Biopolymer Composites A Review

International Journal of Biobased Plastics
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Biopolymer composites: a review
Basheer Aaliya, Kappat Valiyapeediyekkal Sunooj & Maximilian Lackner
To cite this article: Basheer Aaliya, Kappat Valiyapeediyekkal Sunooj & Maximilian Lackner
(2021) Biopolymer composites: a review, International Journal of Biobased Plastics, 3:1, 40-84,
DOI: 10.1080/24759651.2021.1881214
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INTERNATIONAL JOURNAL OF BIOBASED PLASTICS
2021, VOL. 3, NO. 1, 40–84
https://doi.org/10.1080/24759651.2021.1881214
REVIEW ARTICLE
Biopolymer composites: a review

a a b
Basheer Aaliya , Kappat Valiyapeediyekkal Sunooj and Maximilian Lackner
a
Department of Food Science and Technology, Pondicherry University, Puducherry, India; bUniversity of
Applied Sciences FH Technikum Wien, Höchstädtplatz, Vienna, Austria
ABSTRACT ARTICLE HISTORY

In spite of the fact that a prodigious portion of petroleum covers Received 18 September 2020
multitudinous products in the commercial world, its non- Accepted 21 January 2021
biodegradable characteristic is an unenviable factor. The utilization KEYWORDS
of biodegradable polymers or biopolymers is a prominent alterna Biodegradable; biopolymer;
tive to petroleum-based plastic products. Reinforcing natural fibers natural fiber; interfacial
to biopolymer matrices significantly improves the properties of bonding; hybrid composite;
prepared plastic products. Such biopolymer composites have automotive sector
been developed by researchers to provide environmentally respon
sible materials and thereby reduce carbon footprint. Modification or
functionalization of natural fibers is important to ameliorate the
interfacial bonding with biopolymers, and to successfully obtain
high-performance composite materials that can compete with con
ventional petrochemical-based polymer composite counterparts.
Another widely accepted composite development technique is by
combining different types of fibers into a single matrix to develop
highly valued hybrid composites. The review focuses on the extrac
tion, processing and characterization of bio-based materials; natural
fibers and biopolymers, and their synergistic application and future
scope as biopolymer composites in automotive and other growing
sectors.
Introduction
Petroleum-based plastics have found their way into our routine livelihood as it showed
the potential to replace various traditional materials in varied applications. Fiber-
reinforced polymer composites are progressively equipped in high-end applications,
such as automobiles, aerospace, and medical science. Apart from this monetary domain,
most of the petroleum-driven materials give rise to an untenable environment. So an
alternative way to develop environmentally safe products is to use bio-based materials.
Bio-based materials are the ones whose building blocks constitute the substances pro
cured from living matter. Natural fibers reinforced biopolymers are known as “green
composites”. It is an environmentally degradable biopolymer composite that can be
degraded by the action of environmental factors such as air, light, heat, or microorgan
isms. Despite low stiffness and strength, natural fibers are more attractive than synthetic
fibers. The use of natural fibers offers some supremacy such as easy accessibility,
combustibility, biodegradability, and non-toxicity. Yet overall quality variance, low
CONTACT Kappat Valiyapeediyekkal Sunooj [email protected] Department of Food Science and

Technology, Pondicherry University, Puducherry, India.
© 2021 The Author(s). Published by Informa UK Limited, trading as Taylor & Francis Group.
This is an Open Access article distributed under the terms of the Creative Commons Attribution License (http://creativecommons.org/
licenses/by/4.0/), which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly
cited.
INTERNATIONAL JOURNAL OF BIOBASED PLASTICS 41
processing temperature, and high moisture absorption of natural fibers adversely affect
their application. To achieve high-performance products from natural fiber-reinforced
biopolymer composites, myriad studies have been reported on functionalizing natural
fibers. In a biopolymer composite, mostly the biopolymer matrix governs the structure,
environmental tolerance, and durability, and the reinforcement fiber determines the
stiffness and strength of the composite. Value-added novel applications of biopolymer
composites ensure potential growth in international markets. The efforts to develop
environmental friendly composite products with improved performance have achieved
some major global applications and are still continuing. In this review, attention will be
focused on production, processing, and application of biodegradable composites pre
pared from polymers like cellulose, starch, polylactic acid (PLA), polyhydroxyalkanoate
(PHA), etc. that are currently commercialized and available in the market and the ones
that are more promising as matrices for natural fiber composites in future. The review
will not cover the non-biodegradable (bio-based and partially bio-based) or fossil-fuel-
based biopolymers.
Natural fibers
Since early civilization natural fibers have been employed to make ropes, twines, and
fabrics and played a significant role in society. Natural fibers do not damage the
environment as they are sustainable, carbon neutral, renewable, and biodegradable
resources [1]. Due to their versatility and local availability, natural fibers are potential
alternative materials to synthetic fibers in composite industry [2]. Unlike synthetic
fibers, natural fibers are biodegradable and eco-friendly in nature. They are renewable
resources which possess remarkable properties such as lightweight, low density, easy
production and processability, and cost effectiveness [3,4]. Natural fibers are currently
preferred over synthetic fibers, as the former produce lesser wear and tear to the
machine and its parts during processing, and also do not contaminate the landmass
or water bodies [3]. These natural fibers are widely used for reinforcements in to
polymer matrices, where polymers are used as the binding materials to hold fibers and
provide dimensional stability [5]. The exceptional strength per unit mass of natural
fibers makes them as an excellent and attractive choice as reinforcing materials [6].
Around 30,000,000 tonnes of natural fibers are produced annually and have been used
as suitable raw material in sectors like clothing, paper making, packaging, sports
equipments, automobiles, and building materials [7].
Classification of natural fibers

