J Mater Sci (2020) 55:829–892

Review
REVIEW

A review of natural fiber composites: properties,

modification and processing techniques,
characterization, applications
Aliakbar Gholampour1 and Togay Ozbakkaloglu2,*

1
Department of Infrastructure Engineering, The University of Melbourne, Melbourne, VIC, Australia
2
Ingram School of Engineering, Texas State University, San Marcos, TX, USA

Received: 17 May 2019 ABSTRACT

Accepted: 4 September 2019 There has been much effort to provide eco-friendly and biodegradable materials for
Published online: the next generation of composite products owing to global environmental concerns
16 September 2019 and increased awareness of renewable green resources. An increase in the use of
natural materials in composites has led to a reduction in greenhouse gas emissions
Ó Springer Science+Business and carbon footprint of composites. In addition to the benefits obtained from green
Media, LLC, part of Springer materials, there are some challenges in working with them, such as poor compati-
Nature 2019 bility between the reinforcing natural fiber and matrix and the relatively high
moisture absorption of natural fibers. Green composites can be a suitable alternative
for petroleum-based materials. However, before this can be accomplished, there are a
number of issues that need to be addressed, including poor interfacial adhesion
between the matrix and natural fibers, moisture absorption, poor fire resistance, low
impact strength, and low durability. Several researchers have studied the properties
of natural fiber composites. These investigations have resulted in the development of
several procedures for modifying natural fibers and resins. To address the increasing
demand to use eco-friendly materials in different applications, an up-do-date review
on natural fiber and resin types and sources, modification and processing tech-
niques, physical and mechanical behaviors, applications, life-cycle assessment, and
other properties of green composites is required to provide a better understanding of
the behavior of green composites. This paper presents such a review based on 322
studies published since 1978.

Introduction The use of environmentally friendly green materials,

which are recyclable, biodegradable, and renewable,
The production of petroleum-based materials and has been recently considered to decrease the envi-
glass fibers results in the release of a significant ronmental impact of petroleum-based materials [2].
amount of greenhouse gases into the atmosphere [1]. Fully green composites are a type of biocomposite

Address correspondence to E-mail: [email protected]

https://doi.org/10.1007/s10853-019-03990-y
830 J Mater Sci (2020) 55:829–892

produced by a combination of biofibers and resins fiber composites. Therefore, to address the increasing
from renewable agricultural and forestry feedstock demand to use eco-friendly materials in different
[1]. This type of composite is disposed of and com- applications, an up-do-date review is required to
posted at the end of their life without harming the allow a better understanding of the behavior of nat-
environment [3]. ural fiber composites manufactured using discontin-
Biofibers have been extensively used as reinforcers uous natural fibers. This paper presents such a
and fillers in composites in recent years [1]. They review based on 322 studies published since 1978.
come from biological origins and are classified into
non-wood fibers (natural fibers) and wood fibers [4].
Natural fibers have superior physical and mechanical Natural fibers
properties than wood fibers, and they are high in
cellulose content and crystallinity, and lighter in In recent years, more renewable plant resources have
weight than wood fibers [1]. Therefore, this type of been discovered and used because non-renewable
fiber could attract more attention in industry [5]. resources are becoming scarce [1]. Figure 1 shows the
Some desirable properties of natural fibers include structural organization of a natural fiber cell wall
high specific strength and modulus, flexibility during [24]. This type of fiber is strong, light, inexpensive,
processing, low self-weight, low cost, and substantial and renewable [24]. These inexpensive natural fibers
resistance to corrosion and fatigue [6]. However, can become a viable alternative for expensive and
natural fibers have drawbacks, such as high moisture non-renewable synthetic fibers (e.g., e-glass, which is
absorption, high anisotropy, low compatibility with alumino-borosilicate glass, and carbon fibers) when
conventional resins, and less homogeneous than glass high elastic modulus is not required [25]. However,
and carbon fibers [3, 7]. the hydrophilic nature of natural fibers results in
Biocomposites are classified into fully and partially swelling of fibers and the production of voids at the
green composites [4]. Petrochemical- and bio-based interface between the matrix and fiber, leading to
resins are used as matrices in the partially and fully poor mechanical properties of composites prepared
green composites, respectively, and natural fibers are using these fibers [26, 27]. Therefore, suitable tech-
used in both [4]. Although all biopolymers are gen- niques must be utilized to produce natural fiber
erally compostable, not all biodegradable and com- composites with high-quality natural fibers.
postable plastics are produced from biopolymers;
some are produced entirely from non-bio-based Sources and types of fibers
materials [4]. Owing to the environmentally friendly
Natural fibers are produced from plant-, animal-, and
characteristic of green composites, they have being
mineral-based sources [1]. Fibrous plants are abun-
increasingly used in industry [1]. Industrial applica-
dantly available in agricultural crops and tropical
tions include aerospace, automobile, military, con-
areas [1]. Plant fibers are mainly composed of cellu-
struction, packaging, medical, sporting equipment,
lose, whereas protein is the major component of
and railway [3]. Table 1 summarizes the advantages
animal fibers [4]. Plant fibers are classified into pri-
and disadvantages of fully green composites over
mary sources, which are fibers produced as by-
traditional composites [8].
products of other principal products (e.g., food,
The physical and mechanical properties of natural
feedstock, and fuel) for industrial usage, and sec-
fiber composites have been investigated in a few
ondary plants, which are produced as by-products
previous review studies [9], which are summarized
derived from manufacturing processes [4]. Table 3
in Table 2. However, detailed information for treat-
shows the major natural fiber sources and their main
ment and modification techniques, fire resistance,
properties. Table 4 shows the main producers and
thermal conductivity and analysis, durability prop-
annual production of these fibers worldwide.
erties, and time-dependent properties was not pro-
There are eight major types of plant fibers: bast
vided in these studies. Additionally, none of the
fibers (jute, ramie, flax, rattan, soybean, hemp, vine,
existing review articles published in journals provide
banana, and kenaf), collected from the skin and bast
any information about creep, shrinkage, wear resis-
around the plants stem; leaf fibers (abaca, banana,
tance, air content, compressive behavior, viscoelastic
sisal, and pineapple), collected from leaves; seed
properties, and life-cycle assessment of the natural
J Mater Sci (2020) 55:829–892 831

Table 1 Summary of
advantages and disadvantages Advantages Disadvantages
of fully green composites over
Less expensive Lower mechanical properties (especially impact strength)
traditional petrochemical-
Lower weight Higher moisture absorption
based composites
Higher flexibility Lower durability
Renewable Poor fire resistance
Biodegradable Variation in quality
Good thermal and sound insulation Restricted maximum processing temperature
Eco-friendly Poor microbial resistance
Nontoxic Low thermal resistance
Lower energy consumption Demand and supply cycles
No residues when incinerated
No skin irritations

Table 2 Previous review studies on natural fiber composites

Year Reference Chemical Physical Processing Water Fire Elastic Tensile Flexural Impact
modification modification techniques absorption resistance modulus strength strength strength

2001 George et al. H H

[10]
2008 John and H H
Thomas [11]
2011 Zini and H
Scandola [12]
2011 La Mantia and H
Morreale [13]
2011 Ku et al. [14] H H
2012 Faruk et al. [4] H H H H H H H H
2012 Dittenber and H H
GangaRao
[15]
2012 Abdul Khalil H
et al. [16]
2013 Koronis et al. H H
[17]
2013 Nguong et al. H H H H
[18]
2014 Faruk et al. [19] H H H
2015 Satyanarayana H
[20]
2015 Mohammed H H
et al. [21]
2016 Pickering et al. H H H
[22]
2018 Sanjay et al. H H H H
[23]

fibers (cotton, coir, and kapok), collected from seeds fibers; root fibers (luffa, swede, and cassava); and
and seed cases; grass fibers (corn, wheat, bamboo, fruit fibers (borassus, tamarind, banana, and coir)
barley, and rice); core fibers (corn and wheat stalk), [1, 4, 28].
collected from the stalks of the plants; wood pulp
832 J Mater Sci (2020) 55:829–892

Figure 1 Structural
organization of a natural fiber
cell wall [24].

There are mainly three types of animal fibers: ani- biodegradable and have no negative effect on the
mal hair, avian fiber, and silk fiber. The fibers of environment, except those grown in temperate zone
animal hair (wool or hair) are taken from hairy with extensive use of agrochemicals (e.g., flax) [1]. On
mammals and animals (e.g., sheep, goats, alpacas, the other hand, animal fibers have low stiffness bal-
and horses) [1, 28]. Silk fibers are taken from the anced by their elastic recovery and high elongation
dried saliva of bugs or insects during the preparation [1]. They are also less hydrophilic than plant fibers,
of their cocoons. Avian fibers are taken from the durable with moderate resistance, poor conductors of
feathers of birds [1, 28]. heat, very sensitive to some alkalis, and able to pro-
vide reinforcement in multi-axial situations [1].
Properties of fibers The cell walls of dried plant fibers are mainly
composed of lignin and sugar-based polymers (i.e.,
Properties of a single fiber are dependent on the cellulose and hemicellulose) and small amount of
shape, size, crystallite content, orientation, and other materials such as starch, extractives, protein,
thickness of the cell walls [1]. The main characteris- and inorganics [1]. Table 5 presents the chemical
tics of natural fibers are low energy consumption, components of the most used dried plant fibers in
low density, non-abrasive nature, low cost, renewa- industry with the average amount (in wt%) of the
bility, biodegradability, easy availability, and world- compositions.
wide abundance [42]. Although plant fibers are Cellulosic fibers have a hydrophilic nature (mois-
normally rigid, unlike brittle synthetic fibers, they are ture absorbent) under natural conditions [1]. The
not fractured during processing [43]. Plant fibers moisture content in fibers can negatively influence
exhibit comparable specific strength and stiffness the mechanical behavior of natural fiber composites.
properties to glass fibers [43]. Bast fibers are extracted Table 6 illustrates the equilibrium moisture amount
from the stem ribbon using a retting process. This of natural fibers at the relative humidity (RH) of 65%
type of fiber has moderately high tensile strength and and temperature of 21 °C.
stiffness; it is inexpensive, exhibits high performance,
and is easily available [1]. This fiber is more appli-
cable when strength, lightweight, and noise absorp-
tion are important, such as in the automotive and
building industries. Most of the plant fibers are cat-
egorized as eco-friendly fibers because they are
Table 3 Sources of major natural fibers and their main properties [1, 28–30]

Group Fiber Source Fiber length (mm) Fiber diameter (lm) Main properties

Bast (plant fibers) Flax Herbaceous plant (Linum Up to 900 12–16 Rapid absorption and desorption of
Usitatissimum) water
Jute Vegetable plant in linden family Up to 4000 17–20 Low thermal conductivity, moderate
[Corchorus capsularis (white jute), moisture regains, high insulation, high
Corchorus olitorius (tossa jute)] anti-static properties, growing in
tropical areas with a humidity of
60–90%
Kenaf Hibiscus (Hibiscus cannabinus L) 6 20–30 Excellent durability
J Mater Sci (2020) 55:829–892

Hemp Cannabis (Cannabis Sativa L) Up to 4000 16–50a Heat conducting, good dying, good
ultraviolet-light blocking, natural anti-
bacterial properties
Ramie Flowering plant in nettle family Up to 1900 25–30 Rapid absorption and desorption of
(Boehmeria nivea) water, low elasticity, easy dying
Leaf (plant fibers) Abaca Abaca plant (Musa textilis) Up to 3000 – High mechanical strength, buoyancy,
resistance to saltwater damage
Pina Pineapple leaf (Ananas magdalenae) Up to 200 – Resistant to salt water, wear resistant
Sisal Agave (Agave sisalana) Up to 1000 200–400b Coarse, hard, durable, strong, and
stretchable, not easily absorb
moisture, resistant to saltwater
deterioration, with a fine surface that
accepts a wide range of dyes
Raffia Raffia palm (Raphia ruffia) Up to 1500 – Rough
Seed (plant fibers) Coir Coconut (Cocos nucifera) Up to 350 12–25 High concentration of lignin, high
strength, less flexibility than cotton,
unsuitability for dyeing, good
resistance to salt water damage and
microbial action
Cotton Shrub (Gossypium) 100–650 11–22 Rapid moisture absorption, high tensile
strength
Kapok Pentandra tree (Ceiba pentandra) 20–32 20a Fluffy
Grass (plant fibers) Bamboo Grass pulp (Bambusoideae) Up to 90 10–20 Excellent durability, high stability, good
tenacity, good flexibility, good
ultraviolet radiation resistance,
excellent permeability
833
Table 3 continued
834

Group Fiber Source Fiber length (mm) Fiber diameter (lm) Main properties

Core (plant fibers) Cornstalk Maize (Maı́z) Up to 3000 40 Lightweight, strong

Wood pulp (plant fiber) Modal Beech tree (Fagus) – 200a Lightweight, soft, wear resistant
Animal fibers Silk Chinese mulberry silkworm Up to 1500 10–13 Good absorbency, low conductivity,
easy dying finish
Byssus Saltwater clam – 10–50 Lightweight
Chiengora Dog hair 25 – Lightweight, fluffy
Qiviut Muskoxen 50–80 15–20 Soft, does not shrink
Yak Yak 16 16–90 Heavy, warm
Rabbit Rabbits – 14–16 Soft
Wool Sheep Up to 152 16–40 Good thermal and acoustic insulation,
high deformability, high durability
Feather Chicken, birds 3–13 5–50 Lightweight, good thermal and acoustic
insulation
Lambswool Lambs Up to 50 15–20 Soft, warm, elastic
Cashmere wool Indian cashmere goat Up to 390 14–19 Soft
Mohair wool North African angora goat Up to 115 25–45 Durable, resilient, holding dyes well
Camel hair Arabian dromedary and Northeast Up to 125 15–23 Warm, lightweight
Asian Bactrian camels
Alpaca South America camels Up to 150 12–29 Soft, warm
Angora wool Angora rabbit – 12–16 Soft, good blending with other fibers
Mineral-based fibers Asbestos cloth Asbestos 12–300 0.03–0.035 Fire resistant, lightweight
Glass Mixed silicates – 5–24 Fire resistant
a
Apparent diameter
b
Apparent diameter when agrochemicals are not used
J Mater Sci (2020) 55:829–892
J Mater Sci (2020) 55:829–892 835

Table 4 Producers and production amount of most widely used natural fibers [1, 4, 31–41]

Fiber Producer Production amount (9 103

ton)

Abaca Philippines (85%), Ecuador 70

Bagasse Brazil, China, India, Thailand, Australia, USA 75,000
Coir India, Sri Lanka, Thailand, Vietnam, Philippines, Indonesia, Brazil 1200
Cotton China, Brazil, India, Pakistan, USA, Uzbekistan, Turkey 25,000
Flax France, Belgium, Netherland, Poland, Russian Federation, China 830
Jute India (60%), Bangladesh, Myanmar, Nepal 3450
Kapok Philippine, Malaysia, China, South America, Indonesia, Thailand 101
Kenaf India (45%), China, Malaysia, USA, Mexico, Thailand, Vietnam 970
Bamboo China, Japan, India, Chile, Ecuador, Indonesia, Myanmar, Nigeria, Sri Lanka, Philippines, 30,000
Pakistan
Hemp China (80%), Chile, France, Germany, UK 214
Ramie China, Brazil, Lao PDR, Philippines, India 280
Sisal Brazil (40%), Kenya, Tanzania, China, Cuba, Haiti, Madagascar, Mexico, Sri Lanka, India 378
Silk China (70%), Brazil, Bulgaria, Egypt, Madagascar, India, Thailand, Vietnam, Uzbekistan, 150
Turkmenistan
Wool Australia, Argentina, China, Iran, New Zealand, Russia, UK, Uruguay 2100
Cashmere China, Mongolia, Australia, India, Iran, Pakistan, New Zealand, Turkey, USA 20
wool
Mohair wool South Africa, USA 5
Camel hair China, Mongolia, Afghanistan, Iran 2
Alpaca Peru, Bolivia, Chile 7
Angora wool China, Argentina, Chile, Czech Republic, Hungary, France 3

Table 5 Chemical
composition of the most Fiber Cellulose (wt%) Hemicellulose (wt%) Lignin (wt%) Waxes (wt%)
widely used plant fibers
Abaca 56–63 20–25 7–9 3
[44–47]
Coir 32–43 0.15–0.25 40–45 –
Cotton 85–90 5.7 – 0.6
Flax 71 18.6–20.6 2.2 1.5
Jute 61–71 14–20 12–13 0.5
Kapok 64 23 – –
Kenaf 72 20.3 9 –
Bamboo 26–43 30 21–31 –
Hemp 68 15 10 0.8
Pina 81 – 12.7 –
Ramie 68.6–76.2 13–16 0.6–0.7 0.3
Sisal 65 12 9.9 2
Bagasse 55.2 16.8 25.3 –
Oil palm 65 – 29 –
Curaua 73.6 9.9 7.5 –
Wheat straw 38–45 15–31 12–20 –
Rice straw 41–57 33 8–19 8–38
Rice husk 35–45 19–25 20 14–17
836 J Mater Sci (2020) 55:829–892

Table 6 Equilibrium moisture content of major natural fibers at degradability. In the fully and partially green com-
RH of 65% and temperature of 21 °C [48] posites, natural fibers are used with bio-based (as a
Fiber Moisture content (wt%) fully degradable matrix) and petrochemical-based (as
a partly degradable matrix) resins, respectively.
Abaca 15
Coir 10 Petrochemical-based resins
Flax 7
Jute 12 A petrochemical-based matrix is a chemical product
Bamboo 8.9 derived from petroleum, which is obtained from
Hemp 9 fossil fuels like coal and natural gas [4]. The two
Pina 13
major types of petrochemical-based matrices used for
Ramie 9
green composites are thermoplastics and thermosets.
Sisal 11
Bagasse 8.8 Polyethylene, polystyrene, polypropylene, and poly-
vinyl chloride (PVC) are utilized as thermoplastic
matrices, whereas epoxy, polyester, vinylester, and
phenolic (phenol formaldehyde) are used for ther-
Matrices for green composites moset matrices [1, 4].

