021b) proposed a method of elec-
oped by printing PLA with shape memory properties on the trically activated hydrogels. Specifically, PVC was dissolved
surface of nylon fabric. A temporary shape was given under in tetrahydrofuran to prepare ink precursor, dibutyl adipate
heating conditions, and then the fabric could respond to (DBA) was utilized as a plasticizer, and the solution content
stimuli and return to its permanent shape when the tempera- to make it printable. The printed objects were solidified by
ture was raised again (Leist et al. 2017). Peng et al. (2019) the volatile solvent, and the mechanical property and drive
developed a new type of PA/PP composite, using maleic capability of the PVC gel were optimized by adding a plas-
anhydride grafted poly(ethylene octene) as a compatibilizer ticizer. This hydrogel could be used to design an electrically
and modifier. The proportional parameters of the three were actuated jellyfish-like driver (Fig. 11j) and an electrically
controlled to ensure adequate mechanical properties and controlled optical diffuser. PVC shows good prospects in
good dimensional stability of PA/PP composites. The higher the field of 4D printing.
melting temperature of the PA6 crystalline phase, along with PVA and its methacrylate derivatives (PVA-MA) were
the doped chemical cross-linking sites, serves as the station- blended by photopolymerization to form a high-toughness
ary phase within the polymer matrix, while PP functions as polymer. N-isopropyl acrylamide (NIPAM) was incorpo-
the reversible phase. This configuration results in composites rated into PVA-MA as a reactive monomer that imparts
exhibiting a shape memory effect, as illustrated in Fig. 11c. thermal response to PVA composites. Digital light process-
The shape memory mechanism of PA6/PP is depicted in ing technology (DLP) was utilized to print the entity, induc-
Fig. 11d, indicating that these shape memory composites ing the formation of PVA nanocrystalline domains by salt
have promising properties in the field of 4D printing. PA6 out, and re-strengthening the composite hydrogel network.
can respond to moisture and make corresponding shape For an application, the composite hydrogel was designed
changes. A double-layer asymmetric 3D-printed structure as a double-layer actuator and mechanical gripper based
was achieved by adding continuous carbon fiber (CCF) onto on thermal drive and mismatched thermal expansion coef-
the top layer of PA6 layer (Fig. 11e). This structure could ficient (Fig. 11k). In addition, remote control capability was
respond to humidity change and show different deforma- realized by applying light absorbers to the gripper of the
tion curvatures at different humidity levels, the relevant 4D printing robot (Fig. 11k). 4D-printed PVA composite
mechanism is shown in Fig. 11f. Presence of CCF reduced hydrogel lattice structure toughened with sodium sulfate
the swelling characteristics of PA materials and enabled the ­(Na2SO4) recovers after loading and also improves thermal
dual-layer architecture to break the slow recovery of water- actuation speeds (Fig. 11l) (Hua et al. 2020). This study
driven actuators by generating heat through external input offers valuable insights for robots or actuators with high
(Le Duigou et al. 2019). toughness and multi-response flexibility. Furthermore, PVA
FDM-printed PVC has been verified to have good shape materials exhibit favorable biological properties; however,
memory effect in recent studies. It is speculated that the limited research has been conducted on the application of 4D
shape memory property of PVC was imparted by the imper- printed PVA composites biology and medicine field.
fect thermodynamically stable crystal, and it can be further Synthetic fibers integrated with 4D printing offer
enhanced by the entanglement of mesocrystals and mol- numerous advantages, including good deformation effect,
ecules. 3D-printed filaments can be obtained by mixing lightweight, strong physical properties, and a wide range
PP with PVC, and the composite of 50% PP and 50% PVC of material sources. The intelligence of 4D-printed syn-
has good mechanical and shape memory properties (Ran- thetic materials is achieved through the rational distribu-
jan et al. 2021). Ren et al. (2021) designed a double-layer tion of crystalline and amorphous domains, as well as the
Table 3  Synthetic fiber printing formulations, printing techniques, related mechanisms, functions, and applications
1960

Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

PET Polyethylene terephthalate FDM A high filler density allows High compression strength Composites with lattice Vijayakumar et al. (2022)
glycol/carbon fiber the composite to withstand structure
higher loads
Polyethylene terephthalate FDM Rigid carbon fibers signifi- High compression strength Composites Mansour et al. (2018)
glycol/carbon fiber cantly enhance the modu-
lus of flexible PETG
Glycol-modified polyethyl- FDM OMMT particles reduce the Rational structural design Aerospace structures and Mahesh et al. (2022)
ene terephthalate glycol IR radiation absorption for high-performance aircraft interior structure
(PETG), short carbon fib- and promote the forma- composites
ers (SCF), and organically tion of hydrogen bonds
modified montmorillonite between SCF and PETG
(OMMT)
Polyethylene terephthalate FDM _ Polyethylene terephthalate Underwater rovers Grigore et al. (2020)
glycol glycol has higher thermal
stability
Polyethylene terephthalate FDM _ _ Optimization of PETG Clarke and Hosseini (2023)
glycol printing parameters
Polyethylene terephthalate FDM Carbon fibers improve com- Excellent friction properties Engineering material Kichloo et al. (2021)
glycol/carbon fiber posite smoothness
Polyethylene terephthalate/ FDM Concept of discrete full _ Materials for engineering Chatham et al. (2019)
Polypropylene (PP)/PP- crystallization is intro- applications
graft-maleic anhydride duced
Polyethylene terephthalate FDM Combination of soft and Excellent biocompatibility, Maxillofacial implants Katschnig et al. (2020)
glycol and thermoplastic hard areas of the PETG/ printability, and mechani-
polyurethane (PETG/TPU) TPU composite contrib- cal properties
utes to impact stability
Dimethyl terephthalate, FDM Molecular arrangement in High glass transition tem- _ Costanzo et al. (2022)
dimethyl isophthalate, the localized region of the perature
ethylene glycol, and weld is frozen during the
1,4-cyclohexanedime­ glass transition
ethano,
Silver nanowire and polyeth- Laser marking and heat Silver nanowire mesh pat- High EM shielding effi- EMI shielding devices Gu et al. (2020)
ylene glycol terephthalate press tern can improve the light ciency
transmittance
Polyethylene terephthalate FDM Sepiolite has an anisotropic Introduction of seafoam to Printed materials Kim et al. (2020a)
glycol/sepiolite arrangement in the print increase tensile properties
direction
Graphene sheet/Polyethylene FDM Interfacial interaction High thermal stability Airplane interior compo- Bedi et al. (2023)
terephthalate glycol between graphene and nents and minor automo-
PETG plays an important bile parts
role in enhancing thermal
stability
Environmental Chemistry Letters (2024) 22:1929–1987
Table 3  (continued)
Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Polyethylene terephthalate FDM CF enhances the machina- Excellent workability _ Vallejo et al. (2023)
glycol/carbon fiber bility properties of
composites
Cellulose nanocrystal, DIW Photoinitiator (Irgacure High print accuracy Artificial meniscus Zhang et al. (2019c)
phenyl acrylate, and soft 2959) initiates the cross-
acrylamide linking reaction under UV
irradiation
PA Maleic anhydride grafted FDM Both POE-g-MAH and PS Improved shape stability of PA6-based filament Jia et al. (2017)
poly (ethylene 1-octene) acted as amorphous phases composites
(POE-g-MAH)/nylon 6 in the blends, reducing the
shrinkage stress
Nylon 12 SLS _ _ Apparel-related industries Beecroft (2019)
Basalt fiber/polyamide FDM Incorporation of BF resulted Incorporation of BF FDM printing filament Hua et al. (2023)
Environmental Chemistry Letters (2024) 22:1929–1987

in an increase in tensile increases the adhesion

modulus, tensile strength, between the composite
and specific energy layers
absorption per unit volume
of the composite without
sacrificing ductility
Polyamide/boron nitride FDM Orientation of BN in the Excellent thermal conduc- High thermal conductivity Geng et al. (2019)
(BN) matrix parallel to the tivity materials
direction of the wearing
surface favors heat transfer
Continuous carbon fiber/ FDM _ Excellent mechanical Metamaterials Chen et al. (2021a)
polyamide and short car- properties
bon fiber/PA filaments
Multi-walled carbon nano- FDM Multi-wall carbon nanotubes Good mechanical, thermal, Joule-heating devices, Vidakis et al. (2022)
tubes/Nylon 12 improve thermal properties and electrical conductivity flexible conductors, and
of composites and have anti-static enclosures
electrical conductivity
Graphene oxide (GO)/poly- SLS Alcohol functional groups Conductivity Metal-free electrostatic De Leon et al. (2018)
amide on the basal surface and motor
carboxylic acid/car-
boxylates along the edges
increase the dispersion
of GO
Carbon fiber/PA/carbonyl SLS Strong interfacial polariza- Strong microwave absorp- wearable functional devices Gong et al. (2021)
iron tion increases the dielec- tion and military stealth protec-
tric constant tion
Carbon fiber/PA and glass FDM _ _ Composites for outdoor Chabaud et al. (2019)
fiber/PA applications
1961
Table 3  (continued)
1962

Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Carbon nanotube (CNT)/ DIW Introduction of CNT gives Hydrophilic, high absorp- Solar vapor generator Liu et al. (2023a)
PAN the printed structure excel- tion and evaporation rates
lent light absorption and
photothermal properties
PAN PAN-copolymer FDW Synthesis of solketal A capacitance of up to 387 Energy storage devices Usselmann et al. (2022)
acrylate (SKA) and the mF ­cm−2
subsequent copolymeriza-
tion with acrylonitrile
Methylammonium lead One-step electrohydrody- PAN imparts printing prop- Excellent optoelectronic Flexible display applications Kang et al. (2022)
bromide/polyacryloni- namic jet-printing erties to the composite, properties
trile ­(MAPbBr3/PAN) and ­TiO2 or TiC enhances
composite the material’s battery
performance
PVA, PAN, and _ Nano-fillers ­(TiO2 or TiC) to High battery efficiency Printable battery materials Venkatesan et al. (2015)
poly(acrylonitrile-co-viny- improve the performance
lacetate) (PAN-VA) of the printable electrolyte
Glass Fiber/Polypropylene FDM Glass fibers enhance the Ability to reduce stress Bone healing Kabiri et al. (2021)
(GF/PP) mechanical properties shielding and strong load-
of PP carrying capacity
PP Continuous carbon fiber- FDM (coaxial extrusion CCF enhances the mechani- Strong mechanical proper- Low-cost printable com- Zhang et al. (2023b)
reinforced polypropylene process) cal properties of PP ties posites
(CCF/PP)
Carbon black-filled polypro- FDM Introduction of dissipative Excellent wave-absorbing Metamaterial absorber Tan et al. (2023)
pylene (PP) materials for radiation- efficiency
absorption conversion and
optimization of dispersion
characteristics to improve
absorption performance
Polypropylene powder Layer-by-layer printing _ Excellent self-clearing and Ultra-thin conformable PP Greenbank and Ebel (2023)
breakdown performance capacitors, multi-compo-
nent sandwich nanocom-
posite capacitors, and
multilayer PP capacitors
SiO2 nanoparticles/PP FDM _ Improved mechanical and 3D printing engineering Vidakis et al. (2021)
thermo-mechanical prop- applications
erties of raw materials
PP/organoclay FDM Modification reaction of Incorporation of nanoclay Engineering materials Aumnate et al. (2019)
nano clay by dioctadecyl facilitates printing
dimethyl ammonium
chloride
PP/geopolymer mortars A custom-made 3D-printing _ Enhanced shape retention Building materials Nematollahi et al. (2018)
test device and fracture strength
Environmental Chemistry Letters (2024) 22:1929–1987
Table 3  (continued)
Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Bamboo fiber reinforced PP/ FDM Maleic acidification-modi- Composites have good Alternative materials to Long et al. (2019)
poly(lactic acid) fied PP increases bonding toughness PLA
capacity between fiber and
matrix
Chitosan (CS) and PVA DIW Genipin was added into Sustainable drug release Tissue regeneration Liu et al. (2021b)
the CS/PVA solution for behavior
crosslinking with CS to
obtain the pre-crosslinked
hydrogels
PVA Cellulose acetate, PVA, and DIW _ Super hydrophilic and Oil/water separation appli- Li et al. (2020)
silica nano-particles (­ SiO2 underwater superhydro- cation
NPs) phobic properties
Polyvinyl alcohol (PVA)/ DIW Incorporation of bacterial Good bio-compatibility Bone tissue engineering Aki et al. (2020)
Environmental Chemistry Letters (2024) 22:1929–1987

Hexagonal boron nitride/ cellulose gives the com-

Bacterial Cellulose posite a porous organiza-
tion
Polyetheretherketone SLS Graphene can adsorb PEEK Excellent mechanical prop- Tissue repair applications Feng et al. (2020)
(PEEK) and PVA and form hydrogen bonds erties and biocompatibility
with PVA to increase the
compatibility properties of
the material
PVA hydrogels DIW Cross-linking reaction of Excellent lipophilicity Bioprinting Zeng et al. (2023a)
glutaraldehyde with PVA
hydrogels
(PVA)/graphene nanoplate FDM Incorporation of glycerol Electromagnetic interference Composites in the electro- Yang et al. (2020)
(GNP) and GNP enhances the shielding magnetic shielding field
processing characteristics
of the composites
Gelatin/PVA DIW PVA enhances the mechani- Strong mechanical proper- Biological scaffolds in the Kim et al. (2018)
cal stability of gelatin ties and facilitates cell field of tissue regeneration
adhesion and proliferation
PVA DIW Physical bonds were intro- Excellent mechanical Soft devices Li et al. (2019)
duced in PVA by doping properties
complexes to increase the
mechanical properties of
hydrogels
Cellulose nanocrystal/PVA FDM Cellulose nanocrystal Excellent mechanical Printable composites Cataldi et al. (2018)
increases the thermal and properties
mechanical properties of
the composite
PVA and Kevlar nanofiber DIW Highly effective hemostasis Aerogel gauzes for hemosta- Yang et al. (2023)
sis applications
1963
Table 3  (continued)
1964

Fiber type Printing formulations Printing techniques Related mechanisms Function Proposed application Ref

Detonation nanodiamonds Layer-by-layer manufactur- A special physical bond can Excellent mechanical Bio-composites Angjellari et al. (2017)
(DND) and PVA ing be formed between DND properties
and PVA to enhance the
mechanical properties of
the material
PVA hydrogel, a printed A PCB printer PVA-based hydrogel elec- Excellent tensile strain All-printed wearable bioel- Kim et al. (2023)
planar gate electrode, trolytes properties ectronics
and, a printed planar gate
electrode
PVA-containing drugs FDM _ Drug release function Biorelevant media Goyanes et al. (2016)
A novel crosslinked polyvi- FDM _ Hydrophilic expansion Personalized bio-integrating Boyer et al. (2019)
nyl alcohol stents for use in biliary
procedures
PVA FDM PVA is resistant to acids Delayed release of drug or Personalized drug delivery Matijašić et al. (2019)
release of both drugs
Poly(lactic acid), PVC, FDM _ Excellent mechanical Smart thermoplastic materi- Kumar et al. (2019)
wood dust, and magnetite properties als
­(Fe3O4)
PVC Poly(vinyl chloride-co-butyl FDM Copolymers obtained by _ Printable materials Calafel et al. (2018)
acrylate) and poly(vinyl single electron transfer-
chloride-co-2-ethylhexyl degenerative chain transfer
acrylate copolymers living radical polymeriza-
tion
PVC highly loaded with FDM _ Excellent performance in Solid contact reference Lewenstam et al. (2019)
dicalcium chloride acid–base titration electrodes (SCREs)
PVC/diisononyl phthalate FDM Diisononyl phthalate doping Printed structures are flex- Flexible materials Calafel et al. (2020)
gives PVC good printing ible
characteristics at high
temperatures
Ethylene–vinyl acetate-gly- FDM Chemical reaction of EVM- High impact strength and Printable composites Lyu et al. (2020)
cidyl methacrylate (EVM- GMA with polylactic acid smooth surface
GMA) random terpolymer,
PVC, and PLA
Polycaprolactone/Polyvinyl FDM PVC/PCL complexes are PCL increases the mechani- Printable composites Rahmatabadi et al. (2023)
chloride (PCL/PVC) compatible due to polymer cal and printability proper-
compatibility and strong ties of composites and also
interactions has a shape-memory effect
The table presents key findings on research regarding 3D printed synthetic fibers, covering formulation, manufacturing techniques, mechanisms, properties, and application areas. This compre-
hensive summary organizes common applications of 3D-printed synthetic fibers, highlighting the effectiveness of physical fillers and chemical modifications in enhancing their properties. These
studies offer valuable insights to drive the advancement of high-performance materials
Environmental Chemistry Letters (2024) 22:1929–1987
Environmental Chemistry Letters (2024) 22:1929–1987 1965