On the basis of biological origin, natural fibers are classified as animal and plant fibers.
Mostly, animal fibers are composed of proteins while plant fibers are composed of
cellulose. Plant fibers are abundantly available and cost effective; on the other hand
animal fibers have recently gained attention as reinforcing material for biopolymer
composites. Animal fibers have received appreciable interest because of their flexibility,
high surface toughness, high aspect ratio, and low hydrophilic nature when compared to
plant fibers [8]. Plant fibers like hemp, kenaf, flax, cotton, ramie and animal fibers like
wool and silk are usually used in textile sectors [3].
42 K. V. SUNOOJ ET AL.
Animal fibers
On the basis of sources, animal fibers are mainly animal hair, bird feather and silk. The
exceptional chemical, physical and mechanical properties of animal fibers make them
a potential reinforcement material in polymer composites. Wool is the animal hair from
hairy mammals like sheep, alpaca, bison, angora rabbit, cashmere/pashmina goats, etc. It
is a commonly used textile fiber, and the major producers are China, New Zealand and
Australia [9]. The physico-chemical properties of wool differ according to its origin. For
example, the diameter of angora, alpaca, qiviut, and cashmere wool fibers ranges between
12 to 16 μm, 12 to 29 μm, 15 to 20 μm, and <18.5 μm, respectively [9]. Wool fibers are
hydrophilic in nature and absorb water to one-third of their weight. The rate of flame
spread, the rate of heat release, and heat of combustion is low for wool fibers [9]. Bodily
hairs of goat, horse and camel are also commonly used animal fibers. Feathers and feather
fibers of chicken and other birds can be regarded as avian fibers. Chicken feather that is
mainly composed of keratin are the by-product waste from slaughter houses [3]. The
chicken feathers fiber comprises of 91% keratin, 8% water, and 1% lipids [9]. Chicken
feather fibers are used in microbial corrosion-resistant application and in production of
absorbent sponges and composite sponges for cleaning lenses and highly polished
surfaces because of the absorbance nature of keratin [10]. Studies have revealed that
chicken feather fiber-reinforced composites showed good mechanical, acoustic, and
thermal properties because of their chemical composition, low density, and morpholo
gical structure [9].
Silk is usually procured from approx. 14,000 species of butterfly larvae and also from
approx. 4000 species of spiders [3]. Silk is the fiber secreted by glands near the mouth of
insects during cocoon development. Chitin, a highly structured protein is present in silk
which gives the fiber good chemical resistance and mechanical strength. The most widely
utilized mulberry silk (Bombyx mori) is composed of two components, fibroin, and
sericin. The fibroin consists of 5263 heavy chain and 262 light chain amino acids. It
has a tensile strength of about 600 MPa which is relatively more than most of the plant
fibers. Silk is used in biomedical applications like tissue engineering and for the produc
tion of medical scaffolds by fiber reinforcements in polymers [9]. The silk produced by
giant wood spiders or banana spiders (Nephilia) is known as dragline silk. Dragline silk
fiber is composed of two highly repetitive proteins, spidroin I and spidroin II. The fiber is
semi-crystalline and shows a lower degree of crystallinity than mulberry silk [9].
Amongst the silk fiber from various species, dragline silk is one of the strongest silks
with a tensile strength of 1.1 GPa that can be compared to high tensile steel (1.5
GPa) [10].
Plant fibers
Over years, the plant fibers are used to produce clothing materials, automobile interiors,
partition boards, packaging materials, and other accessories, thus served as a good source
of raw material for various uses [11]. The fibers obtained from plants are mostly
composed of cellulose, hemicelluloses, lignin, pectin and wax where their proportion
varies from one plant to another and also differs with various parts of the same plant [5].
The chemical composition and physical properties of plant fibers depend on the
geography and soil condition, type of plant, age and growth of the plant, part of the plant
where fiber is obtained and the mode of extraction of fibers [12]. Plant fibers are of
remarkable demand to replace synthetic fibers to use it as environmental friendly renew
able reinforcing materials to develop biopolymer composites. Kenaf and sisal are two
most commonly used plant fibers instead of glass fibers for producing polymeric com
posites [13].
Depending on the utility, the plant fibers are classified as primary and secondary
fibers. Primary fibers are kenaf, hemp, jute, sisal, cotton, etc. which are from the plants
that are mainly grown for fibers. Coir, oil palm, pineapple, and banana leaf fibers that are
obtained from their respective plants as by-products are called secondary fibers [3]. For
the commercial uses, the plant fibers are widely classified on the basis of botanical origin
as bast, leaf, seed, fruit, stalk, grass, and wood fibers. Bast fibers are the ones obtained
from the stem of a plant (kenaf, hemp, ramie, flax, jute, banana, etc.), leaf fibers (sisal,
agave, abaca, PALF (pineapple leaf fibers), curaua, raphia, fique, etc.), seed fibers (coir,
cotton, kapok, soya, rice hulls, etc.), fruit fibers (luffa, coir, oil palm, etc.), stalk fibers
(rice, wheat, maize, barley, rye, oats, etc.), grass fibers (bamboo, baggase, esparto,
elephant grass, canary grass, switchgrass, phragmites, etc.) and wood fibers are mainly
softwood and hardwood (rosewood, teak, etc.) [4]. Besides, certain plants possess more
than one type of fiber. For instance, kenaf, hemp, flax, and jute have bast as well as core
fibers, while coconut, oil palm and agave have both stem and fruit fibers and cereal grains
have hull and bast fibers [11]. Among the plant fibers, the bast fibers show excellent
modulus of elasticity and flexural strength whereas the leaf fibers show great impact
properties [13].
Kenaf (Hibiscus cannabinus L.) from the family of Malvaceae is a warm season annual
herbaceous fiber plant native to Central Africa [14]. Kenaf fiber is a widely accepted bast
fiber comprising around 65.7% cellulose and 21.6% pectin and lignin [11]. The fiber
possesses excellent tensile and flexural strength, and can substitute fiber glass and other
synthetic fibers [13]. Kenaf fiber is suitable for textiles, carpet padding, automobile
dashboards and corrugated medium and other extruded or injection molded polymer
applications [11]. Flax (Linum usitatissimum) also from the family of Malvaceae is one of
the oldest grown fiber crops in temperate regions [15]. Flax fiber consists of 70%
cellulose, 20% of hemicelluloses, and 10% lignin and pectin. The fiber shows tensile
strength and modulus between glass and aramid fibers [11]. Flax fiber is employed as an
alternative to glass fibers for varied applications like reinforcements in concrete and
polymers, asbestos replacement, packaging materials, lining materials, panel boards and
to manufacture other lighter parts in automotive industries [11,14]. Hemp fiber from an
annual herbaceous flowering plant, Cannabis sativa, from the family of Cannabaceae is
a widely used bast fiber [16] native to Asia and largely cultivated in Europe [13]. Raw
hemp is usually thin, coarser, shiny, and light colored [14] and exhibit excellent strength
and water resistance [16]. The tenacity of hemp fiber is 20% higher than flax fiber. Hemp
fibers are used in varied applications like textiles, paper, medical supplies, construction
materials, automobiles, etc [14].
Jute fiber from annual plant Corchorus capsularis, Tiliaceae family is a versatile strong
lignocellulosic bast fiber grown in monsoon climate in India, Bangladesh, and China
[15]. For retting process, the plant is cut and soaked in water throughout all seasons. The
jute fiber has low gravimetric thickness, low scraped spot, low thermal conductivity,
moderate water retention and good mechanical properties. It also possesses excellent
isolate and antistatic properties [11]. Jute fibers are used in shopping bags, ropes, and as
polymer reinforcement materials. Ramie (Boehmeria nivea) from Urticaceae family is
a flowering plant producing one of the easily accessible bast fibers [16]. Ramie fibers are
obtained underneath a thin bark layer of the stem. It consists of 73–74% cellulose, 13–
15% hemicelluloses, 1.0–5.5% pectin, and 0.6–1.5% lignin. Ramie fibers are finer and
strong in dry state and become stronger once wet [11]. It has cellulose content and longer
durability when compared to other natural fibers [16]. Besides, the characteristics of
ramie fibers match other bast fibers like jute and flax. Out of all bast fibers, ramie, flax and
hemp are more resistant to insects and pests and do not require special soil conditions for
growth [11].
Sisal (Agave sisalana) from the family of Asparagaceae is native to Mexico, yields a stiff
fiber on decortication which is traditionally used for twine and rope making [13,16]. It is
commercially grown in India, Indonesia, Brazil, Haiti, and East Africa. Sisal fiber is
a strong, coarse and hard fiber. Its annual production is half of the total textile fiber
production. The cultivation of sisal plants is comparatively easy as it can withstand hot
climates and have potential to grow in arid regions. It is resistant to any insect or pest
diseases and can grow in any soil type except clay [17]. Sisal fiber is composed of 65%
cellulose, 12% hemicellulose, 10% lignin, 0.8% pectin, and 0.3% wax [16]. It has specific
strength and modulus comparable to glass fibers. Sisal fibers are used in polymer
composites in automotive applications such as internal engine covers, seat backs, sun
visors, package trays, hat racks, door panels, and exterior or under-floor paneling. It is
also used in interior paneling in aircraft industries [17]. The abaca fiber obtained from
banana plant (Musa textilis) of Musaceae family, is durable and resistant to seawater. It is
one of the strongest commercially available cellulose fibers in Ecuador and Philippines
[15]. Abaca is used in making cordages and it is a good replacement to glass fibers in
automobiles [3]. Pineapple leaf fiber (PALF) which is rich in cellulose is isolated from
Ananas comosus, a tropical plant from Bromeliaceae family native to Brazil. PALF is an
abundantly available waste product obtained after the pineapple cultivation, which is
currently used for varied polymer reinforcement applications [15]. Curaua fibers are leaf
fibers obtained from an Amazon forest plant, Ananas erectifolius that is similar to
pineapple plant. Compared to other natural fibers, curaua fibers exhibit low density,
good tensile strength and elongation at break suitable for practical applications [18].
Coconut fiber or coir is a lignocellulosic fiber located between the outer shell and the
husk of coconut (Cocus nucifera), a tropical palm from the family of Arecaceae [13]. It is
an abundantly available by-product after coconut processing and mostly used in textiles,
ropes, bags, baskets, mats, etc. The durability and hard-wearing quality of coir make it an
acceptable reinforcement material in polymers [16]. Coir fiber-reinforced composites are
employed in the manufacture of cushions for car and bike seats [3]. Oil palm fiber is also
a leading lignocellulosic fiber obtained from trunk, frond, fruit mesocarp, and empty fruit
bunch of oil palm (Elaeis guineensis) from Arecaceae family. Oil palm fiber has gained
growing acceptance as reinforcement for polymer matrices due to its characteristic
properties [16]. Bamboo (Bambusoideae) is an evergreen perennial flowering plant
from the grass family Poaceae, which grows up to 40 m height in monsoon climate
[15]. Bamboo fibers are obtained from the hard trunk, branches, and leaves of the plant
mostly through steam explosion and mechanical treatment [16]. Apart from all the
natural fiber properties, bamboo fibers exhibit good ultraviolet (UV) light absorbency
and are thus employed in hand-made paper, carpentry and construction applications
[11,15]. From studies, it is noticed that bundles of bamboo fibers showed sufficient
specific strength comparable to conventional glass fibers [15]. Bagasse is the fibrous
residue from sugarcane juice milling process. After harvesting, the sugarcane plant
(Saccharum officinarum) is crushed between the serrated rollers in the mill. The cellulose
and hemicellulose comprise around 70 % of the sugarcane bagasse [19]. Bagasse fibers are
gaining acceptance from many researchers as they can be used as a reinforcement
material in composite preparation [13]. Wood flour or wood fiber is one of the mostly
used natural fillers for numerous applications [2]. Wood fibers, commonly obtained from
the wood waste from different processing (like pulp and paper, carpentry, building and
construction, etc.) are employed in reinforcement purposes after a simple sieving process
[4]. Recently, many novel plant fibers, namely, Parthenium hysterophorus [20], Impomea
pescaprae [21], Catharanthus roseus [22], Coccinia grandis stem [23], Carica papaya bark
[24], Cardiospermum halicababum [25], Saccharum bengalense grass [26], Tridax pro
cumbens [27], Cereus hildmannianus [28], Ficus racemosa [29], and Dracaena reflexa [30]
were observed as a potential reinforcement for polymer matrices than the existing natural
fibers.
Extraction and processing techniques of natural fibers