A matrix is used in composites to hold the reinforcing

Thermoplastics
materials together by surface connection. The main
responsibilities of the matrix are the environmental Thermoplastic resins are based on polymers that can
tolerance, surface appearance, and durability of the be shaped easily in the viscous state and solidified by
composite [1]. As the matrix is stressed, it transfers cooling (physical change) [49]. In the melted condi-
the external load uniformly to the fibers, and it is tion, the viscosity of thermoplastic resins is approxi-
applied to resist the propagation of cracks and mately 500–1000 times higher than that of uncured
damage [1]. In recent years, many studies have been thermoset resins [4]. They are solid at room temper-
carried out in an attempt to find an alternative for ature and can be reformed and reshaped when
conventional petroleum-based matrices because of heated without chemical reactions [4]. Thermoplastic
limited fossil fuel resources and the environmental resins have higher impact resistance (approximately
impact of using petroleum-based matrices [4]. Fig- 10 times), more reform-ability, higher damage toler-
ure 2 shows the classification of polymeric matrices ance, and higher processing temperatures and
used in green composites based on their

Matrices for Natural Fiber Composites

Fully degradable Partly degradable

Natural based Oil based • Polypropylene

• Polylactic acid • Aliphatic polyester • Polyester
• Thermoplastic starch • Aliphatic-aromatic polyester • Polyethylene
• Cellulose • Poly(ester amide) • Polyvinyl alcohol
• Polyhydroxy alkanoate • Poly(alkyene succinate)s
• Poly(vinyl alcohol)

Figure 2 Classification of polymeric matrices for natural fiber composites [1].

J Mater Sci (2020) 55:829–892 837

Table 7 Advantages and disadvantages of petrochemical thermoplastic resins [50]

Resin Advantage Disadvantage

Polyethylene High ductility and impact strength Poor weathering resistance

Good fatigue resistance Flammable
Lightweight High thermal expansion
Low moisture absorption
Low cost
Polypropylene High temperature resistance Difficult to process
High dielectric resistance Comparatively expensive
Excellent chemical resistance Limited availability
Good fatigue resistance
Polystyrene Good chemical resistance Flammable
Resistance to stress cracking Low impact resistance
Very low moisture absorption Brittle
Weather resistance
Polyvinyl chloride High impact resistance Poor resistance to UV
Versatility Poor resistance at low and high temperatures
Good chemical resistance
Flame retardant
Low cost
Good dimensional stability

Table 8 Advantages and disadvantages of petrochemical thermoset resins [53–56]

Resin Advantage Disadvantage

Epoxy High thermal and mechanical properties More expensive than vinylester
High water resistance Corrosive amine hardener
Low curing shrinkage Difficult to process
Long working times ability
Polyester Easy to use High curing shrinkage
Lowest cost Limited range of working times
Moderate mechanical properties
High styrene emissions in open molds
Vinylester Very high chemical and environmental resistance High curing shrinkage
Higher mechanical properties than polyester More expensive than polyester
High styrene content
Requires post-curing for good properties
Phenolic High fire resistance Difficult to process

pressures than thermoset resins [1]. Table 7 shows the polymer chains (chemical change), this type of
the advantages and disadvantages of petrochemical- resin has a higher modulus, improved creep resis-
based thermoplastic resins. tance, higher thermal stability, and higher chemical
resistance than thermoplastic resins [4]. They are also
Thermosets brittle at room temperature and show low fracture
toughness. Table 8 shows the advantages and dis-
Thermoset resins are infusible and insoluble materi- advantages of petrochemical-based thermoset resins.
als that are cured by heat or a catalyst [51]. Ther-
mosets are completely different from thermoplastics; Bio-based resins
they cannot be melted and reshaped by heating [52].
Owing to three-dimensional covalent bonds between Bio-based resins are polymers that are fully or par-
tially obtained from renewable resources [1]. Bio-
838 J Mater Sci (2020) 55:829–892

Table 9 Advantages and

disadvantages of bio-based Resin Advantage Disadvantage
resins [57–60]
Starch Fully biodegradable Brittle
Low cost Difficult to process
Water-sensitive
PLA High modulus and strength Brittle
Nontoxic Relatively poor impact strength
Relative low cost Low thermal degradation temperature
PHA High molecular weight Relative low decomposition temperature
Fully biodegradable Low stability
Brittle
Low deformability
More expensive than other bio-based polymers
Cellulose Abundant High moisture absorbance
Relative low cost Relative low decomposition temperature
Ease to modify
Moderate impact resistance
Moderate heat resistance

based polymers can be produced from plants (e.g., Fully bio-based and biodegradable polymers con-
starch and cellulose) or through the polymerization tain renewable carbon, which is taken from the
of plant-based sugars and oils [e.g., polylactic acid atmosphere and then returned to the atmosphere as
(PLA), polyethylene terephthalate, and polypropy- the polymer decomposes [4]. This renewable carbon
lene] [4]. Based on the physical properties, there are can be obtained by collecting the polymers, which are
three types of bio-based polymers: fully bio-based currently used for disposable cutlery and flexible
and biodegradable, e.g., polyhydroxyalkanoates food packaging, in which the plastics are disposed of
(PHA) and starch, partially bio-based and alongside the food waste [1]. Drop-in bio-based
biodegradable, e.g., cellulose and PLA, and partially polymers like bio-based polyethylene terephthalate,
bio-based and non-biodegradable, e.g., bio-poly- which are chemically identical to petrochemical-
ethylene terephthalate, bio-polyethylene, and bio- based polymers, can be traditionally recycled [1].
polypropylene [1, 4]. Table 9 shows the advantages This type of polymer can be combusted to create
and disadvantages of different types of bio-based renewable energy when it is not possible to recycle it.
resins. Bio-based resins offer several advantages over
It was reported that in 2011 approximately 3.5 petrochemical-based resins: they are energy efficient
million tons of bio-based polymers were produced in in production (65% less energy required to produce),
the world, whereas 235 million tons of traditional safe (remain nontoxic as they degrade), recyclable
petrochemical-based polymers were produced in that (break down faster with less energy), completely
year [1]. The growth rate of bio-based polymer pro- renewable (as they are made from biomass), and
duction has been high in recent years, and it has been environmentally friendly (generate 68% less green-
estimated that the production will reach approxi- house gases) [61]. However, their production cost is
mately 12 million tons per year by 2020 [1]. However, approximately 10% higher than that of petrochemi-
this amount is significantly lower than the produc- cal-based resins [62].
tion of petrochemical-based polymers, and it needs to
be increased further to decrease the negative envi-
ronmental impact of petroleum-based materials [1]. It Modification of natural fiber composites
has been shown that, for the same applications, some
types of PLA made from maize starch utilize up to The interfacial adhesion across the phase boundary
50% less oil and release 60% fewer greenhouse gases (i.e., at the interface between two materials) is vital
into the atmosphere compared to petrochemical- for the mechanical behavior of composites [4]. Poor
based polymers [1]. bonding at the phase boundary leads to a composite
with weak mechanical properties. The main concern
J Mater Sci (2020) 55:829–892 839

of the utilization of natural fiber composites is the The surface energy of cellulose fibers with corona
relative high moisture absorption of natural fibers, treatment is changed to improve the compatibility
which results in weak compatibility between fibers between the hydrophilic fiber and matrix [64]. In this
and the matrix [4]. Although moisture absorption approach, using a high voltage at low temperature an
mostly affects natural fibers, there are some resins atmospheric pressure plasma is generated [65, 66].
that absorb a large amount of moisture [1]. Therefore, The surface energy of cellulose fibers is changed in
both the fiber surface and the matrix need to be the plasma treatment method by a surface modifica-
modified to enhance the adhesion of natural fibers to tion technique similar to that of the corona treatment
the matrix for improving the strength and stiffness of [67]. However, in plasma treatment, the gas type,
the natural fiber composite. flow, pressure, and concentration are controlled; in
corona treatment they are not [67, 68]. The UV
Fiber modification treatment method increases the polarity of the fiber
surface, which leads to better wettability of the fibers
Owing to the high sensitivity of natural fibers to and increased strength of the composite [64, 69]. In
moisture, moisture absorption results in delamina- the fiber-beating approach, an increase in the surface
tion between the matrix and fiber, severely reducing area, defibrillation of the fibers, and mechanical
the mechanical properties of the composite [4]. This is interlocking can result in 10% increase in the strength
attributed to the fact that because of the presence of of natural fibers [70]. In heat treatment, fibers are
non-cellulosic components (i.e., pectin, lignin, and heated to a temperature close to the fiber degradation
hemicelluloses), natural fibers in nature are polar and temperature. This condition affects the physical,
hydrophilic, and thus, they create active conditions mechanical, and chemical properties of the fibers,
(i.e., accessibility to hydroxyl (OH) and carboxylic including their water content, chemistry, strength,
acid groups) for water absorption [63]. Furthermore, cellulose crystallinity, and degree of polymerization
differences in the environmental conditions, such as [71, 72].
the amount of sun, rain, soil conditions, and the
amount of water the plant receives during the Chemical modification
growing period, as well as the processing and pro-
duction conditions, may also affect the natural fibers Chemical modification on natural fibers improves the
performance [1]. Therefore, performance and prop- adhesion between the matrix and natural fibers via
erties of natural fibers may be different in every chemical reactions. Extensive studies have been per-
harvesting season and even in the same cultivation formed to understand the effect of chemical treat-
population. The other limiting factor for the utiliza- ment on natural fibers. The hydrophilic nature of
tion of the natural fibers in composites is their low natural fibers and the hydrophobic nature of matrices
thermal stability [4]. However, the problems regard- are considered two different phases, resulting in
ing the utilization of natural fibers in the composite weak bonding at the interfaces of natural fiber com-
can be solved by physical and chemical posites [4]. The chemical treatment of natural fibers
modifications. decreases the inherent hydrophilic behavior of the
fibers and improves the adhesion properties of the
Physical modification matrix and fiber [1]. Chemical treatment methods
include alkaline, silane, acetylation, benzoylation,
Physical modification on natural fibers enhances the peroxide, maleated coupling agents, sodium chlorite,
mechanical adhesion between the natural fiber and acrylation and acrylonitrile grafting, isocyanate,
matrix by enhancing the interface without changing stearic acid, permanganate, triazine, oleoyl chloride,
the chemical properties of the fibers [4]. Extensive and fungal treatments [19, 73].
researches have been conducted to understand the
influence of physical treatments on natural fibers. Alkaline treatment The alkaline treatment approach
Physical treatment methods include corona, plasma, is one of the simplest and most economic and effec-
ultraviolet (UV), fiber beating, and heat treatment. tive methods for improving the adhesion properties
These techniques are applied only to change the of natural fibers to the matrix [74]. In this method, the
surface properties of natural fibers. cellulosic molecular structure of the natural fibers is
840 J Mater Sci (2020) 55:829–892

modified using sodium hydroxide (NaOH) [74]. (SEM) micrographs of longitudinal views of
Alkaline treatment increases the speed of fiber frag- untreated and 6% alkaline-treated kenaf fibers [78].
mentation and disaggregation [75]. The orientation of
the highly packed crystalline cellulose order is Silane treatment In this approach, silane coupling
changed by creating amorphous regions in which agents coat micro-pores on the fiber surface. Silane
cellulose micro-molecules are separated and the forms a chemical link between the fiber surface and
spaces are filled with water molecules [1]. Alkali- the matrix via a siloxane bridge [4]. At the initial
sensitive OH groups are broken down and moved stage of this treatment, silanols are created using
out from the fiber structure, and a fiber cell–O–Na existing moisture and hydrolyzable alkoxy groups
group is created between cellulose molecular chains [4]. One end of the created silanol reacts with a cel-
by the remaining reactive molecules. Therefore, the lulose OH group, and the other end reacts with the
number of hydrophilic OH groups decreases, the matrix functional group by the condensation process.
resistance of the fiber to moisture increases, and a As a result, molecular continuity is formed across the
certain amount of hemicelluloses, lignin, pectin, wax, interface of the composite and a hydrocarbon chain is
and oil are taken out [1]. The surfaces of the fibers obtained to restrain the fiber swelling into the matrix
become clean and uniform, which improves the stress [1]. It has been shown that fibers subjected to silane
transfer capacity between the cells. An optimum treatment exhibit better tensile strength than those
alkali concentration should be obtained to prevent subjected to alkali treatment [24]. Figure 4 shows
extra delignification of the fibers, but higher concen- SEM micrographs of surface views of untreated and
trations can weaken and damage the fibers. With an 2%, 4%, and 6% silane-treated hemp fibers [79].
optimum alkali concentration, the diameter of the
fibers is decreased, resulting in better adhesion due to Acetylation treatment In acetylation treatment, acid
the increased effective fiber surface area and aspect catalysts are used to graft acetyl groups to the cellular
ratio (length/diameter) [76]. Based on the report by structure of the fibers [80]. The fibers are firstly soaked in
Brigida et al. [77], alkaline treatment is the most the acetic acid and then treated with the acetic anhydride
efficient approach for cellulose exposition of natural for 1–3 h at high temperature to accelerate the reaction
fibers. They also found that alkaline treatment can because acetic acid and acetic anhydride cannot sepa-
maintain the native hydrophilic characteristic of rately react with the fibers [4]. In this approach, an
green coconut fibers and increase their thermal sta- esterification reaction happens between OH and car-
bility. Figure 3 shows scanning electron microscopy boxylic/anhydride groups of the natural fibers [81].
Figure 5 shows SEM micrographs of surface views of

Figure 3 SEM micrographs

of longitudinal views of
a untreated and b 6% alkaline-
treated kenaf fiber [78].
J Mater Sci (2020) 55:829–892 841

Figure 4 SEM micrographs

of surfaces of a untreated and 100μm 100μm
b 2%, c 4%, and d 6% silane-
treated hemp fiber [79].