distribution of soft or hard segments of molecular chains, challenge, especially in the high-value-added application
physicochemical cross-linking points, and molecular field, despite various technological developments related
switches. Synthetic materials-based 4D printing has proven to textile waste treatment. Blended fabrics and the use of
applications in smart alarms, multi-response systems, and different dyes in textile products pose challenges in terms
engineering. However, there is still a lack of practical-ori- of extraction and purification, making cost-effective recy-
ented and innovative applications. Advances in AM tech- cling processes and high-value-added applications dif-
nologies, material design processes, integration of different ficult. Consequently, there is a pressing need to develop
field technologies, and innovative applications are expected sustainable closed-loop and efficient recycling technolo-
to drive 4D-printed composites to new heights in the future. gies for handling textile waste. This section provides a
Currently, there is a significant demand for 4D-printed summary of recycling methods for textile waste, with a
synthetic fiber composites in terms of high toughness, fast focus on cotton fabrics and PET as examples. Addition-
response, multi-response, self-healing capability, biocom- ally, we reviewed the research on textile waste materials
patible properties, high driving force, high reliability and in additive manufacturing.
stability, flexible programming, and sustainability. These
aspects will shape future development. While 4D-printed Methods to recycle textile waste
synthetic fiber composites have found applications in flexible
electronics, bio-engineering, tissue engineering, aerospace, Recycling of natural fibers
and smart building equipment, research in many areas is
still in its early stages. The integration of technology and In recent years, renewable resources have seen a significant
materials design from multiple fields will enable synthetic increase in demand and interest. As a result, many compa-
materials-based 4D printing to meet the application needs nies are now prioritizing the development of natural fiber
of various fields. composites to meet environmental policies and the grow-
ing need for sustainable advanced materials. Owing to the
maturity of natural fiber extraction and processing, natural
Textile waste in additive manufacturing fibers have a price advantage, the price is only one-third
or less than that of glass fibers (Faruk et al. 2014). Cotton
In 2015, the United Nations established a significant goal fiber is an important textile raw material, occupying 24%
titled “Transforming our world: the 2030 Agenda for of the total textile fiber. Cotton waste contains both low-
Sustainable Development”. This goal focuses on achiev- cost and high-value cellulose, green sustainable recycling
ing sustainable development by addressing the interplay technologies and innovative applications will be key to the
between societies, economies, and the natural environ- effective use of cotton waste. Recycling methods for cotton
ment. Unfortunately, current statistics indicate that only fibers include mechanical, chemical, and biological strate-
a few countries are making sufficient progress to meet gies. Mechanical recycling can be achieved by loosening
this goal within the given timeframe (Arora and Mishra or tearing textile waste and re-spinning it with other fibers
2019; Sachs et al. 2021). Textile industry currently has for new products or fiber-reinforced composites. However,
a large output and rapid iteration speed, but this results mechanical recycling makes it difficult to separate cotton
in pressing issue of textile waste disposal (Nayak et al. fibers from blended fabrics effectively. Recycled cotton short
2023). The textile industry plays an important role in the fibers often have problems, such as uneven length and open-
national economy, clothing and textiles contributed 6% to ing, not conducive to independent spinning. Cotton waste
world manufactured goods (Juanga-Labayen et al. 2022; has deficiencies and limitations that affect its use in recy-
Xonkeldiyeva 2021). The global consumption of textiles cled value-added products. Chemical pre-treatment of cot-
has increased by 400% compared to 20 years ago, lead- ton wastes can bring back their application potential (Rizal
ing to a projected amount of 134 million tons of global et al. 2021). Common chemical recovery methods are that
textile waste by 2030 (Jia et al. 2020; Kerr and Landry dissolved and separated waste cotton fabric from the blended
2017). The production of synthetic fibers alone consumes textiles, which can be applied in wet spinning, film prepara-
a staggering 98 million tons of oil, resulting in carbon tion and functional materials development, contributing to
emissions exceeding 1.7 billion tons, and consuming 79 high value-added and practical applications (De Silva and
billion ­m3 of fresh water (Desore and Narula 2018; Her- Byrne 2017; Haslinger et al. 2019; Liu et al. 2021c; Ma et al.
rmann 2017). Furthermore, an alarming $183 million 2018, 2019; Mu et al. 2021; Qin et al. 2020; Sun et al. 2021;
worth of textiles are disposed of in landfills annually Wang et al. 2022a; Zhou and Wang 2021). Cotton waste can
(Wrap 2020). These statistics highlight the unprecedented be converted into environmentally friendly and renewable
challenges faced by the textile industry in terms of sus- biofuels through biochemical or thermochemical processes.
tainability. Effective reuse of textile waste is still a big It also can be transformed into bioethanol and methane by
1966 Environmental Chemistry Letters (2024) 22:1929–1987

fermentation technology or biochar by carbonization, giving has advantages in terms of fabric separation, dye separation,
rise to clean treatment of cotton wastes (Osman et al. 2021). and recovered products.
However, biological recycling methods still face some chal- Chemical recovery methods generally use some chemi-
lenges of low biofuel conversion rates, and higher recycling cal reagents to break the hydrogen bonds of cellulose and
costs (Hanoğlu et al. 2019). In contrast, chemical recycling mainly include purification and separation techniques
such as decolorization and dissolution (Niazi et al. 2021).
 Environmental Chemistry Letters (2024) 22:1929–1987 1967