Fiber extraction process is a critical step governing the qualitative and quantitative nature
of fiber. Type of fiber and required application decide the method of fiber extraction [3].
The animal fibers are extracted by different methods according to their origin. For
instance, the wool is extracted by manual labor and further washed to remove the
impurities [9]. On the other hand, the silk from cocoon is obtained by slightly boiling
the cocoon in mild soap solution. The spider silks are obtained by sedating the spider and
flipping them upside down to expose the spinnerets. Later the fibers are removed and
separated with the help of a brush and microscope [3]. Water vapor exposure, sun
exposure, and dry heat exposure are the other silk cocoon stifling processes reported
by the researchers [31].
Like animal fibers, there are varied ways of retting to extract fibers from plant
sources. Retting is the process of separating and extracting the fibers from non-
fibrous tissues of plants by detachment, disintegration, and deterioration of pectin,
gums and other adhesive substances [11]. The method of retting determines the yield,
quality, structure, chemical composition, and properties of the fibers. Two major points
to consider while performing retting process are to completely separate fibers from
pectin materials and to cease the retting process at the correct time to prevent over-
retting [11]. Thus, continuous screening retting procedure is crucial to guarantee the
quality of fibers. Various types of retting are biological retting, mechanical or green
retting, physical retting, chemical retting, protein retting, and enzyme retting. Earlier,
the most commonly utilized retting methods were water retting and dew retting
process. In these methods, the part of the plant takes around 14–28 days to degrade
into individual fiber strands [3]. Since, it is a time-consuming process, alternate
techniques like mechanical, chemical, and enzymatic methods have been currently
encouraged.
Biological retting
Biological retting is of two types; natural and artificial retting [11]. Dew or field
retting and water retting are two types of natural retting. Dew retting is usually
performed in optimum humidity and temperature ranges. After the plant is mown,
the harvest is laid over the fields for the microbes to isolate the fibers from xylem
and cortex. Later, the stalks are dried and baled [32]. In water retting, the water
penetrates to the central part of the stem and ruptures the outer layer of the
harvested plants. Microorganisms present inside the stem of the plant are used to
break down large cellular tissue, pectin and various gums around the fibers which
are submerged in lakes, ponds, small streams, or artificial water tanks or vats [3]
(Figure 1). This method relies on the bacterial inoculums, type and temperature of
water, and usually takes about 7–14 days to complete the process [11]. Dew retting
is widely used to produce bast fibers. However, it is not a highly preferred method,
as it is time-consuming, contaminates water bodies and produces low-quality fibers
[3]. Another type of water retting is simulated retting, which is waterway or warm
water retting that produces high quality homogenous and clean fiber within
3–5 days [11].
Mechanical or green retting

Mechanical retting is also mostly performed in bast fibers. Unlike water retting,
mechanical retting produces better quality fibers within short duration. The
mechanical decorticators are made of beaters and rollers through which the plant
stems are fed. On repeated feeding of plant stem between the rollers, the gums and
skin are removed [3]. The machine finally ribbons the bark, packs the strips and ties
up the individual ribbon into a set (Figure 2). The process of ribboning separates
the bark from core material and the single portion of bark is called ribbon.
Decortication is also a similar procedure to ribboning [11]. Finally, all the retted
fibers are collected, washed, and sun dried.
Figure 1. Water retting process.
Figure 2. Mechanical retting process.

Physical retting
Steam blast strategy and ultrasound are two mainly used physical retting techniques. In
steam blast strategy, pressure and expanded temperature are applied along with other
added substances to enter into the interspaces of bast fiber packs. The abrupt relaxation of
steam causes powerful separation and degradation of fiber composites to fine fibers [11].
In ultrasound retting, the plant stems are cut and washed after reaping. Partially squashed
stems are then immersed into water containing alkalis and surfactants as pre-treatment to
extreme ultrasound. This continuous process separates the fibers and hurds [11].
Chemical and surfactant retting

In chemical and surfactant retting, the plant parts or straws are immersed into warm
water tanks which contain sodium hydroxide (NaOH) or potassium hydroxide (KOH),
chlorinated lime, soda ash and corrosive sulfuric acid (H2SO4) to break and separate the
pectin at high temperature. Oxygen is also supplied in controlled condition for dying and
shining of fibers. The fibers obtained from these physical-chemical retting techniques are
usually uneven in vibe, coarser and solid. So it is mandatory to modify the fiber strands by
manual rubbing to reduce their stiffness [11].
Protein and enzyme retting

Protein retting employs pectin-corrupting pectins to extract fibers from woody tissue
[33]. It uses enzymes to control the process by specific biodegradation of pectinaceous
substances. By extending the temperature to an ideal temperature, the enzyme action
augments and denatures the fibers [11]. In enzyme retting, the fibers are first subjected to
pre-treatment with aqueous solution of Triton X-100 (0.85%) and further treated with
aqueous solution of pectinase (1.0 %) at 50 °C for 24 hours. The diameters of the fibers
are reduced in this retting procedure [3]. Several factors like equipment accessibility,
assembly location, availability of industrial markets, and economic variables determine
the processing methods and equipments. All the fiber separation techniques have dis
tinctive economic ramifications which aid in harvesting, processing, integrated produc
tion and utilization systems [34]. If the innate properties of fiber are not disturbed by the
extraction process, that particular process may be considered as its standard fiber
extraction process.
Chemical composition of natural fibers

The chemical composition of natural fibers varies with the size of the fibers [2].
Biochemical composition of plant fibers differ from one plant to another with type,
age, and maturity within different tissues of the same plant, and also with soil type,
climatic condition, fiber extraction and degradation process [4]. Animal fibers are
generally composed of proteins such as keratin, fibroin and collagen and chitosan,
which govern the strength of the fibers. The protein structure varies with species [3].
Whereas the plant fibers are mainly composed of cellulose, hemicellulose, pectin, lignin
and wax that are joined by hydrogen bonds to provide inflexibility and strength [5].
The cellulose forms the main skeleton component of plant fibers. Cellulose is a linear
polysaccharide of β-1,4-linked glucose units that impart good strength, stiffness, and
structural stability to the fiber [11]. The tighter cell wall in natural fibers is obtained when
the celluloses are clubbed together by pectin and this accounts for strength and resistance
to lysis in the presence of water [1]. It is a thermally stable polysaccharide having
decomposition temperature range between 315 and 400°C. While the hemicelluloses
are accountable for the moisture absorption, thermal and biological degradation of plant
fibers, as they exhibit least resistance when compared to celluloses [1]. Lignin is an
amorphous, cross-linked polymer network composed of irregular array of bonded
hydroxy- and methoxy-substituted phenylpropane units [11]. In plant fibers, even
though lignin is responsible for UV degradation, it is thermally stable as the decomposi
tion temperature is between 165 and 900°C [1]. Pectin is a structural acidic heteropoly
saccharides that is composed of modified glucuronic acid and rhamnose residues. The
structural integrity of plant is improved by the pectin chains that are often cross-linked
with calcium ions [11]. The cellulosic framework structure in plant fiber composites on
a whole is held together by collective function of hemicelluloses, lignin and pectin as
a matrix. On an average, plant fibers are mostly composed of 60–80% cellulose, 5–20%
lignin, and around 20% moisture [11]. The percentage of chemical composition of each
constituent varies with type and parts of plants from where fiber is extracted [1]. The
chemical constituents play a key role in predicting both thermal and mechanical perfor
mance of fiber and composite [3].
The chemical constituents of fibers are analyzed by several methods. With chemical
analysis, the weight percentages of these constituents are determined [3]. To analyze
different chemical components, the Technical Association of the Pulp and Paper Industry
(TAPPI) standards like T203 cm-99 (α-cellulose) and T222 cm-06 (lignin) are used [3].
To determine total cellulose content, the calorific method apparatus is usually employed
[35]. There are numerous American Society for Testing and Materials (ASTM)
International standards to analyze the chemical composition of a material. Lignin and
cellulose content are determined according to ASTM D1106–96 and ASTM D110360
standard, respectively [36]. The holocellulose is determined according to ASTM D1104–
56 by delignification and mercerization methods [3]. The moisture content of fibers can
be determined by an electronic moisture analyzer. The ash content of fibers is analyzed
by ASTM E1755–01 and is expressed in mass residue percentage obtained after dry
oxidation [3]. The percentage of wax and other fatty substances are determined by
Conrad method with Soxhlet extraction [37].
Physical properties and characterization techniques of natural fibers