100μm 100μm

untreated and 18% acetylation-treated flax fibers [80]. In improve the interfacial adhesion and thermal stability
the acetylation treatment, the wax and cuticle on the of fibers [84]. First, in a pretreatment step, lignin,
surface of the fiber are removed by the interaction with waxes, and covering oil are extracted and reactive
acetyl, resulting in a smoother surface. Based on the OH groups are exposed on the fiber surface. The
report by Tserki et al. [82], acetylation treatment of flax fibers are then treated with the benzoyl chloride,
and hemp fibers resulted in their reduced moisture where the OH groups of the fibers are replaced with
absorption, removal of the non-crystalline constituents of benzoyl groups. Last, OH groups are attached to the
the fibers, production of a smooth fiber surface, and cellulose backbone [81]. Figure 6 shows SEM micro-
improvement of the stress transfer efficiency. In addition, graphs of surface views of untreated and benzoyla-
based on the study reported by Zafeiropoulos et al. [83], tion-treated flax fibers [85].
acetylation changed the bulk properties of the flax fibers,
as well as their surface properties. Peroxide treatment In peroxide treatment, peroxide-
induced grafting of polyethylene is cohered to the
Benzoylation treatment To decrease the hydrophilic fiber surface and free radicals of peroxide react with
nature of natural fibers, benzoyl chloride is used to the OH groups of the fiber and matrix [86]. This

Figure 5 SEM micrographs

of surfaces of a untreated and
b 18% acetylation-treated flax
fiber [80].
842 J Mater Sci (2020) 55:829–892

Figure 6 SEM micrographs

of surfaces of a untreated and 10μm 10μm
b benzoylation-treated flax
fiber [85].

(a) (b)

method improves the adhesion of the fibers to the of untreated and maleic anhydride (MA)-treated jute
matrix at the interface, decreases the moisture fiber surfaces [91]. The MA-treated fiber shows
absorption ability of the fibers, and increases the improved fiber–resin adhesion at the interface, which
thermal stability of the fibers [81]. Figure 7 shows leads to failure of the fiber by tearing instead of
SEM micrographs of surface views of untreated and interfacial failure.
peroxide-treated flax fibers [85].
Sodium chlorite treatment In sodium chlorite treat-
Maleated coupling agents Maleated coupling agents ment, fibers are bleached in an acid solution using
provide sufficient interaction between the functional sodium chlorite (NaClO2) [92]. This approach
surface of the fibers and the matrix, and they can removes moisture from the fiber and increases their
form carbon–carbon bonds to the polymer chains of hydrophobic nature, which increases the flexibility of
the matrix [87]. The fiber surfaces are coated with the fibers [81]. Figure 9 shows SEM micrographs of
long-chain polymers due to the reaction of maleic surface views of untreated and sodium chlorite-
anhydride with the OH groups in the amorphous treated flax fibers [93].
region of the fiber cellulose structure [88, 89]. The
coating excludes the OH groups from the fiber cells, Acrylation and acrylonitrile grafting In the acrylation
reducing the hydrophilic tendency of the fibers, and acrylonitrile grafting method, more access is
which leads to the formation of a bridge interface and provided for the reactive cellulose macro-radicals to
efficient interlocking between the fiber and the matrix the polymerization medium by the reaction of acrylic
because of the covalent bonding between OH groups acid (CH2=CHCOOH) with the cellulosic OH groups
of the fibers and the anhydride groups of the maleic of the fibers [94]. Ester linkages with the cellulose OH
anhydride [81, 90]. Figure 8 shows SEM micrographs groups are produced by the carboxylic acid of

Figure 7 SEM micrographs

of surfaces of a untreated and 10μm 10μm
b peroxide-treated flax fiber
[85].

(a) (b)
J Mater Sci (2020) 55:829–892 843

Figure 8 SEM micrographs

of surfaces of a untreated and
b maleic anhydride-treated
jute fiber [91].

Figure 9 SEM micrographs

of surfaces of a untreated and
b sodium chlorite-treated flax
fiber [93].

coupling agents, and fiber moisture is eliminated by a views of untreated and isocyanate-treated oil palm
reduction of the hydrophilic OH groups of the fiber fiber [95].
structure [94]. Peroxide radicals start to graft with
acrylic acid on the matrix, producing oxygen–oxygen
Stearic acid treatment In stearic acid treatment, the
bonds by extracting the hydrogen atoms of the
water resistance of the fibers increases due to the
polymer chains [1]. Therefore, the bonding capacity
reaction of the carboxyl groups of stearic acid,
and stress transfer of the interface increase by the
obtained from an ethyl alcohol solution, with the
coupling mechanism of the fibers and the matrix [81].
hydrophilic OH groups of the fibers, thus eliminating
Figure 10 shows SEM micrographs of surface views
the non-crystalline constituents of the fiber structure
of untreated, acrylated, and acrylonitrile-grafted-
[97, 98]. Therefore, the fibers are dispersed better in
treated oil palm fiber [95].
the matrix by breaking down the fiber bundles with
more fibrillation [81]. Figure 12 shows SEM micro-
graphs of surface views of untreated and stearic acid-
Isocyanate treatment Isocyanate treatment increases
treated flax fibers [98].
the bonding properties between the fibers and the
matrix by providing strong covalent bonds between
them [96]. It also increases the moisture resistance Oleoyl chloride treatment Oleoyl chloride (fatty acid
properties of the fibers [96]. The strong covalent derivate) reacts with the OH groups of the fibers and
bonds (chemical bondage) and moisture resistance improves their wettability and adhesion properties
are obtained by the reaction of the functional groups [99]. This improvement is obtained by making the
(–N=C=O) of isocyanate with the OH groups of the fibers more hydrophobic by eliminating the hydro-
cellulose and lignin constituents of the fibers [81]. philic OH groups from the external surfaces of the
Figure 11 shows SEM micrographs of the surface fibers [81]. Figure 13 shows SEM micrographs of
844 J Mater Sci (2020) 55:829–892

Figure 10 SEM micrographs

of surfaces of a untreated,
b acrylated-treated, and
c acrylonitrile-grafted-treated
oil palm fiber [95].

1μm 200μm

(a) (b)

200μm

(c)

Figure 11 SEM micrographs

of surfaces of a untreated and
b isocyanate-treated oil palm
fiber [95].

1μm
200μm

(a) (b)

Figure 12 SEM micrographs

of surfaces of a untreated and
b stearic acid-treated flax fiber
[98].
J Mater Sci (2020) 55:829–892 845

Figure 13 SEM micrographs

of surfaces of a untreated and
b 24-h oleoyl chloride-treated
jute fiber in pyridine [99].

surface views of untreated and 24-h-oleoyl chloride- triazine with the hydrophilic OH groups of the cel-
treated jute fibers in pyridine [99]. lulose and lignin constituents [81].

Permanganate treatment Chemical interlocking at the Fungal treatment Fungal treatment is a new biologi-
interface between natural fibers and the matrix is cal treatment in which specific enzymes are applied
improved by treating the fibers with permanganate to eliminate the non-cellulosic components of the
[100]. In this approach, better adhesion between the fiber surface [102]. Extracellular oxidase enzymes are
fibers and the matrix is provided by the reaction of produced from white-rot fungi, which react with the
potassium permanganate (KMnO4) with the cellulose lignin peroxidase to remove lignin from the fibers.
OH groups and lignin constituents of the fibers, thus Better interlocking between the fibers and matrix
improving the thermal stability of the fibers [81]. creates fine holes in the fiber surface via producing
Figure 14 shows SEM micrographs of the surface hyphae [81]. Figure 15 shows SEM micrographs of
views of untreated and permanganate-treated flax surface views of untreated and fungal-treated hemp
fibers [100]. fibers [102].

Matrix modifications
Triazine treatment Triazine (C3H3N3) treatment
increases the adhesion properties of the fibers and
In general, the concern of moisture absorption in
matrix by providing covalent bonds between them,
composites stems mainly from the natural fibers.
and it enhances the moisture resistance of the fibers
However, some matrices (especially bio-based resins)
[101]. The covalent bond and moisture resistance are
such as soy protein resins absorb a large amount of
obtained by the reaction of the functional groups of

Figure 14 SEM micrographs

of surfaces of a untreated and
b permanganate-treated flax
fiber [100].
846 J Mater Sci (2020) 55:829–892

Figure 15 SEM micrographs

of surfaces of a untreated and
b fungal-treated hemp fiber
[102].

moisture [1]. Soy protein concentrate resin was degradation of the most of natural fibers is 200 °C
modified by Chabba and Netravali [103] through within 20 min [108, 109]. Any temperature above this
adding glutaraldehyde in one case and vinyl alcohol limit can cause degradation, shrinkage, and low
in the other. Both methods resulted in approximately performance of the natural fiber composite because
2% less moisture absorption as compared to that of the chemical, physical, and mechanical properties of
the unmodified resin. Kumar and Zhang [104, 105] the natural fibers are changed by depolymerization,
improved the moisture absorption of soy protein oxidation, hydrolysis, decarboxylation, dehydration,
resin made with different superplasticizers using and recrystallization [110]. The major manufacturing
benzilic acid. They found that immersing the soy methods for natural fiber composites are compres-
protein resin in 0.5% benzilic acid for 26 h resulted in sion molding, extrusion molding, injection molding,
61% (with thiodiglycol superplasticizer) to 76% (with and resin transfer molding techniques. Table 10 pre-
formamide superplasticizer) decrease in the moisture sents the advantages and disadvantages of the pro-
absorption of the resin. Newill et al. [106] found that cessing techniques for manufacturing natural fiber
a 0.254-mm-thick polymeric coating resulted in an composites.
approximately 47% reduction in the moisture
absorption of the matrix. Doherty et al. [107] illus- Processing techniques of thermoplastic
trated that the moisture absorption of a matrix could composites
be reduced by 61% by applying a natural lignin-
based coating with a 0.204-mm thickness. Compression molding

Compression molding has been used since 1990s for

Processing techniques thermoplastic composites as the demand for light-
weight and high-performance materials increased [1].
The main parameters influencing the processing of In this technique, preheated materials are initially
natural fiber composites are moisture, fiber type, fiber placed in the molding cavity. Then, they are com-
volume fraction, and temperature of the composite. pressed and deformed by the core side of the mold
The moisture of both the fiber and the matrix must be while subjecting the cavity to high pressure [1].
controlled before processing, and the required mod- Before opening the mold and removing the compos-
ifications must be performed if moisture is present ite, the high pressure is maintained until the com-
[1]. The length, aspect ratio, and chemical composi- posite solidifies. The important parameters that must
tion of the fibers also have great effects on the pro- be considered with this technique are the amount of
cessing, sustainability, and performance of material, heating time, pressure applied to the mold,
composites [1]. An increase in the fiber volume frac- and cooling time [109].
tion of the composite increases the composite’s stiff- Sheet molding, as a type of compression molding
ness, strength, and water uptake and decreases its technique, is one of the main processing approaches
deformability [1]. The processing temperature is for composite production. Figure 16 shows the pro-
another important factor. The maximum temperature cess diagram of sheet molding technique [123]. In this
that can be used in the processing period to avoid technique, a measured amount of a specific resin is
J Mater Sci (2020) 55:829–892 847

Table 10 Advantages and disadvantages of different processing techniques [109, 111–122]

Technique Advantage Disadvantage

Compression Fast setup time Low production speed

molding Low wasted material Suitable only for flat or moderately curved composite shapes
Low cost for large and complex composites
Good surface finish
Even pressure distribution on the composites
Sheet molding Excellent part reproducibility Suitable only for the preparation of composites with a low fiber
Very high volume production ability volume fraction
Low labor requirements on a production level
Extrusion Fast setup time Moderate production speed
molding Low initial setup costs Suitable only for the preparation of composites with a uniform
Low production costs cross section
Mediocre precision
Injection molding Low operational cost High initial setup costs
Low cost in mass production
High throughput
Flexibility to make parts with complex shapes
High precision
Hand lay-up Simple principles to teach Labor intensive
Low tooling cost Styrene emission from unsaturated polyester and vinylester
Wide choice of material types and suppliers resins
Flexibility in material design Dependency of the quality of the laminate to the skill of
laminators
Resins need to be low viscosity to be workable by hand
Resin transfer Better product consistency than that of More material is wasted than with compression molding
molding compression molding Production speed is lower than that of injection molding
Tighter tolerance and more intricate parts than
injection molding
Fast setup time and low setup costs
Low maintenance costs
Resin infusion Excellent surface quality on both sides Slow cycle times and high consumable costs
molding Short process time
Highly even quality and material thickness

dispensed with a paste reservoir into the plastic car- Extrusion molding
rier film, which is passed under a chopper to cut the
fibers onto the surface [123]. Another sheet is added Extrusion molding is one of the most widely used
on top of the layer after placing the fibers in the resin procedures in the manufacturing process of natural
paste. The sheets are then compacted and sent fiber composites. This technique is preferred because
through to the take-up roll for storing the product. of the high stiffness and strength of the composites
The carrier film is removed, and the material is cut and because the formation of the composites with
into charges and molded under heat and pressure to this technique is very easy [1]. This technique begins
prepare the composite based on the requested shape. with storing the thermoplastic material in the form of
Finally, the product is removed from the mold after pellets or granules in a hopper. Then, they are
full curation [1]. delivered to a heated barrel to be molten. The molten
plastics are subsequently used for the required shape
of the composite. The final stage is cooling the pro-
duct [1].
848 J Mater Sci (2020) 55:829–892

Figure 16 Process diagram of

sheet molding technique for
composite production [123].

Figure 17 Process diagram of

resin transfer molding
technique for composite
production [123].

Injection molding Processing techniques of thermoset

composites
Injection molding is the most common approach
utilized in the manufacturing of mass-produced Hand lay-up
composites. This method is initiated by putting the
polymers in the form of pellets or granules into the Hand lay-up is the most common, simplest, and
hopper and heating them to be molten. The molten cheapest technique for production of composites [15].
materials are then injected into a chamber formed by In this technique, a release agent as an anti-adhesive
a split die mold and kept in the mold. The melt is agent is initially applied to the open mold, and the
chilled down to solidify before opening the mold fibers are then placed in the mold. Resins are applied
[120]. to the fibers by pouring and brushing with a roller or
brush. Lay-up is made by building layer upon layer
till the desired thickness. Entrapped air in the lami-
nate is removed manually with squeegees or rollers.
J Mater Sci (2020) 55:829–892 849

Table 11 Density of major natural and synthetic fibers and Vacuum is often used to avoid air bubbles and to
polymers [15, 22, 129] help draw the resin into the cavity [116].
Fiber and polymer type Density (kg/m3)
Resin infusion molding
Cotton 1520–1560
Jute 1440–1520 Resin infusion molding (RIM) is a double-mold pro-
Flax 1420–1520 cess with medium flow as one type of vacuum-as-
Hemp 1470–1520 sisted RTM, in which the second mold face is
Kenaf 1435–1500
replaced with a flexible membrane [125]. The process
Ramie 1450–1550
takes place on timescales where the fibers swell
Sisal 1400–1450
Coir 1150–1220
during infusion [126, 127]. It is initially started by
Pina 1440 laying dry fibers in the metal face, and the flexible
Abaca 1500 tool face is then pressed down over the composite
Bamboo 600–1100 object. The liquid resin is injected under moderate
Bagasse 1250 pressure into the mold and saturates the fibers. The
Banana 1350 mold can be subjected to a vacuum to minimize air
Oil Palm 700–1550 pockets to enhance the quality of the composite [128].
Curaua 1400
Pulp 1500
Silk 1300 Physical properties
Feather 900
Wool 1300 Unit weight and density
Carbon 1800–1840
Glass 2550–2600 Table 11 shows the densities of most widely used
Polypropylene 890–910
natural and synthetic fibers and polymers, showing
Low-density polyethylene 910–925
that the natural fibers have a lower density than
High-density polyethylene 940–960
Polystyrene 960–1040 synthetic fibers.
Polyester 1040–1400
Nylon 6 1120–1140 Air content
Nylon 6,6 1130–1150
Vinylester 1200–1400 Over several years of producing synthetic composite
Epoxy 1110–1400 materials, it is now possible to control and optimize
Phenolic 1160–1210 the void content to be lower than 2% by volume of
Starch 1000–1390 the composites [130]. Baley et al. [131] reported dif-
PLA 1210–1250 ferent techniques to determine the void content of
PHA 1180–1260