◂Fig. 11  Synthetic fiber-based 4D printed structures and their defor- non-5-enium acetate ([DBNH]OAc) are also viable for sep-
mation mechanisms. a, b Introduction of π–π stacking and synergistic arating and recovering cellulose from polyester/cotton fab-
crosslinking units into poly(ethylene terephthalate) to improve self-
healing, shape memory, and flame retardant properties. a Reprinted
ric or PET/cotton fabric blends (De Silva and Byrne 2017;
with permission of RSC from the reference (Chen et al. 2019a). Haslinger et al. 2019; Mu et al. 2021; Sun et al. 2021). It
Shape memory composites are then created using two-phase poly- was found that [AMIM]Cl solution could selectively dis-
mers and chemical cross-linking sites, such as polyamide 6/poly- solve cotton fibers from waste PET/cotton blends and be
propylene acrylic composites (c, d). c Reprinted with permission of
Springer Nature from the reference (Peng et al. 2019). e, f Bilayer
used to prepare high-performance films (Isik et al. 2014). In
structures are developed with the hygroscopic deformation properties short, ionic liquid recycling is not the best option for waste
of polyamide 6, where the incorporation of electrothermal materials fabric disposal due to its high cost and complicated process.
addresses the slow deformation recovery in response to moisture. f Regenerated cellulose obtained by dissolving waste
Reprinted with permission of Wiley from the reference (Le Duigou
et al. 2019). g, h 4D-printed composite layers with simultaneous
denim in NMMO solution has better physical properties
water and heat response are achieved by utilizing heat-shrinkable and moisture absorption than standard Lyell fiber. Further-
and hydrosoluble materials. h Reprinted with permission of Frontiers more, dissolution of textile waste with phosphoric acid is
from the reference (Ren et al. 2021). i, j Electrically stimulated defor- feasible at room temperature, and its solubility increases as
mation properties are realized in 4D printed structures, demonstrated
by the deformation photos of PVC hydrogel jellyfish with electrically
temperature decreases. Thus, phosphoric acid may be an
stimulated response. j reprinted with permission of ACS from the ideal reagent for chemical dissolution and recovery of tex-
reference (Wang et al. 2021b). k Photo-thermal coatings and fillers tile waste due to faster speed, lower cost, and recycling of
enable bilayer structures with thermally responsive deformation to be phosphoric acid with lower secondary pollution (Fan et al.
remotely controlled. l The deformation process of a 4D printed poly-
vinyl alcohol-based composite hydrogel bilayer architecture is dis-
2023a). In addition, many researchers also use other pro-
cussed, showcasing selective actuation with the addition of a photo cesses to achieve high-quality recycling of cotton wastes.
absorbent and corresponding images of the hydrogel. Reprinted with Chen et al. (2019b) carbonized waste cotton in a nitrogen
permission of ACS from the reference (Hua et al. 2020) environment and combined it with latex to form a composite
material with excellent conductivity, which can be used as
Regenerated cellulose retains cellulose’s characteristics and a sensitive and durable flexible wearable sensor. Jiang et al.
offers significant advantages in the textile sector, packag- (2022) developed a colorimetric sensor using cotton as a
ing films, cellulose suspension preparation, and functional carrier for detecting the presence of ­Cu2+ in solution. The
materials (Ding et al. 2018; Liu et al. 2021c; Liu et al. 2019; surface of cotton cloth has good hydrophilicity, making it
Ma et al. 2018; Qin et al. 2020; Sun et al. 2021; Wang et al. very suitable for mutual contact between metal cations and
2022a). Common solvents for dissolution of cotton fib- colorimetric parts, with fast response time, accurate detec-
ers include alkaline/urea aqueous (NaOH/urea) solution, tion, durability, and good mechanical performance compared
hydrosulfuric acid (­ H2SO4) aqueous solution, ionic liquids, to traditional paper sensors. These novel approaches provide
N-methyl morpholine-N-oxide (NMMO), phosphoric acid, important insights and innovative applications for cotton
and so on. Table 4 summarizes the advantages and short- waste recycling.
comings of several major cellulose chemical dissolutions. It
was found that H­ 2SO4 had better solubility, but the stability Recycling synthetic fibers
of cellulose became poor. N, N-Dimethylacetamide/Lithium
Chloride (DMAc/LiCl) system did not require pretreatment An economic-wide assessment has estimated that recycling
and had a higher recovery rate, lower dissolution concen- PET monomers could reduce environmental impacts by 95%
tration, longer dissolution time, or higher dissolution tem- and generate 45% economic benefits (Singh et al. 2021a).
perature (Zhou and Wang 2021). The alkali urea system has Scholars have evaluated the recycling potential of textile fib-
a relatively faster dissolution rate, higher yield, and better ers, including synthetic fibers like PP and PA, which have
thermal stability for regenerated cellulose, leading to obvi- a lower cost compared to raw fiber (Tran et al. 2022). PET
ous advantages in membrane preparation, fiber spinning, and is the most common textile fiber, nearly 70% of all textile
functional materials (Liu et al. 2021c; Liu et al. 2019; Ma fibers. PET has become a mainstream material in the era
et al. 2018; Wang et al. 2022a). However, the dissolution of fast fashion due to its low cost and easy processing. The
conditions of alkali urea system are relatively strict, usually shortened life cycle of PET has led to high growth in PET
requiring low temperatures (around − 12 °C) to obtain high production, with global production expected to reach 100
solubility. million tons by 2030 (Garcia and Robertson 2017; Zhou
Many ionic liquids such as 1-allyl-3-methylimidazolium et al. 2022a). PET waste can be recycled using melt spinning
chloride ([AMIM]Cl), 1-butyl-3-methylimidazolium ace- technology, but the presence of blended fibers, dyes, and
tate ([Bmim]OAc), 1-butyl-3-methylimidazolium chloride other contaminants results in poor PET fiber performance.
([BMIM][Cl]), 1-Methyl-3-methylimidazolium dimethyl Currently, simple and economical fiber separation and con-
phosphate ([MMIM][DMP]), and 1,5-diazabicyclo[4.3.0] taminant elimination processes are extremely lacking. It is
Table 4  Comparison of chemical recycling methods of cellulose
1968

Fabric type Chemical reagents Dissolution conditions Applications Ref

Cotton/Polyethylene terephthalate, 1-butyl-3-methylimidazolium chloride 130 °C, 10 h Recycled cellulose/wool composite Sun et al. (2021)
Wool/Polyethylene terephthalate ([BMIM][Cl]), 1-Methyl-3-meth- material
ylimidazolium dimethyl phosphate
([MMIM][DMP])
Waste cotton 1-allyl-3-methylimidazolium chloride 100 °C Spinning rheology test De Silva and Byrne (2017)
([AMIM]Cl)
Waste cotton Sodium hydroxide (NaOH)/urea 0 °C Heavy metal removal Ma et al. (2018)
Cotton/ Polyethylene terephthalate 1,5-diazabicyclo[4.3.0]non-5-enium 80 °C,1 h Textile fibers Haslinger et al. (2019)
acetate ([DBNH][OAc])
Waste cotton Sulfuric acid ­(H2SO4), NaOH/urea, N,N- 8 min, 8 min, 6 h (80 °C), and 18 h Regenerated films Zhou and Wang (2021)
dimethylacetamide/Lithium chloride (25 °C)
(LiCl/DMAc)
Waste cotton/elastane Sulfuric acid ­(H2SO4), sodium hydrox- 45 min, 45 min, 3–5 days Regenerated films Wang et al. (2022a)
ide (NaOH)/urea, dimethylacetamide/
Lithium chloride LiCl/DMAc
Waste cotton Sodium hydroxide (NaOH)/urea − 12 °C, 2 h Flame retardant, aerogel Qin et al. (2020)
Waste cotton Lithium hydroxide (LiOH)/urea, sodium − 12.5 °C Fiber spinning Liu et al. (2019)
hydroxide (NaOH)/urea
Cotton/ Polyethylene terephthalate 1-allyl-3-methylimidazolium chloride 80 °C, 3 h Cellulose film Mu et al. (2021)
([AMIM]Cl)
Waste cotton Sodium hydroxide (NaOH)/urea − 20 °C, 2 h Solar steam generator Liu et al. (2021c)
Waste denim N-methyl morpholine-N-oxide (NMMO), Constant temperature, vacuum Fiber spinning Haule et al. (2016)
N-propyl gallate
Waste cotton phosphoric acid 4 °C, 24 h Cellulose suspension Ding et al. (2018)
Waste cotton and denim 1-butyl-3-methylimidazolium acetate 80 °C, 30 min Man-made cellulose fibers Ma et al. (2019)
([Bmim]OAc), dimethyl sulfoxide
(DMSO)
Denim waste 2,2,6,6-tetramethyl piperidine-1-oxyl Sodium hypochlorite (NaClO), sodium Colored papers and intelligent packaging Wang et al. (2023a)
(TEMPO) bromide (NaBr), 1 h papers
Woven fabrics 2,2,6,6-tetramethyl piperidine-1-oxyl Sodium hypochlorite (NaClO), sodium Spherical cellulose nanocrystals Vanzetto et al. (2021)
(TEMPO) bromide (NaBr), 20 min
Cotton raw material Sulfuric acid ­(H2SO4) Pre-treatment 4 h, hydrolysis followed by Cellulose nanocrystals Pandi et al. (2021)
ultrasound for 1 h
Waste-colored cotton fibers Sodium hydroxide (NaOH), nitric acid Grinding and 3% NaOH, boiled for 6h, Microcrystalline cellulose Cao et al. (2021)
­(HNO3) and hydrochloric acid (HCl) then added to mixed acid ­(HNO3, HCl)
at 60 °C for 1h
Waste cotton fabrics Phosphotungstic acid (­ H3PW12O40) 130–170 °C, 4–8 h Microcrystalline cellulose Hou et al. (2019)
Cotton liner Sodium hydroxide (NaOH), sulfuric acid NaOH treatment at 80 °C for 5 h, fol- Cellulose nanocrystals Hemmati et al. (2019)
­(H2SO4) lowed by homogenization with ­H2SO4
at room temperature for 3–7 min
Environmental Chemistry Letters (2024) 22:1929–1987
 Environmental Chemistry Letters (2024) 22:1929–1987 1969

difficult to find a balance between economy and fiber perfor-

The table outlines key parameters of the chemical recovery process for cotton waste, detailing the source of cotton waste, chemical reagents, dissolution conditions, and value-added applica-

closer to room temperature and the reaction time is shorter. Consideration should also be given to the cost and recyclability of the chemical solvents used. Furthermore, sustainable and innova-
tions. Due to the high polymerization of cellulose, the dissolution conditions are relatively complex. It is noted that the process becomes more cost-effective when the dissolution temperature is
mance in recycling waste PET using melt spinning, and its