Unlike chemical composition, the physical properties of natural fibers shows great
differences among each other [38]. Animal as well as plant fibers do soften, shrink or
expand on heating or become brittle and ductile on cooling and are prone to microbial
degradation [39]. Physical properties of natural fibers are dependent on various factors
like species, age and maturity of plant, geographical location, ecotype (sun, rain and soil
conditions) and fiber extraction methods [5,38]. The natural fiber properties, especially
mechanical properties depend on the amount of cellulose, microfibril angles, and the
degree of polymerization of cellulose in the fibers [40].
Knowing the characteristics of fiber is essential to expand its utilization and applica
tion in composites preparation with improved performance. The structure and morphol
ogy of natural fibers are greatly controlled by the amount of lignin present in the fiber [4].
Major structural differences in cell wall length, thickness, diameter and density develop
huge differences in physical properties [15]. The surface roughness, cell wall structure,
diameter, and other morphological characteristics of fibers are determined by scanning
electron microscope (SEM) and atomic force microscope (AFM). SEM analysis gives
a detailed high-resolution image of the fiber by scanning through an electron beam, as it
is focused over the desired surface by detecting the secondary and backscattered electro
nic signal [3]. AFM is a very high-resolution type microscope of scanning probe micro
scope (SPM). It shows resolution on the order of fractions of nanometer (nm), which is
1000 times better than optical diffraction limit. Surface roughness parameters like
average surface roughness (Ra), maximum peak to valley height (Rt), and root mean
square roughness (Rrms), etc., are determined by AFM [3]. The surface roughness of
fibers is also determined by vertical scanning methods like confocal microscopy, confocal
chromatic aberration and coherence scanning interferometry (CSI), and by horizontal
scanning methods like structured light scanning and scanning laser microscope. The
non-scanning methods like digital holography microscopy are also used to determine the
surface roughness [3]. The diameter and surface roughness of the fibers play a significant
role in deciding the wettability nature of fiber with matrix and mechanical strength of the
composites. The wettability of natural fibers by water is determined by contact angle
measurement, and it depends on the nature and amount of waxy substance in the fibers
[4]. The density of the fiber is studied with the help of pycnometer experimentation using
toluene and real density analyzer (helium pycnometer). It is also determined by ASTM
D3800 M based on the Archimedes method using hexane [41].
Fourier-transform infrared (FTIR) spectroscopy is an experimental technique to
qualitatively and quantitatively analyze the organic compounds, and thereby provide
necessary information on molecular structure and chemical bonding in natural fibers [1].
Out of the two FTIR spectroscopy methods; absorbance and transmittance methods, the
FTIR transmittance method is widely employed for natural fibers [3]. The spectrograms
are determined as the specific peaks which appears in wave number versus transmittance
graph that depends on the stretching, bending and vibration of the functional groups in
the fiber [30]. X-ray diffraction (XRD) is a nondestructive analytical method used to
examine the crystallographic structure, crystal size and crystallinity index of natural
fibers. The scattered intensity of an X-ray beam hitting a fiber sample is observed as
the function of wavelength or energy, polarization, incident and scattered angle [1]. The
two distinct peaks of diffractogram are detected in plant fibers. The first peak is observed
around at 2θ = 18°, indicating the presence of amorphous constituents like, hemicellu
lose, pectin lignin, wax, etc. The second peak is observed around 2θ = 22° corresponding
to cellulose I [3]. The crystal size and crystallinity index play a major role in enhancing
the mechanical properties of fiber-reinforced composites, and by surface modification or
chemical treatment, the same can be modified. As the crystal size increases the hydro
phobicity of fiber and composite are also improved [3].
Natural fibers possess good acoustic insulation and thermal properties as these fibers are
hollow and lignocellulosic in nature [2]. The chemical composition and thermal perfor
mance are determined by differential scanning calorimetry (DSC) and thermogravimetric
analysis (TGA). TGA is also used to find out the thermal stability and weight loss percent
of natural fiber on degradation. Amongst natural fibers, the plant fibers show good thermal
insulation and are used to develop products, which can be used for thermal applications
[3]. Fiber strength is a major criterion for selecting natural fibers for specific applications
[15]. Even though the mechanical properties of natural fibers are comparatively lower than
synthetic fibers, they can be made equal or even greater in mechanical performance by
appropriate surface modification techniques. Unlike synthetic fibers, the low density, high-
specific modulus and elongation at break attract many industries to employ natural fibers
for various polymer engineering composite applications [2,5]. Usually in plant fibers, the
cellulose content affects the mechanical properties [4]. The hydrogen bonds and other
linkages in the cellulose determines the strength and stiffness of fibers [40]. As the cellulose
content increases the tensile strength and Young’s modulus were found to increase [4].
Thus the overall performance of a fiber for specific application depends on major factors
like structure, cell dimension, density, microfibrillar angle, chemical composition, mechan
ical properties, and fiber–matrix interaction under specific environmental conditions [42].
Drawbacks of natural fibers

The natural fibers have some innate drawbacks such as irregularity in the size, shape, and
diameter of the fiber and their effect on the density, hardness, and strength of the
composite [3]. Most of the existing fiber extraction methods are a time-consuming process,
especially for fibers like silk. Thus, better extraction techniques need to be identified to
produce fibers in an environmentally friendly way. Other major problems of natural fibers
are the poor resistance to microbes and pests, high moisture sensitivity, and moderate
thermal stability [4]. The low microbial resistance and high moisture sensitivity increase
the chance of getting rotten by spoilage, and subsequently releasing unpleasant smell [43].
Plant fibers are susceptible to decomposition in humid and dark environment, while
animal fibers like silk and wool are susceptible to pest and insect infestations. One way
to get rid of this problem is to develop natural fibers with anti-microbial and anti-pest
coupling agents to prevent microbial degradation and pest infestation, respectively [3]. The
high hydrophilicity characteristic of natural fibers, obstructs in widening their reinforce
ment in composites in automotive applications. The function of natural fibers as com
pliance products is affected by the hydroxyl (OH) and other polar groups and various
physical impurities found in the fibers [2]. Another key resistance of natural fiber compo
site application is the innate hydrophilicity of fibers and hydrophobicity of polymer
matrices, resulting in poor coupling at the interface and weak interfacial bonding of the
composite that leads to poor performance [2,40]. The unpredictable durability that affects
both processing and application of natural fibers is one major obstacle to use them in
composites [38]. To overcome these shortcomings, the natural fibers are subjected to
biological, physical and chemical treatments to remove impurities, improve water resis
tance, mechanical properties, and interfacial bonding with the composites.
Modification methods of natural fibers