60
Laminates are then left to cure under standard
Flexural Strength (MPa)

50
atmospheric conditions [113].
40
Resin transfer molding 30

In resin transfer molding (RTM), the resin is pre- 20

heated and loaded into the holding chamber instead 10

of loading the polymer into an open mold [124]. This
0
technique is most suitable for medium-volume pro- 0 10 20 30 40 50 60 70
duction of large components. Figure 17 shows the Void Content (%)
process diagram of RTM technique [123]. Layers of
the textile are prearranged in the solid mold, and the Figure 18 The effect of void content on the flexural strength of a
vacuum-treated random-oriented wood pulp fiber/starch
resin is then injected to impregnate the preforms.
composite manufactured using hot pressing [135].
850 J Mater Sci (2020) 55:829–892

composites. The void content in natural fiber com- Tensile properties

posites is a concern because of the voids inherent in
natural fibers, which affect the transverse failure of The tensile properties of natural fiber composites are
the composites [132]. Air or other volatile substances mainly affected by the interfacial adhesion between
can be trapped inside the composites during inser- the resin and fibers [1]. Physical and chemical mod-
tion of the fibers into the resin, and micro-voids can ification of the fiber and resin enhances the tensile
form after curing of the composites. Voids can form properties of composites [14]. Tables 13 and 14 pre-
during compounding or melt-flow processing, or sent the tensile properties of natural fibers and
because of uneven shrinkage owing to thermal gra- polymers (thermoplastics and thermosets), respec-
dients during the solidification process (cooling). An tively. The tensile properties of natural fiber com-
increase in the cooling rate results in an increase in posites are highly dependent on the fiber volume
the void content of composites. Micro-voids create fraction in the matrix resin. Although a number of
poor mechanical properties, which result in sudden researchers showed irregular trends for tensile
failure of the composites [87]. The fiber volume properties of composites as a function of fiber volume
fraction and fiber length in the composites are the fraction, it is generally true that by an increase in the
main factors for void or bubble formation. Higher fiber volume fraction below an optimum value, the
fiber content and length in the composite increase the load is distributed to more fibers and the matrix can
probability of void formation [133]. It was reported carry the applied load after fibers fracture. This can
that a high void content in graphite fiber/polyimide lead to a higher tensile strength for the composite
and glass fiber/polystyrene composites (i.e., over [14]. With further increases in the fiber volume frac-
20% by volume) results in low fatigue resistance tion after the optimum amount, brittle fracture occurs
[133, 134]. The shapes of the voids can be changed in the fibers and the matrix cannot support the
from spherical to elongated, and the void content can additional load from the fibers. Under these condi-
be decreased by a post-extrusion hot-drawing tions, the low tensile strength eventually leads to
approach [133]. Dong and Takagi [135] assessed the failure of the whole composite [160]. The contrary
effect of void content on the flexural properties of a and irregular trends for the tensile properties can be
vacuum-treated random-oriented wood pulp fiber/ because of many factors, including incompatibility
starch composite manufactured using hot pressing between the fibers and matrix, fiber degradation, and
(see Fig. 18). Judd and Wright [136] studied quanti- incorrect manufacturing processes [14]. Figures 19
tatively the effect of voids on the mechanical prop- and 20 illustrate the influence of fiber content on the
erties of fiber/resin composites and reported that, tensile strength and elastic modulus of flax (manu-
regardless of resin, fiber type, and fiber surface factured using extrusion and injection molding) and
treatment, the interlaminar shear strength of a com- hemp fiber/high-density polyethylene (HDPE) com-
posite decreases about 7% for each 1% void. Ghiorse posites (manufactured by compression molding)
[137] showed that laminate lay-up type affects the [14, 93, 161]. Figure 21 shows the influence of the
void distribution, and void length, area, and aspect fiber content by weight on the elongation at break of
ratio increase with an increase in the void content. cross-plied flax fiber/HDPE, cotton fiber/corn starch
(CS), and jute fiber/polybutylene succinate (PBS)
composites [14, 93, 145, 162].
Mechanical properties
Flexural properties
In general, the mechanical properties of natural fiber
composites are lower compared to those of synthetic Flexural stiffness is one of the key parameters for
fiber composites. However, these properties can be measuring the resistance of a composite against
enhanced by proper modifications of the natural bending deformation. Flexural properties are mainly
fibers and matrices through the application of tech- dependent on two parameters: the modulus of the
niques summarized in previous sections. Table 12 composite material and the moment of inertia [4].
presents a summary of the existing studies on the Table 15 presents the flexural properties of polymers
mechanical properties of natural fiber composites. used in natural fiber composites. An increase in the
fiber content up to the optimum amount increases the
J Mater Sci (2020) 55:829–892 851

Table 12 Summary of existing studies on the mechanical properties of natural fiber composites

Reference Composite Apparent fiber Manufacturing Observation

diameter (lm) method

Zampaloni et al. Random-oriented hemp, flax, kenaf, sisal, – Compression 40% by weight hemp fiber composite
[138] and coir fiber/polypropylene composite molding exhibited a higher tensile and flexural
strength than 40% by weight kenaf,
flax, coir, or sisal fiber composites
Joseph et al. Cross-plied abaca fiber/phenolic – Compression Fiber length of 30 mm was optimum for
[139] composite molding achieving maximum tensile, flexural,
and impact strength
Biswas et al. Random-oriented coir fiber/epoxy – Hand lay-up Fiber length of 30 mm was optimum to
[140] composite achieve maximum tensile and flexural
strength. An increase in fiber length
resulted in an increase in the impact
resistance of the composite
Gao and Mader Random-oriented jute fiber/ 22 Injection Fiber length is an important parameter
[141] polypropylene composite molding that can affect the tensile behavior of
the composite
Karmaker and Cross-plied jute and kenaf fiber/ – Injection Superior mechanical properties for the
Schneider polypropylene composite molding jute fiber composite than kenaf fiber
[142] composite
Shibata et al. Random-oriented kenaf and bagasse Kenaf: 140a Compression 60% and 66% increase in flexural
[143] fiber/corn-starch composite Bagasse: 394a molding modulus of kenaf and bagasse fiber
composite with increasing fiber
volume fraction, respectively
Sharma and Cross-plied banana fiber/polyurethane 80a Compression 15% fiber content by weight resulted in
Kumar [144] composite molding the maximum flexural strength
Liu and Hughes Woven flax fiber/epoxy composite – Resin infusion Fracture toughness is mostly dependent
[145] on the fiber volume fraction rather
than reinforcement architecture
Zhang et al. Unidirectional flax fiber/phenolic – Compression Crack propagation was accompanied by
[146] composite molding extensive fiber bridging in the analysis
of interlaminar fracture energy
Li et al. [147] Unidirectional flax fiber/epoxy composite 5–35a Resin infusion Approximately 30% increase in the
interlaminar fracture energy of the
composite using 1% by weight of
multi-walled carbon nanotubes on the
surface of flax fibers
Kafi et al. [148] Woven jute fiber/polyester composite – Compression Improved resistance to crack
molding propagation when fiber treated by
styrene and composite cured by an
out-of-autoclave curing process
Kinloch et al. Woven flax fiber/epoxy composite 17 Resin infusion Maximum increase in fracture
[149] toughness of the composite by adding
both micro-rubber and nanosilica
particles
852 J Mater Sci (2020) 55:829–892

Table 12 continued

Reference Composite Apparent fiber Manufacturing Observation

diameter (lm) method

Hsieh et al. Random-oriented rubber fiber/epoxy 1.24 Resin infusion 175% increase in the fracture toughness
[150] composite with the addition of 20% by weight
silica nanoparticles
Agunsoye and Random-oriented bagasse fiber/ 13 Compression Fracture toughness steadily decreased
Aigbodion polyethylene composite molding with increasing fiber content
[151]
Wong et al. Random-oriented bamboo fiber/polyester 300–380a Hand lay-up The highest fracture toughness was
[152] composite achieved using 50% volume fraction
and a fiber length of 10 mm
Alamri and Random-oriented recycled cellulose/ 5–10 Compression Fracture toughness increased with an
Low [26] epoxy composite molding increase in the fiber content up to 46%
by weight
Muralidhar Unidirectional flax fiber/epoxy composite – Hand lay-up Compressive strength and stiffness of
[153] the composite was because of
reinforcing the matrix rather than the
fiber/matrix synergy
Bledzki et al. Woven jute and flax fiber/epoxy Jute: 37 Compression An increase in the fiber content
[154] composite Flax: 20 molding enhanced the impact strength of the
composite. Flax fiber composite had
higher impact resistance than jute fiber
composite, and an increase in the
number of voids decreased the impact
strength of composite
Cao et al. [155] Bagasse fiber/polyester composite 390a Compression Impact strength of the composite 30%
molding increased with an increase in the fiber
content up to an optimum amount of
65%
Biswas et al. Sisal fiber/polyester composite – Compression At 0.5% fiber volume fraction, sisal
[34] molding fiber/polyester composite had
comparable impact strength to glass
fiber/polyester composite
Dhakal et al. Random-oriented hemp fiber/polyester 20 Hand lay-up Increasing the hemp fiber volume
[156] composite fraction up to 10% led to a 228%
increase in the impact strength
Jandas et al. Random-oriented banana fiber/polylactic – Compression An increase in the fiber volume fraction
[157] acid composite molding up to 25% resulted in the maximum
impact strength
Liang et al. Unidirectional flax fiber/epoxy composite – Hand lay-up Compressive strength of the composite
[158] 15–30% decreased by applying 10 J
impact loading
a
Diameter of a fiber bundle

flexural strength of natural fiber composites [4]. content also increases the flexural modulus of the
However, further increases in the fiber content composites [4].
decrease the flexural strength, owing to defects in the The fracture toughness of natural fiber composites,
wetting of fibers that can induce stress concentration which means a composite’s resistance to crack
points in the composites. An increase in the fiber propagation, is mainly influenced by the intrinsic
properties of the matrix, the fiber volume fraction,
J Mater Sci (2020) 55:829–892 853

Table 13 Tensile properties

of most widely used natural Fiber Tensile strength (MPa) Elastic modulus (GPa) Elongation (%)
fibers [14, 15, 22, 159]
Cotton 287–800 5.5–12.6 7–12
Jute 393–860 13–60 1.5–1.8
Flax 345–1500 27.6–90 2.7–3.2
Hemp 550–920 55–70 2–4
Kenaf 195–666 53–66 1.3–5.5
Ramie 400–938 61.4–128 3.6–3.8
Sisal 468–790 9.4–25 2–7
Coir 135–240 4–6 15–40
Pulp 1000 40 4.4
Pina 413–1627 34.5–82.5 1.6
Abaca 430–760 6.2–20 1–10
Bamboo 140–800 11–32 2.5–3.7
Bagasse 222–290 17–27.1 1.1
Banana 500 12 1.5–9
Oil Palm 80–248 0.5–3.2 17–25
Curaua 87–1150 11.8–96 1.3–4.9
Silk 100–1500 5–25 15–60
Feather 100–203 3–10 6.9
Wool 50–315 2.3–5 13.2–35

Table 14 Tensile properties of polymers used in natural fiber composites [129, 159]

Resin Tensile strength (MPa) Elastic modulus (GPa) Elongation (%) Type of resin

Polypropylene 26–41.4 0.95–1.77 15–700 Thermoplastic

Low-density polyethylene 40–78 0.055–0.38 90–800
High-density polyethylene 14.5–38 0.4–1.5 2–130
Polystyrene 25–69 4–5 1–2.5
Nylon 6 43–79 2.9 20–150
Nylon 6,6 12.4–94 2.5–3.9 35–300
Starch 5–6 0.125–0.85 31–44
PLA 21–60 0.35–3.5 2.5–6
PHA 18–24 0.7–1.8 3–25
Polyester 41.4–89.6 2.07–4.41 2–2.6 Thermoset
Vinylester 69–83 3.1–3.8 4–7
Epoxy 55–130 3–6 2–10
Phenolic 50–60 4–7 1

and the interfacial bonding strength [4]. The energy obtained for the composite, owing to a decrease in the
dissipation is influenced by pull out of fibers in the number of voids [4]. Increased compressive strength
wake of crack propagation of the composites [149]. is also attributed to good homogeneity and high
compaction between the fibers and the matrix.
Compressive properties However, as the fiber volume fraction exceeds the
optimum value, the compressive strength decreases.
The compressive behavior of natural fiber composites Generally, when the fiber volume fraction exceeds
is highly dependent on the reinforcement architec- 1.5%, a reduction of compressive strength of
ture and fiber volume fraction of the composite approximately 8.5% occurs for every 0.5% increase in
[4, 163]. With increasing fiber volume fraction below fiber volume [164, 165]. However, it was shown that
the optimum amount, higher compressive strength is the compressive strength of natural fiber composites
854 J Mater Sci (2020) 55:829–892

50 architecture parameter on the compressive behavior

of a hemp fiber/polyester composite tube manufac-
Tensile Strength (MPa)

40
tured by filament winding technique with fiber ori-
30 entation of 10°, 30°, 45°, 60°, and 90°. Figure 22 shows
the macro- and micro-images of the tubes with fiber
20
orientation of 45° and 90° [163]. They found that a
10 Flax-HDPE
fiber orientation of 10° with the loading direction
Hemp-HDPE
resulted in the highest compressive strength and
0 modulus, and the observed fracture modes were
0 10 20 30 40 50
diamond-shaped buckling, micro-buckling, con-
Fiber Volume Fraction (%)
certina-shape buckling, and progressive crushing.
Figure 19 The effect of fiber content on the tensile strength of
flax (manufactured using extrusion and injection molding) and Impact strength
hemp fiber/high-density polyethylene (HDPE) composites
(manufactured by compression molding). The impact behavior of natural fiber composites
mainly depends on the bonding level between the
8 matrix and fiber [4]. This property plays a major role
during the service life of natural fiber composites [4].
Elastic Modulus (GPa)

6 The impact properties of natural fiber composites can

be improved by modification methods. The impact
4 loading may be the result of bumps, crashes, and
falling objects and debris. Some of the influential
2 parameters on the impact strength of composites are
Flax-HDPE
the level of adhesion, favorable bonding, fiber pull-
Hemp-HDPE
0 out, and energy absorption [4].
0 10 20 30 40 50
Fiber Volume Fraction (%) Effect of fiber/matrix treatment
on the mechanical properties
Figure 20 The effect of fiber content on the elastic modulus of
flax (manufactured using extrusion and injection molding) and
Several researchers have assessed the effect of fiber or
hemp fiber/high-density polyethylene (HDPE) composites
matrix treatment on the mechanical properties of
(manufactured by compression molding).
natural fibers composites. Table 16 presents a sum-
120 mary of the existing studies on the effect of
Flax-HDPE fiber/matrix treatment on the mechanical properties
100 Cotton-CS of natural fiber composites.
Elongation (%)

80 Jute-PBS

60 Effect of crystallinity on the mechanical

40
properties
20 Crystallinity restricts the mobility of the molecular
0 chains of the material and plays a major role in the
0 5 10 15 20 25 30 35 physical and mechanical behavior of natural fiber
Fiber Content by Weight (%) thermoplastic matrix composites [207]. The structure
of a cellulose material composes amorphous and
Figure 21 The effect of fiber content on the elongation at break
of cross-plied flax fiber/HDPE, cotton fiber/corn starch (CS), and crystalline regions. The amorphous region absorbs
jute fiber/polybutylene succinate (PBS) composites. chemicals, such as dyes and resins, whereas the
compactness of the crystalline region makes it diffi-
gradually reduced with increasing fiber volume cult for chemical penetration [207]. Chemical treat-
fraction [165, 166]. Wecławski et al. [163] assessed the ments on the fiber increase its crystallinity, owing to
influence of the fiber orientation as a reinforcement the removal of lignin and hemicellulose after
J Mater Sci (2020) 55:829–892 855

Table 15 Flexural properties

of the polymers used in the Resin Flexural strength (MPa) Flexural modulus (GPa)
natural fiber composites [1]
Polypropylene 40 1.5
Low-density polyethylene 9 0.2
High-density polyethylene 32 1.2
Polystyrene 70 2.5
Nylon 6 85 2.3
Nylon 6,6 103 3.1
Polyester 70–110 2–4
Vinylester 130–140 3
Epoxy 110–150 3–4
Phenolic 80–135 2–4
Starch 52 2.4
PLA 51–70 4.2
PHA 94 2.7

Figure 22 a A diagram with

positioning of cross section
and fiber orientation, and
macro- and micro-images of
hemp fiber/polyester
composite with fiber
orientation (h) of b 45° and
c 90° [163].