Elmetwaly et al. (2022)

Soleimani et al. (2022)

Mohamed et al. (2021)

widespread application is limited. Generally, PET is chemi-

Jiang et al. (2021b)

Wang et al. (2019)

Fan et al. (2023b)

cally degraded to PET monomers to achieve recycling. Com-
mon methods used to recover chemicals include hydrolysis,
glycolysis, ammonolysis, and so on.
PET is usually found in blends with cotton fibers. The
Ref

separation process is inevitable to obtain pure PET fibers.

Some researchers have chemically recovered cotton fibers
from PET/cotton blended fabrics to obtain pure PET fib-
Cellulose nanocrystals and methyl-

ers, which can then be reused by melting and spinning pure

PET fibers (Haslinger et al. 2019; Mu et al. 2021; Sun et al.
2021). Recycled PET fibers often contain varying degrees
Flexible Supercapacitors

of impurities, causing defects in the processability and

Cellulose nanocrystals

Cellulose nanocrystals

Cellulose nanocrystals
UV protective paper

mechanical properties (Abbasi et al. 2018). Akato et al.

cellulose films

(2018). mixed a high oleic fatty acid into the waste PET as a
Applications

modifier, leading to a relative decrease in melting tempera-

ture, recrystallization temperature, and glass transition tem-
perature of regenerated PET fibers. As a result, the process-
ing characteristics and mechanical properties of PET fibers
were significantly improved. Waste PET can be degraded to
Sodium hydroxide (NaOH), hydrochloric NaOH treatment at 70 °C for 2 h, mixed

NaOH treatment at 80 °C for 3 h, then

­ 2O2, ­H2SO4 treatment at
NaClO treatment for 2 h, ­H2SO4 treat-

tive applications of cellulose from recycled cotton waste are essential to align with future trends and enhance its value

terephthalic acid (TPA)and ethylene glycol (EG) monomers

­ 2SO4) at 65 °C for 5 h

by hydrolysis with acid, alkaline, and neutral reagents. It

was reported that the hydrolysis of PET in alkaline solution
H2SO4 treatment 65 °C, 5 h
ment at 80 °C for 30 min

under microwave irradiation has shortened hydrolysis time,

and reduced cost (Siddiqui et al. 2010).
Dissolution conditions

Calcination 60 min

PET can be hydrolyzed in an alkaline condition, and then

45 °C for 1 min

the PET/cotton mixture can be separated into TPA, cotton,

acid (HCl, H

cleaned in H
60 °C, 30 min

and EG filtrates. The addition of phase transfer catalysts

reduces separation time and cellulose hydrolysis while
increasing yield (Palme et al. 2017). Recyclable phospho-
tungstic acid is used as a catalyst to hydrolyze polyester-
Sodium hydroxide (NaOH), sulfuric acid

cotton blends, degrading the polyester to TPA and the cotton

Sodium hypochlorite (NaClO), sulfuric

to MCC with high yields of 99.77% and 85.12%, respec-

acid (HCl), sulfuric acid ­(H2SO4)

tively. (Ling et al. 2019). For the recycling of PET waste,

a multifunctional plastic hydrolysis process based on poly-
Needling and carbonization

oxometalates has been proposed with a hydrolysis rate of up

to 100%. The recycled PET has been used to produce high-
Sulfuric acid ­(H2SO4)

Sulfuric acid ­(H2SO4)

Chemical reagents

quality metal–organic frameworks that serve as catalysts

acid ­(H2SO4)

for the synthesis of cyclic carbonate compounds, achiev-

ing the transition from plastic waste to new plastic (Chen
­(H2SO4)

et al. 2019c). Zhang et al. (2022b) developed a nonaqueous

hydrolysis method using EG and tetrahydrofuran (THF) as
co-solvents to obtain pure TPA in presence of potassium
hydroxide (KOH). It has mild hydrolysis conditions, high
Cotton fiber and polyester fiber

recovery rate, and high degradation rate. Moreover, this

system can also be used for selective decomposition and
Waste denim and MXene

separation of PET/spandex color blends.

Table 4  (continued)

Waste cotton cloth

Waste cotton cloth

Glycolysis is another low-cost recovery method for PET,

in which the recovered bis (hydroxyethyl) terephthalate
Waste cotton

Cotton fiber
Fabric type

(BHET) monomer can be used directly in PET production.

Glycolysis of PET depends on the catalyst. Mg–Al double
oxide pellets, as a glycolytic catalyst, can cyclically catalyze
1970 Environmental Chemistry Letters (2024) 22:1929–1987

the degradation of PET, but their catalytic performance is environmentally friendly and sustainable. Many researchers
low and the reaction temperature is too high (Guo et al. extracted materials from waste materials, such as natural
2021). Liu et al. (2023b) proposed a high catalytic activ- and synthetic fibers. And they utilized additive manufactur-
ity cobalt single-point catalyst with photothermal function ing to create high-level design products and develop high-
for PET glycolysis catalysis. The catalyst has a high reac- performance printing materials, realizing the transformation
tion permeability and space–time yield of about one order from “waste” to “treasure”.
of magnitude higher than general catalysts. Moreover, the Christophe Guberan and MIT’s self-assembly laboratory
cyanamide-catalyzed PET glycolysis reaction has mild reac- have launched a 3D-printed sports shoe (Fig. 12a). Materials
tion conditions and high BHET yield (Wang et al. 2022b). of various thicknesses and properties are printed onto tense
Abdullah and Ahmad (2013) degraded PET through gly- textiles and then released after printing, allowing the shoe to
colysis and compounded it with modified coconut fibers to deform into pre-programmed shapes. Complexity and labor
obtain composite materials with strong mechanical proper- of shoe production are effectively reduced while combin-
ties. Besides, some researchers have made additional efforts. ing various materials for self-forming and adaptive shoes
Melt-spun waste PET is dissolved in the m-cresol solvent (Christophe Guberan and Carlo Clopath + Self-Assembly
and chemically regenerated onto cotton fibers, improving the Lab 2017). 4D printing provides important insights into
mechanical properties and thermal stability of PET (Sharma reducing manual assembly and adaptive textiles. In 2014,
et al. 2020). The use of melt polycondensation can produce Nervous System Studio created a 3D-printed hinge structure
biocomposites from renewable resources and PET, and its that forms a flexible fabric. The 3D printed fabrics rigid
three-dimensional porous scaffold is conducive to inducing hinge has exquisite structures with a large number of hinged
stem cells to develop osteogenesis and cartilage (Ghosal mechanism links (System 2014).
et al. 2020). PET waste recycling and application research In 2016, the Nervous System presented a dress made
have achieved good results, and the future industrialization of 1600 pieces of rigid nylon. This dress is made of 4D
of the relevant technology will effectively reduce the harm printed petal-shaped hinges, and the length, direction and
caused by textile waste. shape of each unit can be customized separately (Fig. 12b).
The high proportion of cotton and PET in the textile The printed unit underwent a shape change after leaving the
industry makes it the focus of waste recycling. Waste cotton printer to achieve complete assembly of the 3D printer. This
can be enhanced in value and sustainability through biologi- new creative approach involves the earliest application of
cal and chemical recycling, avoiding environmental damage 4D printing, eliminating the assembly process and ensuring
and wasted resources compared to traditional physical incin- fit, the most prominent benefits of AM technology (Jenna
eration and landfilling. The high-quality recycling of PET 2016). Iris van Herpen’s team has revolutionized the fashion
is demonstrated through two main aspects. Firstly, reduc- industry by combining 3D printing technology with recycla-
ing degradation conditions or enhancing monomer yield is ble polyester materials. The team has successfully designed
crucial to minimize recycling costs. Secondly, enhancing dresses that showcase exquisite details and enhanced flex-
the overall performance and functionality of recycled PET ibility (Fig. 12c).
composite materials is essential for achieving high-quality By integrating SLS technology into 3D printing, intricate
PET recycling. Although there are numerous green sustain- details can be added and a high-quality finish is ensured for
able technologies available for textile waste recycling, the the designed structures (Grain 2016). This groundbreaking
low rate of textile waste recycling and the limited innovative work not only contributes to the recycling of textile mate-
application areas still pose challenges. rials but also paves the way for their application in high-
value-added contexts. The Advanced Materials Laboratory
Application of textile waste materials in additive of Edinburgh Napier University collected textile waste,
manufacturing including mixed fiber trim, wool trim, and recycled leather
waste, and mixed it with recyclable materials to prepare
The rapid development of additive manufacturing offers new printable filaments (Fig. 13a). The associated structures can
game changers for broadening the application field of recy- be designed by laser cutting technology or machined into 3D
cled textile waste. Especially 4D printing emerged, deforma- printed jewelry by AM technology (Fig. 13a) (Vettese For-
tion of printing entities as changes in time have produced ster 2017). What is clear is that 3D printing can help more
interesting practical applications. For example, printed two- passionate creators create sustainable new products, which
dimensional patterns can be transformed into preset shapes means “Textile waste + Additive manufacturing” can bring
under external stimuli, effectively reducing installation sustainability, multidimensional design, and high creativity
and assembly labor costs. In contrast to traditional manu- to printed structures.
facturing technologies, AM technology allows for greater Cellulosic materials occupy a high percentage of textile
freedom of design and more complex processing, and it is waste, but their high-value-added applications are usually
Environmental Chemistry Letters (2024) 22:1929–1987 1971