Since natural fibers contain several OH groups within cellulose and lignin compounds
they are very much flexible to modifications [11]. The chemical modifications activate
these groups or introduce new functional groups which make the fibers interact effec
tively with the matrix and improve the compatibility between fibers and biopolymers [4].
By reacting with the OH groups, chemical treatment reduces the hydrophilicity,
improves the moisture resistance property and ameliorate the mechanical properties of
fibers [43]. Overall the natural fiber modification brings about alteration in the physical,
chemical, thermal and mechanical properties of natural fibers and it depends on various
factors like method, duration, temperature and chemical concentration. The surface
modification of natural fibers can be classified into physical and chemical methods.
Physical methods
The physical treatments are mainly done to separate fiber bundles into individual
fibers and to modify fibers for composite applications. The physical process in which
bundles of natural fibers are separated to discrete filaments is one of the oldest fiber
modification methods. The natural fibers are physically modified by stretching,
calendaring, thermo treatment, or by electrical conduction [11]. By these treatments,
the structural and surface properties of natural fibers are altered to augment their
mechanical bonding to polymers. Other physical methods employed in treatment of
fibers are plasma treatment, corona treatment, steam explosion treatment, dielectric
barrier technique, laser, and γ-ray treatment [44]. Treatments like plasma and
corona aid in surface cleaning of fibers by removing the unwanted materials and
functionalizing them [4].
In plasma treatment, the surface of the fiber is exposed to very high voltage,
which is supplied for ionizing the gas and to use it as plasma in vacuum conditions
[4]. The treatment improved the surface strength of the fiber by crosslinking the
fiber surface by introducing free radicals [11]. Oxygen plasma refers to plasma
treatment by introducing oxygen to the plasma chamber. Oxygen plasma treatment
removes the organic contaminants by chemical reaction with highly reactive oxygen
radicals [4]. With this method, the surface of the fiber is cleaned by surface etching
and improved the surface roughness for enhancing the adhesion and interfacial
bonding by creating interlocks with the matrix [45]. Oxygen plasma treatment
also promotes surface hydroxylation, oxidation, and increases the wetting property
of the natural fiber surfaces [46]. Corona treatment carried out in a corona dis
charge reactor modifies the fiber surface oxidation to improve the interface between
hydrophilic fiber and hydrophobic matrix [47]. The treatment improves the
mechanical strength by changing the surface energy [42], and acidity of the fiber
surface [48]. Steam explosion process is a high-pressure steaming, which requires
heating of lignocellulosic fibers at high pressures and temperatures, followed by
mechanical disruption of pre-treated fibers to a collecting tank by violent discharge
(explosion). Steam explosion process resulted in reduced stiffness, smoother surface,
better fineness distribution, and improved bending properties of the fibers. This
process is used in lignocellulosic fibers to improve the dispersibility and adhesion
with polymeric matrices [44]. The vacuum ultraviolet (VUV) irradiation is a widely
accepted method for removing impurities from fiber surface. The fibers were placed
in a stainless steel chamber and high energy radiations <200 nm and pressure of
2.5 Torr is applied at room temperature [49]. The treatment enhances the
wettability, insulation, tribological properties, and biocompatibility of fibers with the