(a)

Hemp fibers

Section A-A 500μm

(b)

Hemp fibers Hemp fibers

Section A-A 500μm Section B-B 500μm

(c)
856 J Mater Sci (2020) 55:829–892

treatment [208, 209]. A limited number of studies studies have investigated the trans-crystallinity of
assessed the effect of crystallinity on the mechanical conventional composites, only a few studies investi-
properties of natural fiber composites. Rong et al. [72] gated the influence of the trans-crystallinity on the
investigated the effect of different fiber treatments on mechanical properties of natural fiber composites.
the crystallinity and found that heat treatment (at Zafeiropoulos et al. [214, 215] studied the effect of
150 °C for 4 h) of unidirectional sisal fibers led to trans-crystallinity on the interface of flax fiber/
slightly higher crystallinity index (66%) than those polypropylene composite and found that the induced
under acetylation (65%) and alkaline treatment (61%). fiber trans-crystallinity from stearation surface mod-
They found that alkaline-treated sisal fiber/epoxy ification resulted in 81% increase in the interfacial
composites manufactured by compression molding shear strength of the composite, owing to the
technique had the highest tensile strength and mod- improved interfacial adhesion between fiber and
ulus, acetylated-treated sisal fiber/epoxy composites polymer by the presence of a trans-crystalline layer.
had the highest flexural strength, and heat-treated Sawpan et al. [216] assessed the influence of the fiber
sisal fiber/epoxy composites had the highest flexural trans-crystallinity from alkaline treatment on the
modulus. Barone [210] investigated the influence of interfacial shear strength of random-oriented hemp
the degree of crystallinity of the polymer on the fiber/PLA composite manufactured by extrusion and
tensile strength and modulus of random-oriented injection molding techniques and reported that
keratin feather fiber/polyethylene composite manu- alkaline-treated fiber composite had 18% higher
factured by compression molding technique. They interfacial shear strength than that with no fiber
found that an increase in the crystallinity of the treatment. They attributed their observation to the
polymer obtained from heat treatment (at 170 °C for positive influence of the fiber crystallinity at the
15 min) led to an increase in the tensile strength and fiber/polymer interface, which is shown in Fig. 24
modulus of the composite because of the increased [216].
fiber/polymer interaction. Zafeiropoulos et al. [211]
and Joseph et al. [87] reported that cooling rate is one Simulation and modeling
of the main parameters affecting the crystallinity
degree of the natural fiber-reinforced composites. Analytical models
They found that lower cooling rates result in smaller
fragment lengths of random-oriented flax fiber/ Six analytical models have been used for prediction
polypropylene and sisal fiber/polypropylene com- of the mechanical behavior of natural fiber compos-
posite, indicating a better stress transfer-ability and ites with discontinuous fibers, including rules of
stronger interface by slow cooling. Suryanegara et al. mixture, series and parallel, Hirsch model, Halpin–
[212] reported that random-oriented pulp fiber/PLA Tsai equation, Bowyer–Bader model, and shear lag
composite manufactured by compression molding model [217]. The fundamental properties used in
technique with 3% fiber weight fraction and fully these models are elastic modulus of the fiber (Ef),
crystallized polymer (heat-treated at 100 °C for 1 h) elastic modulus of matrix (Em), tensile strength of
had 4% and 16% higher tensile strength and modulus fiber (rf), tensile strength of matrix (rm), fiber volume
compared to those with fully amorphous polymer, fraction (Vf), and matrix volume fraction (Vm). In
respectively. However, they found that the crys- these models, the micro-defects in the polymer and
tallinity of polymer increased the brittleness of the fiber/polymer interface are not considered [218].
composite. Figure 23 shows the axial tensile stress– Virk et al. [219] used rules-of-mixture model to
strain curves of pulp fiber/PLA composite under predict the elastic modulus and tensile strength of
amorphous and crystallized states [212]. unidirectional jute fiber/epoxy composite manufac-
When a fiber is embedded into a semicrystalline tured by resin infusion molding technique and
polymer, the fiber may act as a nucleating site for the reported that using the common method to measure
growth of spherulites [213]. If many nucleation sites the cross-sectional area of the fibers by linear mea-
exist along the fiber surface, the resulting spherulite surements of fiber diameter and an assumption of
growth will be restricted in the lateral direction and a circular cross section results in an overestimation of
columnar layer, known as trans-crystallinity, devel- the cross-sectional area and hence leads to low values
ops and encloses the fiber [213]. Although several of key mechanical properties of natural fibers. They
J Mater Sci (2020) 55:829–892 857

Table 16 Effect of fiber/matrix treatment on mechanical properties of natural fiber composites

Reference Treatment Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Gassan and Fiber corona Tossa jute fiber/epoxy – Compression 30% increase in the flexural strength
Gutowski [64] treatment composite molding under optimum corona treatment
condition
Fiber ultraviolet 30% increase in the flexural strength
(UV) treatment
Ragoubi et al. Fiber corona Random-oriented hemp – Extrusion Improved Young’s modulus,
[167] treatment fiber/polypropylene molding stiffness, and tensile strength
composite
Pizzi et al. [168] Flax and hemp – Compression Improved tensile strength and
fiber/tannin and hexamine molding modulus by optimum duration of
composite corona treatment of 10 min
Ragoubi et al. Random-oriented – Extrusion– Improved mechanical properties
[169] miscanthus fiber/polylactic compression
acid and polypropylene molding
composite
Marais et al. [67] Fiber plasma Random-oriented flax fiber/ 20 Compression Improved permeation and
treatment polyester composite molding mechanical properties
Martin et al. [68] Random-oriented sisal fiber/ – Compression 25% and 18% increases in the tensile
high-density polyethylene molding strength and modulus, respectively
composite
Seki et al. [170] Woven jute fiber/high- 30a Compression 35% and 30% increases in the
density polyethylene molding interlaminar shear strength and
composite flexural strength, respectively
Sinha and Random-oriented jute fiber/ 30a Hand lay-up 14% increase in the flexural strength
Panigrahi polyester composite
[171]
Seki et al. [172] Woven jute fiber/polyester 100a Hand lay-up 72% and 129% increases in the
composite interlaminar shear strength through
the low- and radio-frequency
oxygen plasma treatment,
respectively
Jang et al. [173] Random-oriented coir fiber/ – Compression Improved mechanical as well as the
polylactic acid composite molding thermal behavior
Beg and Fiber-beating Random-oriented kraft fiber/ 25 Extrusion 10% enhancement in the tensile
Pickering [70] treatment polypropylene composites molding strength
Ray et al. [74] Fiber alkaline Jute fiber/vinylester – Compression 35%, 23%, and 19% increases in the
treatment composite molding flexural strength, modulus, and
laminar shear strength, respectively
Aziz et al. [78] Random-oriented hemp and Hemp: Compression 25% and 150% increases in the
kenaf fiber/polyester 180a molding flexural strength of hemp and kenaf
composite Kenaf: fiber composite, respectively.
110a
Cao et al. [155] Random-oriented bagasse 390a Compression 13% and 65% increases in tensile
fiber/polyester composite molding and impact strength, respectively,
with a 1% alkaline fiber treatment
Prasad et al. Random-oriented coir fiber/ 150–300a Hand lay-up 40% increase in the impact and
[174] polyester composite flexural strength by 5% alkaline
treatment for 72 h
858 J Mater Sci (2020) 55:829–892

Table 16 continued

Reference Treatment Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Ray et al. [175] Random-oriented jute fiber/ – Hand lay-up 20% enhancement in the flexural
vinylester composite strength by 5% alkaline treatment
for 4 h
Onal et al. [176] Random-oriented carpet 10 Compression Improved impact strength
waste jute yarn composite molding
Huda et al. [177] Woven pina fiber/polylactic 50a Compression 26% improvement in the flexural
acid composite molding strength through 40% alkaline
treatment
Qin et al. [178] Unidirectional ramie – Compression 23% improvement in the tensile
fiber/cellulose composite molding strength through 9% alkaline fiber
treatment for 1 h
Bledzki et al. Unidirectional flax and – Filament Improved flexural strength, tensile
[179] hemp fiber/epoxy and winding strength, tensile modulus, and
polypropylene composite elongation
Venkateshwaran Random-oriented banana 150a Hand lay-up 20, 12, 132, and 131% increases in
et al. [180] fiber/epoxy composite the flexural strength, flexural
modulus, tensile strength, and
tensile modulus through 1%
alkaline treatment, respectively
Suardana et al. Fiber silane Random-oriented hemp – Compression 2% and 4% increases in the flexural
[79] treatment fiber/polypropylene molding and tensile strength through 6%
composite silane treatment, respectively
Jandas et al. Banana fiber/polylactic acid – Compression 136% and 49% enhancement in the
[157] composite molding tensile and impact strength,
respectively
Xu et al. [181] Random-oriented kenaf 50–120a Compression 45% and 25% increases in the
fiber/polystyrene molding storage modulus and tand (the ratio
composite of viscous to elastic properties)
through 5% silane fiber treatment,
respectively
Pothan and Abaca fiber/polyester 50–250a Compression Improved storage modulus
Thomas [182] composite molding
Cantero et al. Random-oriented flax fiber/ – Extrusion 6% and 3% increases in the tensile
[183] polypropylene composite molding and flexural strength through 2.5%
silane treatment, respectively
Abdul Khalil Oil palm empty-fruit-bunch – Compression Improved tensile strength
and Ismail and coir fiber/polyester molding
[184] composite
Ismail and Oil palm empty-fruit- 180a Compression Improved tensile strength, modulus,
Abdul Khalil bunch/natural rubber molding tear strength, fatigue life, and
[185] composite hardness
Sgriccia et al. Hemp and kenaf fiber/epoxy 160a Compression Silane-treated fiber composite had a
[186] composite molding higher flexural modulus than
alkaline-treated composite and
similar to glass fiber composite
Eng et al. [187] Random-oriented oil palm – Melt blending 18% improvement in the tensile and
fiber/polylactic acid flexural strength
composite
J Mater Sci (2020) 55:829–892 859

Table 16 continued

Reference Treatment Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Bledzki et al. Fiber acetylation Random-oriented flax fiber/ 100a Injection Up to 35% increases in the tensile
[80] treatment polypropylene composite molding and flexural strength
Joseph et al. Random-oriented abaca 240a Compression 81, 700, and 8% enhancement in the
[188] fiber/phenolic composite molding tensile strength, Young’s modulus,
and impact strength through 50%
acetylation treatment, respectively.
Hill and Abdul Random-oriented coir and Coir: Compression Higher improvement in the tensile
Khalil [189] oil palm fiber/polyester 336a molding strength, Young’s modulus, flexural
composite Oil Palm: strength, and impact strength of the
408a composite by acetylation treatment
than those by silane treatment
Zafeiropoulos Flax fiber/polypropylene 20 Compression Improved stress transfer efficiency at
et al. [98, 190] composite molding the interface of fiber and resin by
determining the optimum treatment
time
Luz et al. [191] Random-oriented bagasse 10 Injection Decreases in the flexural properties
fiber/polypropylene molding
composite
Manikandan Fiber Sisal fiber/polystyrene – Compression 91% improvement in the tensile
et al. [84] benzoylation composite molding strength
treatment
Wang et al. [85] Flax fiber/low-density – Compression 6% enhancement in the tensile
polyethylene composite molding strength
Manikandan Random-oriented sisal fiber/ – Combined Improved storage modulus and
et al. [192] polystyrene composite compression/ damping properties
extrusion
molding
Joseph et al. [86] Fiber peroxide Sisal fiber/polyethylene – Compression Improved tensile strength
treatment composite molding
Sreekala et al. Random-oriented oil palm 150–500a Compression Improved impact resistance and
[95] fiber/phenolic composite molding flexural and tensile properties
Sapieha et al. Cellulose fiber/polyethylene – Compression Dicumyl peroxide-treated
[193] composite molding composites exhibited superior
mechanical properties than
treatment benzoyl peroxide-treated
composites
Abdul Razak Kenaf fiber/polylactic acid – Compression Improved tensile and flexural
et al. [194] composite molding strength
Hong et al. [91] Fiber treated by Random-oriented jute fiber/ 45a Compression Improvements in the Young’s
a maleated polypropylene composite molding modulus and dynamic storage
coupling agent modulus through maleic anhydride
treatment
Yang et al. [195] Random-oriented rice husk 209a Injection Improved tensile strength through
fiber/polypropylene molding the positive influence of maleated
composite polypropylenes on the interfacial
bonding
860 J Mater Sci (2020) 55:829–892

Table 16 continued

Reference Treatment Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Li et al. [196] Random-oriented – Injection Improved tensile strength through

hildegardia fiber/ molding maleated polypropylenes
polypropylene composite
Keener et al. Random-oriented jute and 10–20 Injection 60% increase in the tensile and
[197] flax fiber/polypropylene molding flexural strength
composite
Liu et al. [198] Random-oriented abaca – Injection Improvement in the moduli and
fiber/high-density molding strength through maleic anhydride-
polyethylene composite grafted styrene treatment
Gassan and Woven tossa jute fiber/ – Compression Improved dynamic modulus and
Bledzki [199] polypropylene composite molding specific damping capacity through
maleic polypropylene anhydride
treatment
Wielage et al. Random-oriented flax and – Injection Improved dynamic mechanical
[200] hemp fiber/polypropylene molding properties through maleic acid
composite anhydride-grafted treatment
Li et al. [93] Fiber bleaching Random-oriented flax fiber/ – Injection Improved tensile strength through
polyethylene composite molding sodium chlorite treatment
Misra et al. [201] Random-oriented sisal fiber/ 50–240 Hand lay-up Improved tensile, flexural, and
polyester composite impact properties through sodium
chlorite treatment
Vilay et al. [94] Fiber acrylation Random-oriented bagasse 10 Vacuum Superior tensile and flexural
and fiber/polyester composite bagging properties for acrylation-treated
acrylonitrile composite than those with alkaline
grafting treatment
Sreekala et al. Random-oriented oil palm – Compression Improved tensile strength, Young’s
[202] fiber/phenolic composite molding modulus, and elongation at break
of the acrylic acid-treated fibers
Joseph et al. Fiber isocyanate Random-oriented sisal fiber/ 100–300 Injection Improved tensile properties
[203] treatment polyethylene composite molding
Paul et al. [204] Fiber stearic acid Banana fiber/polypropylene 125–150a Compression Improved tensile and flexural
treatment composite molding strength
Kalaprasad et al. Random-oriented sisal fiber/ 100–300 Compression Improved tensile strength and
[205] low-density polyethylene molding Young’s modulus
composite
Torres et al. Sisal fiber/polyethylene 223 Compression 23% increase in the shear strength
[206] composite molding through 3% stearic acid treatment
Li et al. [100] Fiber Random-oriented flax fiber/ – Injection Improved tensile strength through
permanganate high-density polyethylene molding potassium permanganate treatment
treatment composite
Pickering et al. Fiber fungal Random-oriented hemp 20 Injection 22% increase in the tensile strength
[102] treatment fiber/polypropylene molding through fungal treatment, 32%
composite increase in the tensile strength
through combined fungal/alkaline
treatment
J Mater Sci (2020) 55:829–892 861

Table 16 continued

Reference Treatment Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Chabba and Resin treatment Unidirectional flax fiber/soy – Compression Glutaraldehyde improved
Netravali [103] by protein composite molding mechanical properties and vinyl
glutaraldehyde alcohol improved the toughness
and vinyl
alcohol
a
Diameter of a fiber bundle

proposed a fiber area correction factor to accurately molding technique obtained by series and parallel,
predict the elastic modulus and tensile strength of the Hirsch, shear lag, Halpin–Tsai, and Bowyer–Bader
composite. Kalaprasad et al. [220] conducted a com- models and reported that all models except the ser-
parison between prediction of tensile properties of ies-and-parallel model showed good agreement with
random-oriented sisal fiber/low-density poly- experimental tensile strength and modulus of longi-
ethylene composite manufactured by injection tudinally oriented composites. They also reported
that Hirsch and Bowyer–Bader models had a good
agreement with experimental results of randomly
80
oriented composites. Facca et al. [221] predicted the
Amorphous Polymer Young’s modulus of random-oriented hemp fiber/
Axial Stress (MPa)

60 HDPE composite manufactured by compression

molding technique using rules of mixture, Halpin–
40 Tsai equation, and shear lag model. Their results
0% Fiber showed that Young’ modulus predicted by Halpin–
3% Fiber Tsai equation had a higher accuracy than that by
20 5% Fiber other models because the efficiency factor in the
10% Fiber
Halpin–Tsai equation is normally derived from
20% Fiber
0 experimental measurements of the material to be
0 0.02 0.04 0.06 0.08
modeled. Beckermann and Pickering [222] predicted
Axial Strain
the tensile strength of hemp fiber/polypropylene
(a)
composite manufactured by extrusion and injection
80
molding techniques by Bowyer–Bader model and
Crystallized Polymer
reported that fiber aspect ratio and orientation are
Axial Stress (MPa)

60 two main parameters that should be considered in

the prediction of the mechanical behavior of natural
40 fiber composites. Migneault et al. [223] predicted
0% Fiber
tensile elastic modulus of random-oriented pulp
3% Fiber
fiber/HDPE composite manufactured by injection
20 5% Fiber
molding technique using shear lag model and Hal-
10% Fiber
pin–Tsai equation and reported that the predictions
20% Fiber
0 considering an orientation factor in the modeling had
0 0.02 0.04 0.06 0.08
a good agreement with the experimental results.
Axial Strain
Munde and Ingle [224] compared the modeling
(b)
results of Hirsch model, Halpin–Tsai equation, and
Figure 23 Axial tensile stress–strain curves of pulp fiber/ Bowyer–Bader model with the experimental results
polylactic acid composites under a amorphous and of the tensile strength and elastic modulus of
b crystallized states.
862 J Mater Sci (2020) 55:829–892

Figure 24 Optical light

micrographs of hemp fiber/
polylactic acid composite with
a untreated fiber and
b alkaline-treated fiber [216].