Fig. 12  3D and 4D printing textiles. The on-demand manufactur- printing adds intelligent characteristics to textiles by allowing shape
ing, manufacturing flexibility, and green manufacturing features of changes over time. This expansion of design dimensions effectively
additive manufacturing technology play a crucial role in the design meets the demands of the design space. a Self-assemble shoe (Chris-
and production of new textiles. Specifically, 4D printing technology tophe Guberan and Carlo Clopath + Self-Assembly Lab 2017). b 4D
has introduced innovative design elements by incorporating time as printed dress from 1600 pieces of rigid nylon (Mcknight 2016). c Iris
a dimension. While 3D printing technology enhances textiles with van Herpen’s presentation of “Roots of Rebirth” at Paris Haute Cou-
intricate details and enables the production of complex shapes, 4D ture Week (Grain 2016). All images have been credited to the source

insufficient. Cellulosic waste denim can be extracted by acid Waste PET can be pelletized, screened, and melted to
hydrolysis, modified, and then compounded with recycled obtain 3D-printed filaments (Little et al. 2020). Exconde
PET to produce a composite with excellent toughness (Car- et al. (2019) developed a printing filament by employing a
rete et al. 2021). Ahn et al. (2022) prepared a building speci- cutting, grinding, and extrusion process using PET waste
men using a cylinder injection printer by mixing waste paper collected from coastal areas. Through a multi-criteria deci-
with a ceramic binder. The specimen exhibited uniform sur- sion-making approach, it was determined that post-consumer
face quality and excellent fire resistance, indicating potential PET offers several advantages over virgin PET for 3D print-
in construction applications. ing applications. Recycled PET has a lower degradation
Stolz and Mülhaupt (2020) produced an ink by mixing temperature and 3D printing advantages compared to the
waste paper (WP) with PVA (Fig. 13b), and corresponding original PET (Ferrari et al. 2020). Similarly, 3D-printed
3D-printed structures have good shape stability. Although filaments can also be prepared by adding ground biochar to
the structure is porous, it still has high modulus and ten- PET bottles and melting them. The test results indicated that
sile strength. The mechanical properties, water resistance, the addition of biochar significantly improved the dynamic
and flame retardance of the printed structure were sig- modulus, dimensional stability, and thermal stability of recy-
nificantly improved by glyoxal crosslinking and miner- cled PET (Idrees et al. 2018). Małek et al. (2022) developed
alization (Fig. 13c). Furthermore, the WP/PVA materials a 3D-printed scaffold using recycled PET and incorporated
crosslinked with glyoxal a shape memory effect, allowing it as the internal structure of cement-glass composite bricks.
them to deform in response to heat and water (Fig. 13d). It is important to highlight that the mechanical and thermal
Similarly, waste office paper (WOP) mixed with polylactic properties of the composite bricks can be altered by varying
acid (PLA) can produce printed filaments, and this fila- the shape of the PET bracket. In comparison to traditional
ment is perfect for printing. The addition of pure WOP ceramic materials, the composite brick holder offers ben-
to PLA results in poor mechanical properties. Increasing efits in terms of enhanced durability and improved thermal
the WOP content reduces the cooling crystallization tem- insulation.
perature, leading to a more ordered amorphous structure. Some studies have used filler reinforcement composites
The bonding interface was significantly improved when and physical modification methods to achieve the transfor-
treated with WOP silane coupling agent, resulting in mation of landfill waste into functional materials. PA6 can
strong mechanical properties (Tao et al. 2021). Although be recycled using a twin-screw extruder to produce print-
cotton textile waste contains higher-quality cellulose than able filaments that exhibit excellent physical and mechani-
other sources, the complex and expensive extraction pro- cal properties. The inclusion of small amounts of acryloni-
cess limits its widespread use. Efficient, cost-effective, and trile butadiene styrene (ABS) and titanium dioxide (­ TiO2)
applicable green recycling processes will be a hot topic for in the filaments enhanced printing performance (Farina
textile waste recycling in the future. et al. 2019). Cellulose collected from waste materials such
as paper, cardboard, and wood powder can be mixed and
1972 Environmental Chemistry Letters (2024) 22:1929–1987

Fig. 13  3D printing technology is utilized to recycle textile waste properties into textile waste represents a significant advancement in
through green recycling processes and physicochemical modifica- the “Textile waste + Additive manufacturing” strategy, enabling the
tion processes, enhancing the functional properties and performance production of 4D-printed devices tailored for real-world applications.
of the materials. This approach allows for the creation of 3D-printed For instance, a wet-responsive metamaterial is developed using con-
filaments that can be laser cut and used in jewelry structures (a). tinuous flax fiber impregnated with a polymer matrix as the active
Reprinted the reference (Vettese Forster 2017) with open access layer and a polymer matrix as the passive layer, resulting in a struc-
Creative Commons CCBY license. Moreover, cellulose derived from ture that deforms in response to water, as shown in (e, f). By adjust-
waste sources can be 3D printed to exhibit exceptional mechanical, ing the distance of the filaments, the metamaterial can exhibit vary-
flame retardant, and shape memory properties, as illustrated in (b–d). ing deformations upon water immersion (g), facilitating the design of
Reprinted from the reference (Stolz and Mülhaupt 2020) with open flexible hinges with a deformation process (h). Reprinted with per-
access Creative Commons CCBY license. The integration of smart mission of Elsevier from the reference (Le Duigou et al. 2021)

melted with recyclable PP to form printable filaments. improvement in storage modulus and elastic modulus when
The obtained 3D-printed structures showed a significant cellulose was added (Zander et al. 2019b).
Environmental Chemistry Letters (2024) 22:1929–1987 1973