matrix [3]. γ-rays treatment enhances the inter-crosslinking of cellulose molecules
and improves the mechanical strength of the fibers [50]. Laser treatment is a way to
remove the lignin content in plant fibers and to ameliorate the structural and tensile
strength of the fibers [49]. Ozone or oxygen-fluorine gas is a successful method to
enhance the surface of the natural fibers. The mechanical properties of natural fibers
can be maintained for a long period by ozone treatment [51].
Chemical methods
Chemical treatments that are frequently used are bleaching, mercerization, and acet
ylation. Other chemical treatments are benzoylation, silanization, acrylation, grafting
and use of peroxide, permanganate, triazine, isocyanate, maleated coupling agents, and
fatty acid derivates [11]. Bleaching is the process of soaking natural fibers in bleaching
solution like sodium hydroxide (NaOH) and hydrogen peroxide (H2O2). By alkaliza
tion the fine structure of native cellulose I changes to cellulose II [52]. Alkali treatment
removes the OH bond by dissolving the amorphous constituents, improves the surface
roughness and interfacial bonding between the fibers and matrix [49]. It also enhanced
the thermal stability and tensile strength of the fibers [53,54]. Research has shown
varied types of alkali treatments. For instance, the alkaline treatment with 6% NaOH
increased the crystallinity index by removing the amorphous compounds from the fiber
[55]. In another study, Borassus fruit fine fibers were treated with 5% NaOH solution
for varied time interval (1, 4, 8, and 12 h). It was noted that after 8 h of alkali treatment,
the tensile properties such as strength, modulus, and percentage of elongation of fibers
increased by 41%, 69%, and 40%, respectively [56]. It was also observed that alkali-
treated natural fiber composites exhibited increased tensile strength when compared to
untreated fiber composites [11]. Mercerization is also an alkali treatment of fibers that
depends on the type and concentration of the solution, temperature, duration, and
tension on the fiber and additives [42]. Mercerization improves the surface roughness
of fiber by dissolving lignin and waxes and thereby increases the cellulose crystal
exposure [4].
Acetylation or esterification is another surface modification process for plasticizing of
natural fibers in which an acetyl group is introduced into the organic compound in
natural fibers. This method modifies the OH groups and makes the fiber more hydro
phobic in nature [42] and enhances the dimensional stability of the composites. The
treatment imparts rough surface topography with a lower number of voids, and that
provides strong mechanical interlocking with the matrix [35]. Acetylation with acetic
acid to improve initial thermal degradation and tensile strength involves submerging the
fibers in 10% acetic acid along with concentrated sulfuric acid solution. Further,
a solution of acetic anhydride with necessary concentration is also added [57].
Benzoylation treatment uses benzoyl chloride to reduce the hydrophilic nature of fiber,
enhance interfacial adhesion, and thus improving the composite strength. For benzoyla
tion process, alkali pre-treatment is done to remove the extractable materials such as
lignin, waxes, and oil covering materials, and OH groups are thus exposed to the surface
of the fibers. Later, the fibers are treated with benzoyl chloride, where the OH groups are
replaced by benzoyl groups and get attached on the cellulose backbone [35]. The
peroxide-induced grafting of biopolymer adheres over the fiber surface. The peroxide
initiated free radicals react with the OH group of fiber and matrix. Thus, peroxide
treatment improves the interface properties of fiber and matrix. It also slows down the
moisture absorption and enhances thermal stability [35]. Benzoyl peroxide treatment
enhances the interfacial bonding of fiber and matrix by removing the OH bond. It
involves pre-treatment of fibers with NaOH solution followed by treating the fibers
with required amount of benzoyl peroxide with acetone [58].
Acrylation uses acrylic acid to improve the interfacial bonding between the fiber and
matrix. Acrylic acid reacts with the cellulosic OH groups of the fiber and provides more
access of reactive cellulose macro-radicals to the polymerization medium. The carboxylic
acids from coupling agents form ester linkages with cellulosic OH groups, and reduces
hydrophilic OH groups from the fiber and promote moisture resistance properties [35].
For fiber surface modification, isocyanate works as a coupling agent. The functional
group of isocyanate reacts with OH groups of cellulose and lignin in fiber, and forms
a urethane linkage. The linkage imparts strong covalent bonds between fiber and matrix
[35]. Stearic acid in ethyl alcohol solution is used for the modification of fiber surface.
The carboxyl group of stearic acid reacts with the hydrophilic OH groups of the fiber and
enhances moisture resistance. The treatment removes non-crystalline constituents from
fiber, which leads to the breakdown of fiber bundles and fibrillation occurs. Fiber
dispersion into the matrix facilitates better bonding at the interfacial region and improves
composite properties [35]. Permanganate treatment on natural fibers is done by using
potassium permanganate (KMnO4) in acetone solution. The treatment produces highly
reactive permanganate ions that react with the cellulose OH groups and forms cellulose-
manganate for initiating graft copolymerization. This improves the chemical interlocking
at the interfacial region and increase the adhesion with matrix [35]. The treatment of
fibers with potassium permanganate also removed impurities and waxes from fiber
surface and improved its physico-chemical properties [59].
Silane is a multi-functional molecule which is used as a coupling agent to modify fiber
surfaces. The composition of silane forms a chemical link between the fiber surface and
the matrix through a siloxane bridge [35]. Silane treatment improves the physico-
chemical properties and tribological performance of the natural fibers [60]. Grafting by
applying compatibilizers (maleic anhydride modified polymers) into natural fiber com
posites is a popular method. Maleated coupling agents helps in efficient interaction of
functional surface of fiber and matrix. During grafting, maleic anhydride reacts with the
OH groups in the amorphous region of cellulose structure and removes OH groups from
the fiber cells. It creates a brush-like long chain polymer coating on the surface of the
fiber and reduces hydrophilic characteristics. Thus, maleated coupler forms carbon-
carbon bond with the polymer chain of matrix. The covalent bond created between
OH groups of the fiber and anhydride groups of the maleic anhydride helps in bridging
interface for efficient interlocking [35]. Numerous studies have reported the improve
ment of mechanical properties of natural fibers by maleic anhydride grafting method. In
a study with PALF, it was found that graft copolymerization technique enhanced the
chemical constituents and thermal stability of the fiber [61]. Another possible way to
modify fiber surface is by coating them. Coating imparts more homogeneous fibers by
smoothing the surface by filling the imperfections [56]. It is also found that the compat
ibility of fiber and the matrix is enhanced by polymer coating over natural fibers [53].
Biopolymer
Biopolymers are the polymers that are derived from plants, animals, and microbes. They
are abundantly available renewable materials usually employed to produce eco-friendly
bioplastics [1]. Biopolymers are produced commercially on a large scale for varied
applications. Despite the fact that biopolymers make up only a small percentage of the
polymer market, it has been predicted that in future they might replace petroleum based
polymers about 30–90 %. Mostly biopolymers are biodegradable except few, that is, they
have the ability to microbiologically decompose into carbon dioxide (CO2), water (H2O),
methane (CH4), and inorganic compounds [38]. The degradation capacity of biopoly
mers is dependent on many factors like type of polymer, chemical composition and
environment conditions [3]. Recently produced biodegradable polymers possess a wider
range of properties which are very much comparable with traditional polymers used in
the market. The biopolymers are employed in specific fields depending upon their cost,
availability, moisture absorption, thermal stability, mechanical behavior, degradation
stability, and biocompatibility [38]. The chemical constituents, molecular weight, mor
phological characteristics, mechanical attributes, and processing technique of
a biocomposite are governed by the biopolymer part of the composite [62]. In spite of
wider applicability, few shortcomings of biopolymers are their hydrophilic nature, low
mechanical properties and low durable degradation ratio in moist environment [11].
Types of biopolymers
One easiest way of classification of biopolymers on the basis of their origin is natural and
synthetic biopolymers. Natural biopolymers are from polysaccharides, proteins and
microbes whereas synthetic biopolymers are the polymers developed by microbial fer
mentation, biotechnological and petrochemical production [63]. With regard to biopo
lymers’ response to thermal conditions, they can be divided into elastomers, thermosets,
and thermoplastics [62]. PLA and PHA are two most commonly used biopolymers with
regard to production and application [38].
Polysaccharides made up of monosaccharides are linked by glycosidic linkages.
Polysaccharide-based biopolymers are cellulose, chitin and chitosan, starch, hyaluronic
acid (HA), dextrin, alginate, carrageenan and various gums. Cellulose, the most abundant
carbohydrate is a promising biodegradable polymer seen in almost all plant materials
[64]. Cellulose is eco-friendly, has a low energy requirement during manufacturing,
possesses remarkable film-forming properties and is easy to recycle by combustion
[65]. Cellulose is a structural polysaccharide made up of microfibrils linked together to
make cellulose fibers [66]. Chitin comprises 2-(acetylamino)-2-deoxy-D-glucose residues
linked by covalent β-1,4 linkages. Chitin is a polysaccharide that is acidic or neutral in
nature which is hydrophobic and insoluble in water and many organic solvents [67].
The second most abundant natural amino polysaccharide is chitosan. It is obtained by
deacetylation of native chitin isolated from shrimp and other crustaceans [63]. Various
functionalities of chitosan like oxygen permeability, water sorptivity, cytokine induction,
and biodegradability make it suitable for preparing scaffolding materials [67]. Starch is
a storage polysaccharide that consists of linear amylose and branched amylopectin chains
of size 0.1–1 nm. The major sources of starches are roots, tubers and cereals.
Thermoplastic starches (TPS) are the type of starch that is thermally and/or mechanically
plasticized to substitute the use of synthetic polymers [68]. TPS is a promising material in
biopolymer composites due to its availability, renewability, recyclability, and thermo
plastic behavior [69].
Proteins are large biological molecules made up of one or more long chain amino acid
residues. Protein can be classified on the basis of origin such as animal proteins (e.g.
collagen, gelatin, silk, keratin, casein, and whey) and plant proteins (e.g., gluten, zein, pea
protein, and soy protein). Collagen found in cartilages, tendons, bones, skin, and con
nective tissues is the most abundant protein on earth [63]. The properties like biode
gradability, water absorption, high mechanical strength, biocompatibility, cross-linking
ability, and low antigenicity make it a suitable material for bioactive molecule delivery
and tissue engineering [67]. Gelatin is a water-soluble denatured fibrous protein prepared
by the partial or controlled hydrolysis of insoluble protein, collagen [70]. Gelatin is
a preferred biopolymer with OH, NH2, COOH, etc. functional groups which aid in the
production of biocomposites. Gelatin is a widely accepted protein biopolymer due to its
abundance, notable biodegradability, biocompatibility, film-forming property, gelling
ability, superior gas barrier properties and cost effectiveness [70]. Silk fibroin is
a natural protein isolated from the silkworm cocoon. It is primarily comprised of alanine,
glycine, and serine [67]. The core is made up of fibroid and is covered with sericin. Sericin
is used in wound dressing and other medical materials [71]. Soy protein isolate (SPI) is
a commercially graded by-product of soy bean oil which comprises over 90 % protein.
SPI is a biopolymer that can be utilized as a potential alternative to petroleum-based
polymers. Soy-based biopolymers possess superior mechanical properties because of the
polar and functional groups of amino acids that help in inter- and intra- molecular
interactions [64]. Wheat gluten is a biopolymeric material containing approx. 50%
gliadin and approx. 50% glutenin proteins obtained as a co-product from food processing
industries. Gluten contains cysteine that determines the functional and mechanical
properties because of its inter and intra-molecular disulfide bonds [72]. The heat treat
ment helps in improving the intermolecular disulfide bonds, which results in polymer
ization and thermosetting of gluten [73]. Thus, polymer processing techniques like
extrusion, compression, or injection molding are used to develop gluten-based bioplas
tics. Biodegradable composites possessing specific strength and stiffness are prepared by
reinforcing natural fibers such as hemp, flax, banana, coconut and wood fibers to gluten
matrix, and are used in packaging, medical, and automotive sectors [72].
Polylactide or PLA is a promising synthetic biopolymer which has unique character
istics such as, strong clarity and high rigidity to substitute conventional polymers [2]. It is
a biodegradable, renewable and recyclable hydrophobic aliphatic polyester showing
excellent processing ability [40]. The PLA synthesis is a multi-step process starting
from lactic acid production to its polymerization [74]. Lactic acid (LA), which is the
basic constitutional unit and main precursor in PLA synthesis, is largely produced from
lactic acid bacteria (LAB) fermentation of a carbon source [67]. The outstanding
mechanical and barrier properties of PLA make it suitable for producing various bioma
terials for several industrial applications in textiles, packaging, biomedical and automo
tive manufacturing industries. The research work on natural fiber-reinforced PLA
composites has revealed noticeable benefits like renewability, recyclability, high durabil
ity, strong processability, high-specific resilience, and compostability [2]. PHAs are the
only biopolyesters family derived from microbial fermentation of sugars or lipids. They
are prepared by exposing bacteria to carbon source and limiting all other necessary
nutrients [1]. It is an attractive biopolymer used in pharmaceutical, tissue engineering,
and conventional medical devices because of its hydrophobicity, biocompatibility, bio
degradability, and thermoplastic properties [67,74]. Polyhydroxy valerate (PHV) or
polyhydroxybutyrate (PHB) and their copolymers poly(hydroxybutyrate-co-
hydroxyvalerate) (PHBV) with different molar ratios are the representatives of PHAs
which are all biodegradable and biocompatible [14]. The mechanical properties of PHBs
are similar to the properties of petroleum-based plastics such as polyethylene (PE) and
polypropylene (PP) [67]. The PHAs do not need any arable land for the production and
can be even produced from CO2 in a marine environment [75,76].
The biodegradable polymers derived from petrochemical resources are polybutylene
succinate (PBS), poly(butylene adipate-co-terephthalate) (PBAT), polyvinyl alcohol
(PVA), polyglycolic acid (PGA), and polycaprolactone (PCL). PBS are easily processed
semi-crystalline thermoplastic polyesters with acceptable thermo-mechanical properties
comparable to PP [77], and thus widely used in bottles and films production. PBS is made
up of 1,4-butanediol and succinic acid from renewable resources [14]. The tensile
strength (30–35 MPa) of PBS is similar to that of PP and the Young’s modulus (300–800
MPa) is between low-density polyethylene (LDPE) and high-density polyethylene
(HDPE) [74]. PBAT belonging to the family of aliphatic-aromatic copolyesters is
a biodegradable copolymer of terephthalate and butylene adipate produced by melt
polycondensation process [74]. PVA is a hydrophilic semi-crystalline biopolymer exhi
biting good mechanical strength and biocompatibility. The properties of PVA make it
a promising material for biological as well as industrial applications [63]. PCL is
a hydrophobic semi-crystalline aliphatic polyester prepared by ring-opening polymer
ization of ε-caprolactone. PCL is tough and ductile (elongation at break ~600–800%) and
has low glass transition temperature (~ −60°C) and melting temperature (~60°C) [74]. It
is mainly used in packaging and biomedical applications.
Biopolymer composites
Composites are heterogeneous structural material mixtures prepared by mixing two or
more constituent materials exhibiting remarkably varied properties [38]. The term
“biopolymer composites” can be referred to as the biodegradable composites made by
reinforcing various natural fibers from animal and plant sources to natural and/or
synthetic biopolymers [1]. In biopolymer composites, natural fiber (reinforcement
agent) in discontinuous phase is added to the biopolymer matrix in continuous phase
to improve the stiffness and tensile strength of the prepared composite. The purpose of
preparing this kind of composite is to obtain a product with good mechanical behavior
and durability performance imparted by natural fiber and biopolymer, respectively.
Usually, maximum stiffness and tensile strength of biocomposites ranges between 1 to
4 GPa and 20 to 200 MPa, respectively [38]. The natural fiber reinforcements also affect
the thermal properties, electrical conductivity, morphological characteristics, crystal
linity, degradability, and production cost of biopolymer composites. The primary appli
cations of natural fiber reinforced polymer composites are in the fields of automobiles,
aerospace, and structural constructions [4]. Some noticeable benefits of biopolymer
composite applications are sustainability, cost effectiveness, lightweight characteristics,