50 μm 50 μm

(a) (b)

random-oriented coir fiber/polypropylene composite the modeling predictions were in a good agreement
manufactured by compression molding technique. with the experimental results. Modniks and Ander-
They found that Hirsch model developed a higher sons [227] also used RVE orientation averaging
accuracy in prediction of the tensile strength and method for prediction of the nonlinear deformation
modulus of the composite than Halpin–Tsai and of the random-oriented flax fiber/polypropylene
Bowyer–Bader models. composite (shown in Fig. 26). They first conducted
the simulation under six load conditions of trans-
Finite element simulation verse tension, transverse compression, pure tension,
axial tension, shear tension, and equi-biaxial tension
Finite element (FE) method has been used to model to determine deformation parameters, and then they
the properties of natural fiber composites, because it input the parameters into the RVE orientation aver-
is possible to efficiently study the effect of different aging method for prediction of the nonlinear defor-
parameters, such as fiber reinforcement type, fiber mation of the composite. They reported a good
volume fraction, fiber aspect ratio, and fiber orienta- agreement between the stress–strain curve predic-
tion, on the properties of natural fiber composites tions and experimental results. Kern et al. [225]
[225]. Among the FE methods, representative volume developed a direct 3D RVE model for investigating
element (RVE) FE, as the most popular homoge- the influence of fibers and micro-cellular voids on the
nization-based multi-scale method and most effective tensile behavior of random-oriented wheat straw
and accurate method for mechanical properties of fiber/polypropylene composite (shown in Fig. 27).
composite materials, has been considered for pre- They found that the composite with voids had a
diction of the mechanical properties of composites. shorter fracture path than that with no void. Their
Two RVE methods of direct RVE and orientation predictions were in a good agreement with the
averaging methods have been used to simulate nat- experimental results. Sliseris et al. [228] developed a
ural fiber composites with discontinuous fibers. In direct 3D RVE model for simulation of the tensile
direct RVE method, matrix surrounds a number of behavior of random-oriented flax fiber/polypropy-
natural fibers, whereas in the orientation averaging lene composite considering the influence of the fiber
method, a single fiber is embedded in the matrix (as a aspect ratio, bundles, and defects. Flax fiber was
block unit cell (UC)). A few studies predicted the modeled as a linear isotropic elastic material and
mechanical properties of natural fiber composites polypropylene resin was modeled as a nonlinear
with discontinuous fibers by FE method. Modniks plastic material. To consider the influence of the fiber
and Andersons [226] used RVE orientation averaging defect in the modeling, they modeled the fibers and
method to predict the Young’s modulus of random- the interface between the fiber bundles as a brittle
oriented flax fiber/polypropylene composite manu- material with a continuum damage mechanic model
factured by extrusion molding technique (shown in (shown in Fig. 28). They found that plastic deforma-
Fig. 25). They assumed that the UC is transversely tion of the composite started at the fiber endings and
isotropic and determined the elastic constants of the around fiber defects, which was in agreement with
composite from five loading nodes. They showed that the experimental results.
J Mater Sci (2020) 55:829–892 863

Figure 25 Schematic of a the

unit cell (comprising a fiber
embedded in a block of Longitudinal modulus
matrix) and b loading nodes of
the unit cell for prediction of
the Young’s modulus by
Transverse modulus
representative volume element
(RVE) orientation averaging
method [226].

Shear modulus

Shear modulus

Orthogonal cross-secons
Poisson’s rao
(a) (b)

absorption, wear resistance, and weathering in nat-

ural fiber composites. Table 17 presents a summary
of the existing studies on the durability properties of
natural fiber composites [230–240].
All natural fibers are hydrophilic in nature, and
their saturation moisture content ranges from 3 to
Figure 26 Schematic of the unit cell for prediction of the 13% [241]. The water absorption of the natural fiber in
nonlinear deformation of a random-oriented fiber composite [227]. natural fiber composites is a serious concern for their
potential outdoor application [241]. The absorption of
Durability properties moisture in natural fibers results in the swelling of
fibers and a reduction of the adhesion between fibers
The low durability of natural fiber composites results
and matrix, dimensional instability, matrix cracking,
in a decrease in the mechanical properties and the
and weak mechanical properties of the composites
growth of fungus and bacteria in the composite [229].
due to debonding between the fibers and the matrix
Several studies have been conducted to investigate
[139, 242]. The water absorption property of natural
the key durability-related properties of water
fiber composites depends on the fiber volume

Figure 27 Meshing of
arbitrarily distributed wheat
straw fibers embedded in
a solid polypropylene and
b polypropylene with micro-
cellular voids in a direct 3D
representative volume element
(RVE) model [225].
864 J Mater Sci (2020) 55:829–892

Figure 28 Modeling of the

failure mechanism considering
the damage at fiber defects
using 3D representative
volume element (RVE) model
for simulation of the tensile
behavior of random-oriented
flax fiber/polypropylene
composite [228].

fraction, fiber orientation, temperature, exposed sur- fiber pull-out, matrix yielding, interfacial debonding,
face area, permeability of the fibers, void content, and and crack coalescence. An imperfect interface leads to
hydrophilicity of the composite components. The repeated frictional sliding in cyclic loading under
water absorption increases with increasing natural fatigue conditions. Three important parameters that
fiber volume fraction of composite. All three dimen- can affect the creep behavior of natural fiber com-
sions of composites increase by the fiber water posites are fiber loading, temperature, and styrene
absorption. Pressurization at low fiber volume frac- concentration [245]. A number of studies have
tions can improve the water absorption of natural assessed the effect of the creep on natural fiber
fiber composites. Chemical treatment of fiber surfaces composites. Alvarez et al. [246] investigated the
can also remove the hydrophilic OH bonds [85, 243]. influence of fiber content on the creep behavior of
Symington et al. [244] found that the mechanical random-oriented sisal fiber/starch composites man-
properties of flax and coir fiber composites decreased ufactured by injection molding technique through
more than those of kenaf, jute, and abaca fiber com- short-term flexural creep tests and found improved
posites under fully soaked conditions. They also creep resistance by an increased fiber content in the
showed that abaca and kenaf fibers had the highest matrix. Acha et al. [247] found the same result for a
capacity to absorb moisture (164% and 150% by woven jute fiber/polypropylene composite. Xu et al.
weight, respectively), which resulted in severe dam- [248] showed that a random-oriented bagasse fiber/
age to the structure of the fibers. Wear resistance PVC composite had better creep resistance than
refers to the ability of the composite materials to random-oriented bagasse fiber/HDPE composites
withstand scraping, skidding, rubbing, and sliding manufactured by extrusion molding technique at low
objects on its surface [233]. The extended exposure of temperatures. Amiri et al. [249] presented a time–
natural fiber composites to sunlight and UV radiation temperature superposition principal to generate a
results in physical and mechanical weakening of the creep compliance master curve for a flax fiber/viny-
composite [237]. lester composite. Yang et al. [250] reported that the
increase in banana fiber content up to 60% by weight
in a PLA matrix in the random-oriented direction
Time-dependent properties resulted in the highest creep resistance. The influence
of fiber treatment on the creep behavior of woven jute
Creep fiber/epoxy composite manufactured by hand lay-up
method was investigated by Militký and Jabbar [251]
The extended exposure of natural fiber composites to through a three-point bending test. They showed that
stress results in a decrease in the strength and elastic a plasma-treated fiber composite exhibited a lower
modulus of composites [1]. The damage mechanisms creep strain than an untreated fiber composite.
in composites due to creep result in fiber fracture,
J Mater Sci (2020) 55:829–892 865

Table 17 Summary of existing studies on the durability properties of natural fiber composites

Reference Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Masoodi and Woven jute fiber/epoxy 103a Compression 26% increase in the water absorption of the composite by
Pillai [27] composite molding incorporating 40% by weight jute fiber
Apolinario Unidirectional flax fiber/ 15 Infusion 9% decrease in the water uptake of 1% silane-treated fiber
et al. [230] polyester composite molding composite under saturation conditions
Assarar et al. Unidirectional flax fiber/ – Hand lay-up Water aging considerably decreased the elastic modulus (i.e.,
[231] epoxy composite 40%) and increased the elongation (i.e., 61%) of the
composite compared to the glass fiber composite
Lu and Unidirectional flax fiber/ 10 Vacuum- Composites made with non-dry fibers (with moisture content
Vuure polyester composite assisted resin of 10%) exhibited lower moisture absorption, degree of
[232] infusion swelling, and shrinking than those made with dry fibers
(dried in an oven at 80 °C)
Yousif and Random-oriented oil 350 Hand lay-up The use of fibers with length of 1–1.5 mm and diameter of
El-Tayeb palm fiber/polyester 350 lm significantly reduced the specific wear rate (i.e.,
[233] composite by about three to four times) of the neat polyester resin
El-Tayeb Random-oriented 1200–2700a Hand lay-up Longer fibers (* 5 mm) had higher wear resistance because
[234] sugarcane fiber/ less pulling-out of fibers occurs at that length. When the
polyester composite ends of the fibers in the matrix were perpendicular to the
counterface and the anti-sliding direction (i.e., anti-parallel
orientation), the composites exhibited higher wear
resistance as compared to other directions
Yousif [235] Coir fiber/polyester 215–304a Compression Coir fiber composite had higher wear resistance than
composite molding sugarcane and oil palm fiber composites
Chin and Unidirectional kenaf 250–400a Vacuum Presence of kenaf fibers oriented in the normal direction
Yousif fiber/epoxy composite bagging enhanced the wear performance of the resin by * 85%
[236]
Abu-Sharkh Random-oriented palm – Injection Reinforcement of polypropylene composite with palm leaf
and Hamid leaf fiber/polypropylene molding fiber increased the weathering stability of the composite as
[237] composite compared to composite without fiber, owing to the natural
antioxidant properties of lignin, which increased the
protection of the composite from UV radiation
Singh and Unidirectional jute fiber/ – Pultrusion Exposing the composite without any treatment to weathering
Gupta phenolic composite technique led to color fading, fibrillation, black spots, bulging, and
[238] resin cracking, as well as a 22% reduction in the flexural
strength of the composite after 2 years
Dash et al. Unidirectional jute fiber/ – Compression Bleaching reduced the effects of weathering
[239] polyester composite molding
Joseph et al. Random-oriented banana – Compression Alkalization and silane fiber modifications slowed the effects
[240] fiber/phenolic molding of weathering
composite
a
Diameter of a fiber bundle

Shrinkage The shrinkage of natural fibers generates internal

stresses at the fiber/matrix interface and causes
Rearranging and reorienting of resin molecules of damage and degradation of the initial properties of
composites in the liquid phase result in shrinkage [1]. the composite. The influential parameters on the
866 J Mater Sci (2020) 55:829–892

volumetric shrinkage of composites are the density, 3.5

Pure
processing conditions, flow pattern, shape, residual 3 5%, Untreated
internal stress, fiber content, crystallinity, and non- 5%, Treated
2.5 10%, Untreated

Shrinkage (%)
uniform cooling rates [4]. The use of fibers in the 10%, Treated
2
longitudinal direction, an increase in the fiber con-
tent, and a decrease in the residual internal stress, 1.5
non-uniform cooling rates, and the crystallinity of the 1
composites all decrease the shrinkage of natural fiber
0.5
composites [252–254]. Figure 29 shows the shrinkage
0
behavior of a random-oriented coir fiber/PLA com-
0 30 60 90 120 150 180
posite manufactured by compression molding tech- Time (min)
nique over time at 80 °C for the longitudinal and (a)
transverse directions of the composite, in which 6
fibers were subjected to plasma treatment with 0%, Pure
5%, Untreated
5%, and 10% fiber content by weight in the composite 5
5%, Treated
[173]. A limited number of studies investigated the 10%, Untreated

Shrinkage (%)
4
10%, Treated
shrinkage behavior of natural fiber composites. San-
3
tos et al. [255] reported that the shrinkage of a ran-
dom-oriented bamboo fiber/HDPE composite 2
manufactured by injection molding technique was
1
reduced up to 58% by an increased fiber content in
the composite. Tan et al. [256] assessed the shrinkage 0
behavior of random-oriented coir fiber/polypropy- 0 30 60 90 120 150 180
Time (min)
lene composites manufactured by injection molding
(b)
technique and found a 13% reduction in the volu-
metric shrinkage of the composite with a 40% Figure 29 Shrinkage behavior of random-oriented untreated and
increase in the fiber content by weight. plasma-treated-coir fiber/polylactic acid composite manufactured
by compression molding technique at 80 °C over time for
a longitudinal and b transverse directions of the composite.
Other properties
natural fiber composites can be improved [257]. The
Thermal properties use of coatings and additives, such as ceramic, intu-
mescent, silicone, phenolic, ablative, and glass mats,
Fire resistance also improves the fire resistance of natural fiber
composites. Heating intumescent materials beyond a
The flammability behavior of natural fiber compos- specific temperature results in the formation of the
ites has become one of the most important issues in cellular and charred surface by initiation of foaming
recent years because of the use of natural fiber com- and expanding, which in turn can protect the
posites in different applications [1]. One of the underlying surface from heat and flame. By adding
weaknesses of natural fiber composites is the loss of talc and nanoparticles as fillers to the natural fiber
strength and stiffness at high temperatures [257]. composites, the fire resistance of the composites
Thermal decomposition and combustion occur when increases by the formation of heat barriers. Several
natural fiber composites are exposed to fire or any researchers have studied the behavior of natural fiber
other high-intensity heat sources [4]. The flammabil- composites at high temperatures. Some studies
ity of natural fiber composites is variable for different reported that natural fibers generally start to degrade
types of natural fibers because they have different at approximately 240 °C [31, 258–260]. However,
chemical compositions and microstructures. By lignin starts to degrade at approximately 200 °C and
decreasing the cellulose content of natural fiber, hemicellulose and cellulose start to degrade at higher
increasing the crystallinity, and decreasing the poly- temperatures [261]. Table 18 presents the decompo-
merization of the composites, the fire resistance of the sition temperature of major natural fibers, and
J Mater Sci (2020) 55:829–892 867

Table 18 Decomposition temperature of major natural fibers 0.4

Thermal conductivity (w/m°k)