Crop rice straw husks can be blended with recycled PP to by layer height in the passive layer (LHp), and the reac-
make 3D-printed filaments. The addition of fibers relieved tion rate could be adjusted by interfilament distance (IDp).
the warpage of PP and the presence of lignin led to faster From the distribution of different IDp in the CFF of the CFF/
degradation. The fibers may act as nucleation sites increas- PBS active layer as shown in Fig. 13g, the printed structure
ing the crystallinity, and printing grating angle change can achieved controllable wet response deformation in the X
adjust the mechanical properties, showing the potential of and Y directions. The printed sample underwent complex
customizable parts (Morales et al. 2021). Chong et al. (2020) geometric motion with gradient curvature along the length
produced a 3D printing filament by introducing different and width directions, as well as the temporal evolution of
components of coconut waste activated carbon (AC) into the order. The 4D printing hinge was designed based on the
recycled high-density polyethylene (HPDE) and PP. The above principles, and the wet-response driving process is
addition of AC increased the thermal stability of the com- shown in Fig. 13h. Its motion can be precisely controlled
posite, while the crystallinity decreased, resulting in a fine by adjusting IDp. This research not only provides insights
and uniform filament surface. The elongation at break of into the development of wet actuators using natural fibers
HDPE/PP at 8% AC content was almost ten times higher but also suggests ideas for the development of advanced 4D
than that of composites without AC. Similarly, a 3D-printed printing components using textile waste. By utilizing high-
filament was developed by collecting HDPE (r-HDPE) and quality textile waste materials, it is possible to explore vari-
PP (r-PP) waste plastics from an ocean shore. ous applications such as 4D printing textile structures, wet
Hot cracking agricultural biochar enhanced the r-HDPE/r- actuators, supramolecular materials, advanced composites,
PP composite material, improved Young’s modulus and and flexible electronics. These contributions are significant
bending modulus, and solved the warping problem of print- for the future of 4D printing materials.
ing materials (Maldonado-García et al. 2021). The printed In the area of cellulose recycling, researchers have
filaments formed by glass fiber-reinforced recycled PP fibers successfully separated and extracted cellulose from waste
can print objects with high dimensional accuracy and good and converted it into high-value-added products. This
surface quality (Zhang et al. 2023a). Zander et al. (2019a) concept of “waste to treasure” aligns with the current
prepared 3D-printed filaments by blending PET, PP plastic development trend. However, there are still challenges
waste bottles, and polystyrene (PS). Adding styrene-ethyl- in obtaining high-quality post-consumer cotton through
ene-butylene-styrene (SEBS) as a bulking agent to increase existing processes. A single recycling process is insuf-
the glass transition temperature. Regenerated PET has the ficient to achieve separation and recycling of diversified
highest ultimate tensile strength and filler contributes to a post-consumer cotton textiles. Furthermore, the diffi-
great improvement of PET extensibility because of the inter- culty in obtaining high-quality regenerated cellulose is
action between SEBS and PET molecular chains. Compared compounded by dyeing and multi-fiber blending. The
to the pure regenerated PET and PS, the elongation at the recycling of synthetic fibers can enhance their compre-
break of co-blended composites showed different degrees of hensive performance through the use of fillers and com-
improvement. The incompatible r-PP/r-PET exhibited poor posite processes, thereby improving their competitive-
interfacial bonding from SEM images of the bonding inter- ness. Synthetic fiber waste can also be processed as a
faces of the differently formulated composites (PP/PET, PP/ potential alternative for 3D printing, offering low-cost,
PET SEBS). Advances in material design techniques have high-performance materials. However, it is worth noting
resulted in superior performance of waste-derived textile that while there have been many feasibility studies on
materials while providing AM with a potentially low-cost recycled waste materials in the field of 3D printing, most
alternative to printed materials. of them do not involve textile waste materials. Therefore,
Currently, research on 4D printing of textiles waste is the integration of textile waste with 3D printing technol-
relatively rare. As summarized in Chapter 4, textile materi- ogy is still lacking in terms of advancements. Addition-
als have the potential to become 4D printed materials. Tex- ally, the flexibility and intelligence of 4D printing com-
tile waste can also be used to design intelligent structures ponents have brought about significant changes, offering
through recycling and purification processes. Le Duigou more possibilities for the high-value-added reuse of tex-
et al. (2021) developed a 4D printing metamaterial struc- tile waste.
ture by impregnating PLA and soft polybutylene succinate
(PBS) with continuous flax fiber (CFF) (Fig. 13e). The
asymmetric structure has a faster response speed compared Perspective
to short fiber reinforcement. In addition, the response rate
and reaction displacement index of CFF/PBS composites Although the advantages of the “Textile waste + Additive
are faster and greater than CFF/PLA (Fig. 13f). The shape manufacturing” concept have been demonstrated, there are
change curvature of the printed structure could be controlled still obstacles in the transition from the concept to market
1974 Environmental Chemistry Letters (2024) 22:1929–1987

application. The major challenges include textile waste trans- Additionally, scientific chemical purification technology,
formed into the printed formulation, AM of printed formula- advanced decomposition methods, and well-designed print-
tion, commercialization, and marketing. These challenges ing materials are crucial for reducing production costs and
can be addressed through technological advances, material improving product reliability. This strategy is still some
innovations, as well as multidisciplinary convergence of challenges away from practical application. We venture to
relevant development trends. Therefore, textile waste-based speculate that practical applications related to this strategy
new materials are sustainable without significantly increas- will emerge around 2030, and gradually increase in 2035.
ing recycling costs. The “Textile waste + Additive manufacturing” strategy
There are several challenges in the process of converting aims to reuse textile waste and develop high-performance
textile waste into printable materials. Firstly, textile waste products empowered by the high-precision and material
typically contains various materials and dye additives, mak- design of AM technology. However, consumers subcon-
ing it difficult to separate and purify using current technolo- sciously perceived this strategy as being related to “shoddy”.
gies, and posing challenges in terms of process feasibility Although the material source of this strategy is waste, in
and sustainability. Secondly, the extracted components from complete contrast to “shoddy”, AM especially 4D print-
textile waste are not directly printable, and printing formula- ing has specific technique that can describe these products
tions need to meet the specific printing requirement. Find- as “luxury”. The “Textile waste + Additive manufactur-
ing the right formulations and printing processes to achieve ing” strategy faces several challenges in terms of market-
printable materials based on textile wastes is a challenge. ability, despite its potential for widespread development in
Lastly, textile waste-based printable formulations should be the future. Creating a market environment in this field and
environmentally, energy-saving, and economically sustain- promoting the “Textile waste + Additive manufacturing”
able. Fortunately, research on clean recycling, purification development-related industries require government policy
and separation, and the design of printed materials is gradu- guidance and support, branding leading, technology, and
ally deepening. The breakthrough in high-performance and economic support.
sustainable printing materials preparation technology will Additive manufacturing, as a clean, efficient, and precise
entail deep changes in the future. advanced manufacturing process, has become a desirable
Current computer-aided design (CAD) has greatly facili- means of textile materials recycling. Surveys have shown
tated the models of manufactured structures, and informa- that reusing 75% of textile waste can save 4.2 trillion liters
tion communication makes creation of digital less difficult. of fresh water, reduce 17 million tons of C ­ O2 emissions,
However, AM technology lacks industry standards and there conserve 75,000 ­m3 land space, and generate numerous
is a weak awareness of intellectual property protection for employment opportunities (Chavan RB 2014). With the
modeling and other rights, which is detrimental to the inno- establishment of the concept of sustainable development and
vative development of firms. The scope of customizability green production, this direction is anticipated, and we envis-
has been further expanded, posing new challenges for enter- age perspectives of research, development, and application
prises to meet market requirements. In addition, AM cur- in the future (Fig. 14). With the increase of environmental
rently has the disadvantages of expensive equipment cost, protection awareness and the deepening of sustainable goals,
low manufacturing precision and efficiency, low product the development of textile waste-based products is gradually
strength, and so on (Zhang et al. 2022a). With the continu- accepted, and the recognition of relevant products will grad-
ous innovation of technology and the application of new ually increase. Textile waste recycling requires government
materials, these disadvantages will be gradually improved. leadership, policy, technical, and economic support, and
“Textile waste + Additive manufacturing” strategy offers brand-led and multi-party collaboration. For the sustainable
personalized product services to consumers, streamlining the development of textile industry in the future, the establish-
product design process and on-demand production making it ment of a green and sustainable development framework and
more profitable. However, stable continuous supply the clas- the promotion of recycling concept are both necessary. At
sification management of textile wastes, and the market com- the technological level, physicochemical recycling methods,
petitiveness of products based on textile waste are important sorting devices, and preparation processes for low-cost and
factors that impact these firms’ operations. The varying qual- high-performance printing materials will advance the textile
ity and variety of textile waste significantly affect product industry towards green and intelligent. In previous reports,
performance, manufacturing costs, and product reliabil- some scholars have recycled textile-related wastes and given
ity, posing challenges to companies in controlling product these materials “luxury” properties, including material per-
quality, reducing recycling costs, and enhancing product formance, functionality, and fine design. AM can give textile
reliability. Efficient textile material identification, sorting wastes multi-dimensional design and new creative elements,
devices, and separation technology can greatly minimize while these waste materials are sustainable and competitive.
the labor required for waste classification and management. In the future, innovative works developed from 3 and 4D
Environmental Chemistry Letters (2024) 22:1929–1987 1975