appreciable specific strength, biodegradability, environmental friendliness of renewable
materials and health and safety of manufacturer and consumers [11].
The fibers and matrices can be made by two methods, bulk and laminate composites.
The fibers are randomly oriented in three dimensions structure, almost exhibiting
isotropic behavior in bulk composites. On the other hand, laminate composites are
orthotropic, where fibers are oriented in multiple layers and bound together in the
matrix. In this composite, each fiber layer shows a two-dimensional orientation [38].
Adhesion of natural fiber to polymer matrix can be by inter-diffusion, adsorption,
chemical bonding, reaction bonding, electrostatic attraction, and mechanical bonding.
The mechanisms of adhesion depend on many factors such as chemical composition
and molecular conformation, morphological property of natural fiber, diffusivity of
element materials and also the atomic arrangement of fiber and matrix [1]. The
biopolymer composites properties are affected by the type of fiber, percentage of fiber
content, moisture absorption of fiber, surface modification method of fiber, structure,
and design of composite, interfacial adhesion between fiber and matrix, presence of
voids and incorporation of additives like plasticizers, compatibilizer, nanofiller and
binding agent [2,35]. Various reinforcement materials and plasticizers affect the den
sity, water sensitivity, gas permeability, degradability, and shelf life of biopolymer
composites. Thus, the hydrophilicity of natural fiber and hydrophobicity of biopolymer
drives the researchers to surface modify the fibers to improve the adhesion between
them in a composite. The performance of biopolymer composites is improved by
chemical modification depending on the processing type, processing requirements,
and environmental conditions [3]. Biocompatibility and durability of biopolymer
composite are of major concern as there is no proper solution adapted till now to
completely control these two factors.
Processing techniques of biopolymer composites

Many processing techniques have been developed and employed for biopolymer com
posites according to their application. Commonly used processing methods of biopoly
mer composite preparations are compression molding, injection molding, and extrusion.
Thermoforming, compounding and long fiber thermoplastic-direct (LFT-D) methods
are also used for natural fiber-reinforced thermoplastics. In compression molding, the
flat semi-finished products or hybrid fleeces are mostly used that are either cut exactly to
the size of the required part or are larger than the form [78]. Ramie fiber incorporated
PLA/PCL matrix-based thermoplastic biodegradable composites along with silane cou
pling agent for increasing interfacial adhesion was prepared by compression molding
process using in situ polymerization method. The effect of fiber content and fiber length
on the tensile and impact strength was determined and found that the same were at the
highest when 45 wt. % fiber content with 5–6 mm length were added [79]. For injection
molding process, the raw materials are incorporated as fiber-reinforced granules to the
injection molding machine and melted to liquid state. Further, under high pressure, the
plasticized thermoplastic material is added into the form [78]. The mechanical, thermal,
and other properties of biopolymer composites prepared by different processing techni
ques are summarized in Table 1.
Table 1. Improved properties of various biopolymer composites prepared by different processing

techniques.
Processing Remarkable characteristics of
Matrix system Reinforcement technique biopolymer composites References
PLA Silkworm silk fiber Extrusion and The modulus of elasticity, [80]
injection ductility, glass transition
molding temperature, and thermal
stability increased. The
composites can be used to
produce polymeric scaffolds
for tissue engineering
applications
PLA Chicken feather fiber Extrusion and Tensile moduli and thermal [81]
injection stability increased
molding
Wheat starch Alkali treated wheat straw Extrusion The mechanical properties [82]
fiber improved
PBS Kenaf fiber Melt mixing The crystallization rate, tensile [83]
modulus, and storage
modulus improved
Maleic anhydride Bamboo fiber Hot press molding Tensile strength and elongation [84]
grafted PCL at break increased, and rate of
biodegradation decreased
SPC Mercerized sisal fiber Soaking and Young’s modulus and fracture [85]
squeezing stress increased
PLA Silane treated ramie fiber Two-roll milling Tensile, flexural, and impact [86]
and hot strength increased.
pressing Dynamic mechanical
properties and thermal
degradation resistance
improved
PBS Kenaf fiber Compression Flexural strength and modulus [87]
molding improved
PHB Kenaf and lyocell fibers Compression The mechanical properties [88]
molding except elongation at break
increased
PLA Kenaf and lyocell fibers Compression Tensile and impact strength, [88]
molding Young’s modulus, and flexural
modulus increased
PLA Alkali treated hemp Extrusion and Crystallinity and crack [89]
injection propagation improved
molding
PLA Poly(butyl acrylate) treated Melt- Hydrophobicity, tensile strength, [90]
rice compounded and thermal stability increased
straw fiber in an HAAKE
rheometer and
hot-press
molded
PBS Alkali treated coir fiber Hot press molding Tensile strength and modulus, [91]
and flexural strength and
modulus increased
PHBV Detergent washing, Compression Flexural strength, tensile [92]
dewaxing, alkalization, and molding modulus, and dynamic
acetylation on jute fibers modulus increased
PLA Hemp Film stacking The coefficient of thermal [93]
method expansion decreased
Pehuen starch Pehuen husk fiber Melt blending Mechanical properties and [94]
thermal stability improved
PLA Alkali, permanganate, Hot pressing of Tensile and flexural properties [95]
peroxide, and silane solvent improved
treated jute fibers impregnated
prepregs
(Continued)
Table 1. (Continued).
PCL/PLA blend Flax fiber Hot press molding The mechanical properties [96]
improved
PLA Jute fiber Injection molding Tensile modulus and impact [97]
strength increased
PLA/PCL Silane coupled jute fiber Hot press molding Tensile strength and modulus [98]
increased
PLA Alkali, silane and maleinized Twin-screw The mechanical properties [99]
polybutadiene rubber extrusion improved
treated chicken feather
fiber
PHBV Kenaf fiber Melt blending Impact strength and flexural [100]
moduli improved
PCL Acylated cork fiber Melt blending Thermal stability improved. The [101]
composite can be used for
composite panels in
automotive industries and
flooring and insulation panels
in construction industries
PLA Hemp fiber Blending-spun, The mechanical properties [102]
twin-screw improved
extrusion and
injection
molding
PLA Oil palm fiber Mixer and Tensile strength, flexural [103]
injection strength, and heat deflection
molding temperature increased
PLA Curaua leaf fiber Twin-screw Impact strength, Young’s [104]
extrusion modulus and thermal stability
increased
Wax/ethylene Flax fiber Hot press molding Stiffness and impact resistance [105]
acrylate increased
copolymer/
butyl acrylate
modified PLA
PLA Silane treated bamboo fibers Injection molding Impact strength and elongation [106]
at break increased
PLA/PCL blend Silanized oil palm fiber Melt blending The mechanical properties and [107]
thermal stability improved
PLA Chicken feather fiber Extrusion and Compressive strength, Young’s [108]
injection modulus, flexural
molding modulus, and hardness
improved
Wheat starch Alkali and silane treated Mixer blending Stiffness increased [109]
hemp fiber
PLA Alkali, corona discharge, maleic Twin-screw Impact strength and elongation [110]
anhydride grafted and extrusion at break increased.
aminopropyltriethoxysilane
treated flax fiber
PHBV Silk fiber Matrix assisted Resistance improved and [111]
pulsed laser degradation rate decreased.
evaporation The composites can be used
technique for drug release schemes and
other biomedical applications
PBS Eugenol grafted coconut fiber Hot press molding The mechanical properties [112]
improved
PLA alkali and silane treated sisal Melt blending Tensile strength increased [113]
fiber
PLA Titanium oxide grafted flax Hot press molding Tensile strength, impact [114]
fiber strength, thermal stability and
hydrophobicity improved
(Continued)
Table 1. (Continued).
Chitosan Emu feather fiber mixture was The composite can be used as an [115]
dropped into absorbent for treating
an alkaline industrial waste water
coagulant containing lead
solution
Sugar palm starch Seaweed blended sugar palm Melt blending The thermal stability, tensile and [116]
fiber flexural properties improved.
Composites exhibited good
water and biodegradation
resistance
PLA Untreated sisal fiber and Compression The impact properties improved [117]
alkali treated sisal fiber molding
blend
Corn starch Curaua leaf fiber Injection molding The hardness, tensile modulus, [118]
tensile and impact strength
increased
PVA Acylated and chitosan Film casting Thermal stability increased. The [119]
grafted silk fiber technique composite films exhibit good
anti-bacterial and anti-fungal
properties which is suitable for
wound healing applications
PVA Acylated and chitosan Film casting Surface roughness increased. The [120]
grafted silk fiber technique haemocompatibility of
composite films can be used
for tissue engineering
applications
Tapioca starch Water hyacinth fiber Casting method Tensile strength, thermal [121]
stability, and hydrophobicity
improved
Tapioca starch PALF Compression The mechanical properties [122]
molding and improved
machine
processing
Potato starch Sugar beet pulp fiber Piston and The mechanical properties and [123]
wooden thermal conductivity
molding improved. The composites can
be used as building materials
because of its good acoustical
and thermal performance
PLA Maleated PLA treated agave Rotational Thermal stability, tensile strength [124]
fiber molding and modulus increased and
hydrophilicity, diffusion
coefficient and damping
behavior decreased
Corn starch Hemp fiber Dry incorporation The mechanical properties [125]
method improved. The composite
boards can be used in building
industries
Wheat gluten Wool fiber Compression Tensile strength and flame [72]
molding retardancy improved
PLA Silane treated flax fiber Manual hot plate The mechanical properties [126]
compression improved
molding
Characterization of biopolymer composites