0.363
[259, 262]
0.3
Fiber Decomposition temperature (°C) 0.251 0.243 0.239
0.230 0.231 0.228
Bagasse 232 0.2
Bamboo 224
Cotton 232 0.1
Hemp 215
Jute 215
0
Kenaf 229 Epoxy Jute Banana Jute Banana Jute Banana
resin 30% 30% 40% 40% 60% 60%
Rice straw 238
Rice husk 234
Figure 30 Thermal conductivity of epoxy resin, and jute and
Pina 240
banana fiber/epoxy composites with different fiber contents.

composites manufactured by hand lay-up method

and reported that the thermal conductivities of the
Table 19 presents glass transition and melting point jute and banana fiber composites were 0.231 and
of major resins used in natural fiber composites. 0.228 W/m K in the - 20 °C to 300 °C range and at
the maximum fiber volume fraction, respectively.
Thermal conductivity Figure 30 shows the thermal conductivity of natural
fiber composites with different fiber contents [264].
The use of heat-insulating materials is an appropriate
Paul et al. [204] reported that an increase in fiber
approach for reducing energy costs and improving
loading decreased the thermal conductivity of a
manufacturing efficiency in industries such as auto-
random-oriented banana fiber/polypropylene com-
motive, construction, and packaging [1]. Natural
posite manufactured by compression molding tech-
fibers contain lumens, hollow portions filled with air.
nique. The thermal conductivity of a random-
As a result, the thermal conductivity of composites
oriented flax fiber/HDPE composite manufactured
decreases with an increased fiber content. By an
by extrusion molding technique was assessed by Li
increased natural fiber volume fraction of the com-
et al. [265]. They found that the thermal conductivity
posites, the amount of air contained in the composite
of the composite reduced with increasing fiber con-
increases, which results in heat insulation. Several
tent. Mangal et al. [266], Osugi et al. [267], Mounica
studies have been performed to investigate the ther-
et al. [268], and Ramanaiah et al. [269] found the same
mal conductivity of natural fiber composites. Pujari
result for random-oriented pina fiber/phenolic
et al. [264] studied the thermal conductivity of ran-
manufactured by compression molding technique,
dom-oriented jute and banana fibers/epoxy
unidirectional hemp fiber/epoxy manufactured by

Table 19 Glass transition

temperature and melting point Resin Glass transition temperature (°C) Melting point (°C)
of major resins [243, 263]
Polypropylene 0.9–1.55 160–176
Low-density Polyethylene - 120 105–116
High-density Polyethylene - 80 120–140
Polystyrene 100–135 –
Nylon 6 40 222
Nylon 6,6 50 250–269
Polyester 60 250–300
Vinylester 104–121 –
Epoxy 70–167 –
Phenolic 170 –
Starch 60 110–115
PLA 58 150–162
PHA 2–15 160–175
868 J Mater Sci (2020) 55:829–892

Thermal analysis

Thermogravimetry analysis (TGA), differential scan-

ning calorimetry (DSC), and differential thermal
analysis (DTA) were used to analyze the thermal
behavior of natural fiber composites. Feng et al. [271]
assessed the thermal behavior of random-oriented
kenaf fiber/polypropylene composite manufactured
by injection molding technique through DSC and
Polylactic acid
Sisal fiber reported that maleated coupling agent reduced the
1% Fiber/Composite
2% Fiber/Composite
melting temperature of the composite. Joseph et al.
3% Fiber/Composite [87] used TGA and DSC to study the thermal
behavior of random-oriented sisal fiber/polypropy-
lene composite. They found that incorporation of
(a) sisal fiber with fiber weight fraction of 20% treated by
maleic anhydride-modified polypropylene, urethane
derivative of polypropylene glycol, and KMnO4,
respectively, caused 12%, 11%, and 9% increase in the
crystallization temperature of the composite com-
pared to that with no fiber, which was because the
surface of the treated fibers acted as nucleating sites
for the crystallization of the polymer. Mofokeng et al.
[272] assessed the thermal stability of random-ori-
ented sisal fiber/PLA and sisal fiber/polypropylene
composites manufactured by injection molding tech-
Polypropylene
Sisal fiber nique through TGA and their crystallization through
1% Fiber/Composite
2% Fiber/Composite
DSC. Figure 31 shows the TGA curves of composites
3% Fiber/Composite with fiber weight content of 1, 2, and 3%. They found
that the thermal stability of both polymers increased
with an increased fiber content, with a more signifi-
(b) cant improvement in the case of polypropylene. Fig-
ure 32 shows the DSC curves of composites. The DSC
Figure 31 TGA curves of sisal fiber composites with a polylactic
results in the figure illustrated a significant influence
acid and b polypropylene resin [272].
of the fibers on the cold crystallization and melting
compression molding technique, unidirectional behavior of PLA. They also reported that fiber con-
bamboo fiber/polyester manufactured by hand lay- tent had a negligible influence on the melting char-
up method, and unidirectional fish tail palm fiber/ acteristics of the polypropylene, but it had a
polyester composites manufactured by hand lay-up significant influence on the non-isothermal crystal-
method, respectively. Agarwal et al. [270] assessed lization temperature range. In 2013, Azwa and Yousif
the influence of fiber treatment on the thermal con- [273] studied the thermal stability of random-ori-
ductivity of an oil palm fiber/phenolic composite. ented untreated and 6% alkaline-treated kenaf fiber/
They found that alkali and silane treatments epoxy composite. Figure 33 shows TGA and DTA
increased the thermal conductivity of the composite curves presented in that study [273]. They reported
more than acetylation treatment, meaning that that the addition of the kenaf fiber into the epoxy
acetylation treatment was more suitable than alkali slightly improved both the charring and the thermal
and silane treatments for improving the heat-insu- stability of the composite. They also reported that
lating characteristics of the composite. untreated kenaf fiber/epoxy composite started to lose
weight earlier compared to the other composites,
which was because of the higher moisture content of
the untreated fibers.
J Mater Sci (2020) 55:829–892 869

Polylactic acid
Viscoelastic properties
1% Fiber/Composite Melting temperature
2% Fiber/Composite
3% Fiber/Composite Polymers are normally viscoelastic fluids that behave
Glass transition temperature as a viscous or elastic material depending on the rate
of flow or deformation [274]. Dynamic mechanical
analysis has been widely utilized to investigate the
viscoelastic properties (storage modulus, loss modu-
lus, and damping factor) of composites [11]. Dynamic
mechanical analysis is a technique that a small
deformation is cyclically applied to a sample under
different temperatures, and the elastic and viscous
response of the sample is then monitored. In this
technique, a sinusoidal force is applied to the sample
at a set frequency and the stiffness and damping of
(a)
the sample are measured [275]. The in-phase com-
ponent, out-of-phase component, and the ratio of the
Polypropylene
1% Fiber/Composite loss of the storage are defined as storage modulus,
2% Fiber/Composite
3% Fiber/Composite loss modulus, and damping factor, respectively.
Melting temperature
Pothan et al. [275] investigated the influence of the
fiber content on the dynamic mechanical properties
of random-oriented banana fiber/polyester compos-
ite manufactured by compression molding technique.
They showed that an increase in the fiber volume
fraction up to 40% led to a decrease in the storage
modulus of the composite below the glass transition
temperature, but an increase in the storage modulus
above the glass transition temperature. They also
reported that, at 40% fiber content, the peak loss
modulus got broadened and peak damping factor
(b) lowered, indicating the improved fiber/matrix
adhesion. Idicula et al. [276] assessed the viscoelastic
properties of random-oriented banana/sisal hybrid
fiber/polyester composite manufactured by com-
pression molding technique and reported that the
storage modulus of the composite enhanced above
the glass transition temperature of the polymer with
an increase in the fiber volume fraction up to 40% and
Crystallization temperature
then decreased. Pan et al. [277] studied the storage
modulus of random-oriented kenaf fiber/PLA com-
Polypropylene
1% Fiber/Composite
posite manufactured by melt mixing technique and
2% Fiber/Composite reported that the storage modulus increased by 28%
3% Fiber/Composite
by reinforcement of the composite with 30% kenaf
fiber by weight. Mofokeng et al. [272] investigated the
viscoelastic properties of random-oriented sisal
(c)
fiber/PLA and sisal fiber/polypropylene composites
Figure 32 DSC curves of sisal fiber composites with a polylactic manufactured by injection molding technique
acid (heating curves), b polypropylene (heating curves), and through dynamic mechanical analysis. Figures 34
c polypropylene (cooling curves) resin [272]. and 35 show the storage modulus (E0 ), loss modulus
(E00 ), and damping factor (tand) curves of composites
with PLA and polypropylene, respectively [272].
870 J Mater Sci (2020) 55:829–892

Figure 33 a TGA and b DTA

curves of random-oriented
untreated and 6% alkaline-
treated kenaf fiber/epoxy
composites [273].

They reported that the storage and loss modulus of polypropylene composite (shown in Fig. 35a, b),
the PLA decreased with an increase in the fiber which was because of the restriction in the segmental
content (shown in Fig. 34a, b). They also reported motion. The existence of fibers had no impact on the
that the cold crystallization of the PLA was around a-relaxation of the composite (shown in Fig. 35c),
110 °C and the existence of the fibers in the composite which was related to the crystalline fraction of the
led to an increase in the modulus between the cold polypropylene. Mylsamy and Rajendran [278] per-
crystallization and melting of the polymer (shown in formed dynamic mechanical analysis on untreated
Fig. 34b). The larger area under the a-relaxation peak and alkaline-treated unidirectional agave fiber/
in Fig. 34c indicates that the molecular chains epoxy composite manufactured by compression
exhibited a higher degree of mobility, therefore better molding technique and reported that the composite
damping properties. The presence of fibers increased with poor interfacial bonding tended to dissipate
the modulus and glass transition temperature of
J Mater Sci (2020) 55:829–892 871

more energy compared to those with good interfacial

bonding.
Glass transition
temperature Morphology
α-relaxation Cold crystallization
region region Optical microscopy, SEM, and atomic force micro-
scopy (AFM) are three main methods for morpho-
logical studies of composites. Optical microscopy is
ideal for general inspection purposes, and SEM pro-
Polylactic acid
1% Fiber/Composite vides detailed topographical and compositional
2% Fiber/Composite
3% Fiber/Composite information of the composite by high magnification
view at micro-scale [277]. On the other hand, AFM is
a useful method to determine the surface roughness
(a) of fibers at nanoscale by measuring the interatomic
forces between the sample surface and the measure-
ment tip [10]. A large number of studies investigated
the morphology of natural fiber composites (e.g.,
Glass transition
temperature [275, 277, 279]). Some of these studies are presented
in this review paper.
Pothan et al. [275] assessed the influence of the
fiber content on the morphology of random-oriented
banana fiber/polyester composite manufactured by
compression molding technique through SEM. Fig-
Polylactic acid ure 36a–c shows SEM micrographs of composites
1% Fiber/Composite
2% Fiber/Composite with fiber volume fractions of 10, 20, and 40%,
3% Fiber/Composite
respectively. They reported that there was a good
fiber/matrix bonding in the composite with 40% fiber
content, whereas fiber/matrix debonding was evi-
(b) dent in composites with 10% and 20% fiber content.
They also showed that there was no gap between the
Polylactic acid
1% Fiber/Composite fibers and matrix in 40% fiber composite owing to the
2% Fiber/Composite
3% Fiber/Composite strong bonding. However, when the fiber concentra-
α-relaxation
peak tion was lower, the packing of the fibers was not
efficient, leading to an easier failure of the bonding at
the interfacial region.
Cold crystallization
Pan et al. [277] studied the morphology of random-
region oriented kenaf fiber/PLA composite manufactured
by melt mixing technique using SEM. Figure 37
shows the SEM micrographs of kenaf fiber [277]. It
can be seen in the figure that the diameter of the
fibers ranged from 5 to 50 lm and their surface was
rough with the adhesion of some smaller fibers. This
was attributed to different sources and processing
(c) history of the kenaf fibers. Figure 38 shows the SEM
micrographs of pure PLA and composite with 30%
Figure 34 Dynamic mechanical analysis of random-oriented sisal
fiber/polylactic acid composite manufactured by injection molding kenaf fiber by weight [277]. The fractured surface of
technique: a storage modulus, b loss modulus, c damping factor the pure PLA was irregular and rough because of the
[272]. brittle behavior of the resin. It is also shown in the
figure that most fibers (indicated by ‘‘A’’) were tight
connected to the matrix, and a lot of fibers were
872 J Mater Sci (2020) 55:829–892

broken during the tensile testing. It can be seen in

Fig. 38 that there are some fibers in the composite
(indicated by ‘‘B’’) separated from the matrix during
the tensile deformation, indicating that the interface
interaction between the matrix and fibers further
improved. Aggregation of kenaf fibers (indicated by
‘‘C’’) and the presence of a small amount of air bub-
bles (indicated by ‘‘D’’) are also visible in the figure,
which was because of the rough surface of kenaf fiber
Polypropylene and high viscosity of the PLA.
1% Fiber/Composite
2% Fiber/Composite Hebel et al. [279] investigated the morphology of
3% Fiber/Composite
unidirectional bamboo fiber/epoxy composite man-
ufactured by compression molding technique pro-
duced by a combination of heat and pressure
(a)
treatment through optical microscopy. Figure 39a–c
Glass transition
shows the optical micrographs of the fractured sur-
temperature face of the autoclave/compression molded compos-
ites produced at 100 °C with pressures of 15, 20, and
25 MPa [279]. It should be noted that the composite
produced by pressure of 20 MPa exhibited a higher
tensile strength than that by 15 and 25 MPa. They
reported that the surface of the composite at 20 MPa
pressure was rather smooth and homogenously
covered by the resin. At this pressure, the polymer
Polypropylene network formed a very thin layer that efficiently
1% Fiber/Composite
2% Fiber/Composite interacted with the surface of the fiber and penetrated
3% Fiber/Composite
into the fibers due to its viscosity. They also reported
that reducing the pressure to 15 MPa resulted in the
formation of large resin beads on the fiber surface,
(b)
which led to the reduction in the wetting and
homogenous coverage of the fibers. At high pressures
Polypropylene
1% Fiber/Composite α-relaxation of 25 MPa, the epoxy formed larger crystal-like beads
2% Fiber/Composite
3% Fiber/Composite than those at 15 MPa and infiltration inhibited by a
propagated carbonization of the fibers (as shown by
Glass transition
the darker color strip).
temperature Lee et al. [280] used AFM to characterize the kraft
fiber treated by Trichoderma reesei enzyme. Fig-
ure 40 shows tapping mode AFM images of treated
kraft fiber and its cellulose aggregate fibrils. The
cellulose microfibril bundles are evident in Fig. 40a,
which can be a potential source for cellulose aggre-
gate fibrils. Several structural imperfections such as
kinks and twists are evident in Fig. 40b that were
because of the conformability of fibers in the treat-
(c) ment process by the removal of the constraining
Figure 35 Dynamic mechanical analysis of random-oriented sisal primary layer of the kraft fiber. George et al. [281]
fiber/polypropylene composite manufactured by injection molding used AFM to investigate the influence of the fiber
technique: a storage modulus, b loss modulus, c damping factor treatment on the nanostructure of the hemp fiber.
[272]. They reported that fiber treatment rendered the sur-
face topography of the hemp fiber clean and exposed
J Mater Sci (2020) 55:829–892 873

Figure 36 SEM micrographs Fiber/matrix

of random-oriented hemp
Fiber pull-out debonding
fiber/polyester composite with
fiber content of a 10%, b 20%,
and c 40% manufactured by
compression molding
technique [275].

Fiber/matrix Matrix
debonding cracking

(a) (b)

(c)

Figure 37 SEM micrographs

of kenaf fiber with
magnification of a 9 100 and
b 9 500 in random-oriented
kenaf fiber/polylactic acid
composite manufactured by
melt mixing technique [277].