Fig. 14  Perspectives of using textile waste and additive manufactur- through this strategy, opportunities arise for advancing smart wear-
ing. This approach relies on raising environmental consciousness, able technology, functional textiles, flexible electronics, biomaterials,
receiving government backing, fostering technological advancements, metamaterials with intricate structures, flexible robotics, and human–
and securing economic support. By leveraging low-cost textile waste machine interaction

printing of all textile wastes will have potential applications multi-material composite, and have a broad development
in functional textiles, flexible electronics, and smart wear- prospect in the field of biomedicine and tissue engineering.
able devices. Synthetic fibers have good processing flexibility in 4D print-
With the advantages of low cost, wide source, and high ing field. Synthetic fibers can bring together shape memory
performance becoming more apparent, we predict contin- and improved mechanical properties, which would facilitate
ued growth in the production and usage of textile natural the design and application of new intelligent structures, pro-
fibers as a sustainable technologies material for addressing viding new development opportunities for functional compo-
global challenges. The main components of textile natural nents, soft robotics, flexible electronics, intelligent devices,
fibers include cellulose and protein. Cellulose has excellent human–computer interaction, and medical applications.
biological affinity and sustainability, and a large number of 4D printing is a highly integrated multidisciplinary tech-
hydrogen bonds facilitate the integration of multiple materi- nology that will be groundbreaking in the future. Especially,
als, giving it additional advantages in composites, hydrogels, recent 5D printing concept has been derived from the addi-
fibrous materials, and thin films (Li et al. 2021b). Integrat- tion of information dimensions to 4D printed smart struc-
ing mechanical, optical, thermal, rheological, and intelligent tures, which can respond to positive changes in the environ-
response properties would make it promising for smart man- ment and has unprecedented potential (Lai and Wang 2023).
ufacturing. In addition, the widespread commercialization of Various functional fillers and composite processes enable
cellulose may become a promising sustainable technological materials to have functionality and intelligent response per-
material in the future. Due to good biocompatibility and formance. Structure design through digital modeling can
mechanical properties, protein-based fibers have great poten- meet application requirements. High-precision printing
tial in composites, biomaterials, flexible electronics, and so technique gives precise manufacturing of material dosage
on. The industrialization and sustainability of protein-based (or type) and micro-nano scale. Modern analysis technol-
materials are expected to be promoted by modification, and ogy, such as finite element analysis, machine learning, can
1976 Environmental Chemistry Letters (2024) 22:1929–1987

achieve the prediction and analysis of function and intel- self-generating components, and sensors, and so on. Ani-
ligence, especially in inverse problem-solving. Therefore, mal fibers, such as silk and wool, show great promise in
multidisciplinary integration can effectively realize the the biomedical field due to their bioactivity. The customiz-
design of new intelligent components in multiple dimen- able advantages offered by additive manufacturing tech-
sions, which is conducive to the application of “Textile nology further expand its application potential. Synthetic
waste + Additive manufacturing” strategy in the fields of fibers can achieve better printability, and mechanical and
wearable, microelectronics, flexible robotics, smart devices, functional properties, mainly through multi-material com-
artificial intelligence, and so on. posites or modified treatments. The combination of textile
Based on the above perspective, the future of the “Textile materials with 4D printing technology not only obtains
waste + Additive manufacturing” strategy is worth envision- smart responsiveness, but also integrates other features
ing. The achievement of “waste” transformed into “luxury” like conductivity, flame retardancy, and biocompatibility.
will not be a fantasy for textile waste, relying on AM tech- The low-cost and sustainable recycling processes for tex-
nology and combining it with innovative material design. tile waste provide an affordable material source for “Tex-
With the breakthrough of 4D even 5D printing technology, tile waste + Additive manufacturing” strategy, ensuring
textile waste will be endowed with smart response and inter- its future viability. Furthermore, numerous companies
action features, including color change, deformation, and and researchers have already recognized the potential in
information exchange, which would further promote the this field, and the “Textile waste + Additive manufactur-
application of textile wastes in high-end fields. In the future, ing” strategy is already showing signs of development.
the vision of the “Textile waste + Additive manufacturing” The transformation of textile waste into printed formu-
strategy would have a green, smart, and advanced picture. lations has a positive impact on the environment. “Tex-
tile waste + Additive manufacturing” strategy aims to
advance textile waste recycling and promote high-value-
Conclusion added applications. Such a framework and ethos would
ultimately promote textile industry to enter a circular
The development of textile industry is accompanied by economy that is ecologically conscious and sustainable.
issues such as the consumption of freshwater, petroleum Additive manufacturing technology, particularly 4D print-
resources and energy, land occupation, marine pollution, ing can introduce innovative technological advancements
carbon emissions, and discharge of wastewater, which are to the field of textile engineering, creating exciting future
serious obstacles to the United Nations Sustainable Devel- development prospects.
opment Goals (SDGs). Additive manufacturing technology
is considered a new game changer in textile waste recy-
Author contributions Weiqiang Fan: Conceptualization, Methodol-
cling and application, playing a crucial role in sustainable ogy, Writing—Original draft preparation, Writing—Review & Edit-
development of textile industry and offering innovative ing, Investigation. Yongzhen Wang: Data curation, Writing—Review &
solutions to expand the application areas and enhance Editing, Supervision, Project administration. Rulin Liu: Visualization,
the value of textile waste. Furthermore, it is essential to Investigation. Jing Zou: Methodology, Investigation. Xiang Yu: Inves-
tigation. Yaming Liu: Supervision. Chao Zhi: Supervision. Jiaguang
explore the potential of 4D printing technology in textile Meng: Supervision.
materials to further enhance the functional and intelligent
features. Based on above background, the strategy of “Tex- Funding This work was supported by National Natural Science Foun-
tile waste + Additive manufacturing” was proposed, which dation of China [52103066, 51903199] and; Young Talent Fund of
Association for Science and Technology in Shaanxi, China (20230430).
would be a promising method for textile waste disposal. Natural Science Basic Research Program of Shaanxi [2021JQ-678,
The development characteristics, trends, research status, 2021JQ-667]; and Science and Technology Guiding Project of China
and challenges of additive manufacturing technology indi- National Textile and Apparel Council [2020042]. Innovation Capabil-
cate that it is a future-oriented advanced manufacturing ity Support Program of Shaanxi [2022KJXX-40]. Key Research and
Development Program of Shaanxi [2023-YBGY-490].
technology, that promotes green and intelligent manu-
facturing especially. Textile materials can be used in the Declarations
AM field due to their advantages of excellent performance
and broad sources. Cellulose materials can be modified Conflict of interest The authors declare that they have no known com-
by doping cross-linker or anisotropic arrangement to peting financial interests or personal relationships that could have ap-
peared to influence the work reported in this paper.
construct high-performance materials. The presence of
numerous active functional groups in cellulose molecular Consent for publication All authors agree to publish this article in
chains allows for modification, functionalization, and the Environmental Chemistry Letters.
printed components have broad application prospects in
various fields such as flexible electronics, biomaterials,
Environmental Chemistry Letters (2024) 22:1929–1987 1977

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