100μm 50μm

(a) (b)

the individual fiber bundles. They also showed that interacting within natural fibers, characterizing their
hemp fibers treated by 10% NaOH, xylanase enzyme, covalent bonding information [26]. Table 20 presents
and laccase enzyme had 250%, 218%, and 16% higher the FTIR analysis peaks for different untreated nat-
surface adhesion forces than those with no treatment. ural fibers. Lu et al. [293] investigated the spectro-
scopic characteristics of the benzylated-treated sisal
Spectroscopic characterization fiber by FTIR and reported that peaks at 1250 cm-1
and 1363 cm-1 related to lignin and hemicellulose
Fourier transform infrared spectroscopy (FTIR) is an partly removed by treatment of the sisal fiber.
effective technique to determine the chemical com- Mofokeng et al. [272] used FTIR analysis to determine
position of the composite and functional groups the existence and type of interfacial interaction in
874 J Mater Sci (2020) 55:829–892

Figure 38 SEM micrographs

of fractured surface of a pure
polylactic acid, and random-
oriented kenaf fiber/polylactic
acid composite with
magnification of b 9 200,
c 9 500, and d 9 500 D
manufactured by melt mixing
technique [277]. C

50μm 100μm

(a) (b)

A
B

50μm 50μm

(c) (d)

random-oriented sisal fiber/PLA composite manu- damaged the fiber surface, leading to the poor fiber
factured by injection molding technique (shown in adhesion and worse mechanical properties of the
Fig. 41). Peaks at 1780–1680 cm-1, 3600–3000 cm-1, composite. Faruk Hossen et al. [295] by FTIR analysis
and 1180 cm-1 corresponded to C=O, O–H, and C– on the propionic anhydride-treated random-oriented
O–C stretches, respectively. They reported that the jute fiber/polyethylene composite manufactured by
O–H band of the composite became more pro- compression molding technique reported that the
nounced and broader with an increase in the fiber band at 1641 cm-1 indicated absorbed water in
content, which was because of the existence of free crystalline cellulose and the band disappeared upon
OH groups in the fiber. They also reported that a new the fiber treatment. They also reported that the band
peak at 1650 cm-1 was created corresponded to OH, at 1512 cm-1 was because of the existence of the
which was oriented from bending of the unresolved aromatic rings in lignin.
OH group of the absorbed water by cellulose. Ala-
vudeen et al. [294] conducted FTIR analysis on the
alkaline- and sodium lauryl sulfate (SLS)-treated Incorporation of nanoparticles in natural
random-oriented banana fiber/epoxy composite fiber composites
manufactured by hand lay-up method. They reported
that fiber treatment removed most of the lignin and Nanoparticles have been utilized as nanofiller mate-
hemicellulose components on the fibers, which rials to improve the properties of natural fiber com-
helped to improve the mechanical properties of the posites [296]. Owing to the high surface area (higher
composite. They also found that an increase in the than 500 m2/g) and pore filling properties of
concentration of alkaline and SLS beyond 10% nanoparticles, the properties of natural fiber com-
posites were enhanced by addition of a small amount
J Mater Sci (2020) 55:829–892 875

Figure 39 Optical
micrographs of the fracture
surface of
autoclave/compression molded
unidirectional bamboo fiber/
epoxy composite produced at
100 °C with pressure of
a 15 MPa, b 20 MPa, and
c 25 MPa [279].

(up to 5% by weight) of nanofillers in natural fiber biomedical industries owing to the eco-friendliness,
composites [297]. A few studies investigated the lightweight, good mechanical behavior, sound
properties of natural fiber composites containing attenuation, and vibration damping of them
nanofillers. Table 21 presents a summary of the [15, 17, 243, 303]. However, their low durability may
existing studies of the influence of nanofillers on the exclude them from being an alternative to glass fiber-
properties of natural fiber composites [298–302]. reinforced composites in wet areas such as in piping,
boats, and kayaks [243]. Henry Ford made the first
attempt to use natural fibers in the automotive
Application of natural fiber composites industry using flax and hemp fibers in 1941 [43].
Many automotive companies are now using natural
Natural fiber composites have been utilized in the fiber composites made with polyester, polypropy-
automotive, construction, aircraft components, pack- lene, flax, hemp, and sisal [304]. In structural appli-
aging, sporting equipment, electrical parts, and cations, natural fiber composites have been utilized to
876 J Mater Sci (2020) 55:829–892

Figure 40 Tapping mode

AFM images of a kraft fiber
treated by Trichoderma reesei
enzyme and b its cellulose
aggregate fibrils [280].

develop load-bearing elements, such as beam, roof, the use of environmentally friendly products in
wall, and pedestrian bridge [305, 306]. Jute fiber/ industry. The global natural fiber composite market
polypropylene composite has been used in primary share by the end-use industries in 2016 was 35%,
structural applications, such as indoor elements in 27%, 9%, 13%, and 16% for transportation, building
housing [1, 28], temporary low-cost outdoor housing and construction, consumer goods, electrical and
for defense and rehabilitation [29, 30], and trans- electronics, and other applications, respectively [311].
portation [307]. Yousif and Ku [308] investigated the Based on this report and recent reports by Dicker
behavior of a liquid storage tank made with coir et al. [243] and Gurunathan et al. [3], the automotive
fiber/polyester composite and reported that the and construction industries were the biggest market
interfacial adhesion strength between coir fiber and for natural fiber composites in 2016–2017 to manu-
polyester resin soaked in water and diesel oil was facture seat backs, headliners, truck liners, door
107 MPa. They suggested the potential application of panels, decking, railing, window frames, dash
the coir fiber/polyester composite in design and boards, and frames. Because of the rapid growth of
manufacture of the body of liquid storage tanks. the use of natural fiber composites in the automotive
Natural fiber composites have also been used in market, high-density glass fibers are being replaced
functional applications of protective medical appar- with low-density natural fiber composites; light-
els, such as baby diapers, feminine hygiene products, weight vehicles reduce the amount of the fuel
and adult incontinence items, plasters, bike frames, required, which in turn leads to a reduction of CO2
golf stick, tennis rackets, and helmets [309]. emission [3]. The study by Yang et al. [312] revealed
According to the reports by MarketsandMarkets that a 25% reduction in the weight of an automobile
Inc. [310] and Grand View Research Inc. [311], the would result in a 220 billion pound reduction in CO2
natural fiber composite market was valued at $16.5 emission per annum. Germany is a leader in the use
billion in 2016 and is projected to reach $46.3 billion of natural fiber composites in automotive industry.
by 2025, because of the governmental regulations for The automotive companies in Germany, such as
J Mater Sci (2020) 55:829–892 877

Table 20 FTIR peaks of different natural fibers (in cm-1)

Reference Fiber OH C–H C=O CH2 C–O Bending b- C–OH

stretching stretching stretching symmetric stretching vibration of C– glycosidic bending
bending C-vibration of H and C–O linkages
acetyl group groups of
in lignin and aromatic ring in
hemicellulose polysaccharides

Mwaikambo Sisal 3447 – 1737 1384 – – – –

and Ansell
[207]
Keshk et al. Kenaf 3397 2902–2918 – 1416 – 1036 – –
[282]
Bilba et al. Banana 3600–3100 2910 – 1416 – 1036 – –
[283]
Spinace et al. Curaua 3200–3500 2750–2900 1740 – 1240 – – –
[284]
Saha et al. Jute 3200–3600 2910 1739 1430 1294 – – –
[285]
Sawpan et al. Hemp 3410 2916 1732 1425 1247 – 892 –
[286]
De Rosa Okra 3100–3600 2854–2925 1734 1430 1243–1384 1320–1370 894 598
et al. [287]
Fiore et al. Artichoke 3342 2854–2923 1737 1422 – 1318–1372 892 589
[288]
Arrakhiz Coir 3330 2910 1725 1420 1235 – – –
et al. [289]
Reddy et al. Borassus 3435 2851–2920 1746 – 1254 1058 893 –
[290]
Neto et al. Pina 3450 2900 1730 – 1260 1050 – –
[291]
Al–Maadeed Palm leaf 3300 2946 1735 – – – – –
et al. [292]

Mercedes, BMW, Audi, and Volkswagen, have taken composite market are FlexForm Technologies (USA),
the initiative to use natural fiber composite for inte- Tecnaro GmbH (Germany), Trex Company Inc.
rior and exterior applications because natural fiber (USA), Fiberon LLC (USA), Meshlin Composites ZRT
composite components are lightweight, impact (Hungary), UPM (Finland), Jelu-Werk J. Ehrler
resistant, nontoxic, and no-sharp edged fracture in GmbH & Co. KG (Germany), Green Bay Decking
the case of a crash. (USA), Universal Forest Products Inc. (USA), Toray
Asia Pacific (especially China, India, South Korea, Industries Inc. (Japan), and Owens Corning (USA).
Thailand, and Indonesia) is expected to have the Table 22 summarizes the applications of natural fiber
fastest-growing market for natural fiber composites composites based on different properties.
during the next 5 years owing to the increasing
demand from the transportation, building, and con-
struction [310]. The European Union’s ban on non-
recyclable plastic is expected to drive the market in
the Europe region. Based on the report by Global
Biocomposite Market in 2018 [313], some of the cur-
rent leading companies in the global natural fiber
878 J Mater Sci (2020) 55:829–892

Life-cycle assessment of natural fiber

composites

Figure 42 shows the life cycle of a natural fiber

composite [19]. The fully environmental superiority
of natural fiber composites than that of synthetic
composites is still questionable due to the relative
excessive processing requirements of natural fiber
composites. Therefore, careful life-cycle assessment
(LCA) is necessary before natural fiber composite is
used commercially [4]. LCA is part of ISO14000 series
of Environmental Management System (EMS) and
determines the overall potential impact of natural
fiber composites on the environment throughout the
whole life cycle from extraction of raw materials to
Figure 41 FTIR spectra of random-oriented sisal fiber/polylactic
end-of-life stage. A number of LCA studies have been
acid composite manufactured by injection molding technique
[272]. conducted to date on natural fiber composites. The
first LCA study on natural fiber composites was
performed by Wotzel et al. [314] on hemp fiber/
epoxy composite and acrylonitrile butadiene styrene
(ABS) for production of automotive side-panel com-
ponent of passenger cars through cradle-to-grave life-
cycle approach. They reported that the cumulative

Table 21 Summary of existing studies on the effect of nanofiller on the properties of natural fiber composites

Reference Composite Apparent Manufacturing Observation

fiber method
diameter
(lm)

Huang and Unidirectional flax 237a Resin transfer 13%, 4%, 8%, 24%, and 17% increase in tensile strength,
Netravali fiber/soy protein molding tensile strain, tensile modulus, flexural strength, and
[298] composite flexural modulus of composite with fiber volume fraction
of 48% incorporating 5% nanoclay, respectively
Sen and Random-oriented coir – Compression The smoke density and limiting oxygen index (as fire
Kumar fiber/epoxy composite molding retardancy properties), respectively, 28% decreased and
[299] 26% increased when the composite contained 1.6% coir
nanofiller
Alamri and Random-oriented recycled 200a Compression 19%, 27%, and 34% decrease in water absorption
Low [300] cellulose fiber/epoxy molding incorporating 1%, 3%, and 5% nanoclay (by weight),
composite respectively. 7%, 3%, and 23% enhancement in the flexural
strength, modulus, and toughness incorporating 5%
nanoclay, respectively
Lim et al. Random-oriented Napier – Resin infusion 163% increase in flexural strength incorporating 3%
[301] grass fiber/epoxy nanoclay. 180% increase in flexural modulus incorporating
composite 5% nanoclay
Ashik et al. Cross-plied jute fiber/ – Compression 60%, 17%, and 12% increase in tensile strength, flexural
[302] epoxy composite molding strength, and damage index of the composite incorporating
5% nanosilica, respectively
a
Diameter of a fiber bundle
J Mater Sci (2020) 55:829–892 879

Table 22 Application areas of natural fiber composites based on their properties [13, 243]

Properties Suitable application

High strength and low Transportation (such as aircraft, automobile), mobile electronics, sport equipment, construction and building,
weight storage devices (such as grain storage silos, bio-gas containers)
Renewability Short-life-span products such as plastic cutlery, packaging, toys, and electronic products of computers, phones,
faxes, radios, stereos, CD players
Non-toxicity Toys, hobbyist-built items, consumer-handled items
Biocompatible Medical devices and implants
Low cost Competitive consumer products such as window and door frames, furniture, railroad sleepers, automotive
panels, gardening items, shelves, noise insulting panels, and packaging
High water absorption Dry-use products
Weak durability Short-life-span products, limited exposure to harsh environments

energy demand of hemp fiber/epoxy composite was superior from an environmental energy point of view
45% lower than that of ABS. Table 23 presents the to spun flax yarn.
summary of the LCA studies on natural fiber com-
posites. The existing LCA studies revealed that nat-
ural fiber composites have superior environmental Conclusions
performance than composites with synthetic fiber or
resin. However, cradle-to-gate LCA studies of flax, as The properties of easy accessibility, low density, low
an agrochemical-based material, and glass by Dis- price, good thermal and acoustic insulation, eco-
sanayake et al. [321, 322] reported that flax sliver is friendliness, recyclability, renewability, and satisfac-
comparable in energy terms to glass fiber mat, and tory mechanical properties make natural fiber com-
continuous glass fiber reinforcement appears to be posites an attractive alternative to carbon, glass, and
other synthetic fiber composites. Natural fiber com-
posites are currently being used in the construction

Figure 42 Life cycle of a

typical natural fiber-reinforced
composite [19].
880 J Mater Sci (2020) 55:829–892

Table 23 Summary of some of the studies on life-cycle assessment (LCA) of natural fiber composites

References Composite Application Life-cycle approach Results

Wotzel Hemp fiber/epoxy versus ABS Side-panel Cradle-to-grave Cumulative energy demand of hemp fiber/
et al. component for epoxy composite was 45% lower than that of
[314] passenger car ABS
(Audi A3)
Mussig Hemp fiber/Triglycerides and Bus body Cradle-to-grave Composite with PTP had 65% and 39% lower
et al. polycarbon acid anhydrides component energy demand and global warming potential
[315] (PTP) versus hemp fiber/ than those with polyester, respectively
polyester
Zah et al. Curaua fiber/polypropylene Automotive Cradle-to-grave Curaua fiber/polypropylene composite had
[316] versus glass fiber/ internal 75% and 66% lower climate change and
polypropylene component ozone depletion potential than those of glass
fiber/polypropylene, respectively
Schmehl Hemp fiber/PTP versus glass Bus body Cradle-to-grave Hemp fiber/PTP composite had 54% and 44%
et al. fiber/polyester component lower global warming and climate change
[317] potential than those of glass fiber/polyester,
respectively
Luz et al. Sugarcane bagasse fiber/ Vehicle interior Cradle-to-grave Sugarcane bagasse fiber/polypropylene had
[318] polypropylene versus talc/ aesthetic 20% and 25% lower energy demand and
polypropylene covering global warming impact than those of talc/
component polypropylene, respectively
Wang Kenaf fiber/soy-based resin Sheet molding Cradle-to-gate Kenaf fiber/soy-based resin composite had
et al. versus glass fiber/polyester compound 58%, 13%, 97%, and 22% lower global
[319] material warming, ozone depletion, hedgehog cancer,
and ecotoxicity potential than those of glass
fiber/polyester composite, respectively
LaRosa Hybrid glass-hemp fiber/epoxy Elbow fittings for Cradle-to-grave Hybrid glass-hemp fiber/epoxy composite had
et al. versus glass fiber/epoxy the seawater 18%, 19%, 20%, and 20% lower global
[320] cooling pipeline energy requirement, global warming
potential, ecotoxicity, and life cycle cost than
those of glass fiber/epoxy composite,
respectively

and building, packaging, transportation, military, properties of natural fiber composites, which points
sporting equipment, and medical industries in an to the feasibility of using these composites as an
effort to reduce greenhouse gas emissions, and it is alternative material in a wide range of applications.
anticipated that this type of composite will be The review presented here will help researchers to
extensively used in other applications in the near better understand various properties of natural fiber
future. However, their drawbacks, such as poor composites to facilitate the development of new
interfacial adhesion between the natural fibers and green materials with improved performance. Based
the matrix, moisture absorption, poor fire resistance, on this review, further investigations are recom-
low impact strength, and low durability, have at least mended to investigate the influence of matrix modi-
partly prevented them from being considered a reli- fication and fiber length on the properties of natural
able alternative for conventional composites. This fiber composites.
paper has presented an up-to-date and all-encom-
passing review on the properties of natural fiber Compliance with ethical standards
composites. It has been shown that the use of modi-
Conflict of interest Both authors declare that they
fication techniques can lead to improved physical,
have no conflict of interest.
mechanical, durability-related, and time-dependent
J Mater Sci (2020) 55:829–892 881

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