The most commonly employed characterization techniques for determining the interface
of biopolymer composites are FTIR spectroscopy, laser Raman spectroscopy (LRS), solid-
state nuclear magnetic resonance (ssNMR) spectroscopy, ion scattering spectroscopy
(ISS), Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS),

wide-angle X-ray scattering (WAXS), and also contact angle measurement [1]. For
examining the particle distribution, reinforcements in the matrix, surface interaction
between the fiber and biopolymer and voids, microscopic visualization techniques like
polarized optical microscope (POM), scanning tunneling microscope (STM), AFM,
SEM, and field emission scanning electron microscope (FESEM) are employed. The
images are captured at required magnifications for easy visualization analysis. AFM
uses high resolution nondestructive analysis for determining the surface roughness of
fibers or biopolymer composites [3]. These morphological techniques also give informa
tion of surface morphology, surface depth profile, physico-chemical changes and fiber–
matrix interaction [1]. Saxena et al. [127] in their study reinforced acacia fibers, bleached
softwood kraft fibers and nanocrystalline cellulose to xylan/sorbitol films, and examined
the impact of reinforcement on water transmission. From the experiment, it was revealed
that the control film has a more open structure than nanocrystalline cellulose composite
films. The FTIR analysis exhibited a strong interaction at the OH band indicating good
interfacial bonding between nanocellulose and matrix surface, and the intensity of band
depends on the nanocellulose concentration. The effect of natural fiber on crystallinity of
biopolymer composites was studied with the help of XRD. The results of XRD are mostly
correlated to the FTIR analysis, thermal, mechanical and barrier properties of the
composites. It is widely noted that, by the incorporation of natural fibers to the biopo
lymer composite the interfacial bonding and crystallinity of the composite is improved
which thereby lead to an enhancement of the mechanical properties [1].
Mechanical properties of biopolymer composites

Natural fiber-reinforced biopolymer composites exhibit appreciable mechanical proper
ties needed for different applications. There are many aspects which affect the mechanical
properties of biopolymer composites, like chemical composition and physical properties
of natural fiber and biopolymer, surface modification of fiber, composite processing
techniques (temperature and force applied), processing environment, fiber loading con
centration, orientation of fiber in the matrix, copolymerization and plasticization [2,3].
The mechanical properties are also influenced by the presence of waxy substances in fiber
which affects the adhesion and wettability characteristics of the composites [128]. The
mechanical properties of biopolymer composites, mainly, tensile, flexure, impact,
dynamic mechanic thermal property, toughness, hardness, ductility, brittleness, creep
and fatigue are been discussed.
Tensile properties
One of the most popularly employed tests for determining the mechanical properties and
knowing the structural design of biopolymer composites are tensile tests. Young’s
modulus is the ratio between stress and strain (in short known as stiffness) of
a material at the elastic stage of a tensile test [1]. Since fibers have higher strength and
stiffness than biopolymers, the latter is reinforced to the biopolymer matrix to enhance
the tensile properties of the composite. Depending on the type of fiber and biopolymer,
the tensile strength, Young’s modulus and elongation at break varies [128]. Out of all
natural fibers, bast fibers exhibit highest tensile strength and Young’s modulus, and are
most commonly used in biopolymer composites because of their availability. Flax fibers
also show similar properties because of low microfibrillar angle and high amount of
cellulose. Ramie and curaua fibers exhibit excellent modulus of rupture and hemp fiber
possess stiffness much greater than E-glass fibers. It is reported that unidirectionally
oriented ramie fiber-reinforced soy protein concentrate (SPC) composites showed tensile
properties similar to steel [129]. One the other hand, coir possesses the lowest tensile
strength among all natural fibers, due to high microfibrillar angle and low amount of
cellulose [128]. The concentration of reinforced fiber greatly determines the tensile
properties of biopolymer composites. PHB composites were prepared by reinforcing
0–30 wt. % coconut fiber. From the experiment, the best results were acquired for the
composite prepared with 10 wt. % coconut fiber, which improved tensile strength and
elongation at break by 35 and 25%, respectively, when compared to pure PHB composite
[130]. However, Petinakis et al. [131] in their study stated that tensile strength of wood
flour fiber/PLA composite is not much dependent on wood flour content. They improved
the tensile strength and tensile modulus of the biopolymer composites by 10 and 135%,
respectively, with the addition of a coupling agent, methylenediphenyl-diisocyanate
(MDI). Besides, many studies showed that surface modification of fibers by chemical
treatment also improved the tensile properties of the biopolymer composites by mini
mizing the hydrophilic nature of the fiber and improving the fiber–matrix interaction.
Flexural properties
Flexural stiffness is a factor for determining the deformability, and flexural characteriza
tion test is the second most preferred mechanical test. Flexural property is dependent on
Young’s modulus and moment of inertia (a function of the cross-sectional geometry) of
a material [42]. The wood fiber-reinforced composites showed highest Young’s modulus
whereas the hemp, ramie, sisal, and caraua fiber-reinforced composites showed better
flexural modulus of rupture [128]. Usually, by increasing the fiber content, the Young’s
modulus and flexural strength along the longitudinal direction increased in biopolymer
composites, while the Young’s modulus and flexural strength exhibited minimal changes
along the transverse direction [128]. Sawpan et al. [132] in their study investigated the
flexural properties of 30 wt. % hemp fiber-reinforced thermoplastic (PLA) and thermo
setting (unsaturated polyester resin) composites prepared by compression molding
method. It was revealed that, by the increase in fiber loading, the Young’s modulus
increased but the flexural strength decreased. The decreased flexural strength is due to
the weak spots (also known as “kinking”) in the hemp fiber which induces stress
concentration in the polymer matrix. So, by increasing the fiber content, the number
of kinks increases, which thereby reduces the flexural stress of the composites. In another
study with melt blending technique, biodegradable composites were made by reinforcing
oil palm empty fruit bunch fiber in PCL matrix. Due to the incompatibility of oil palm
fiber with PCL, polyvinylpyrrolidone (PVP) was used as a binder to enhance the fiber–
matrix interaction, and the prepared composites were subjected to irradiation to aug
ment the mechanical properties. The study indicated that, with 10 kGy dosage and
addition of 1 wt. % PVP, the flexural strength, and modulus of biodegradable composites
were increased [133].
Impact properties
The capacity of a material to withstand fracture under applied speed is the impact
strength of that material [42]. Since natural fibers innately possess low impact strength,
it is required to perform impact tests on biopolymer composites. Several factors like fiber
and biopolymer type, particle size, interfacial adhesion and test, and specimen condition
(unnotched or notched) affect the impact resistance of the composites [128]. In a study, it
was found that, by reinforcing PLA composites with bamboo fiber the impact strength
decreases, and for increasing the same, the fibers were modified by silane treatment. After
treatment, there was 33% increment in impact strength of the composite [134]. The
impact strength of the biopolymer composites can also be enhanced by hybridization
technique [128].
Dynamic mechanical thermal properties

Dynamic mechanical thermal analysis (DMTA) determines the heat deflection tempera
ture (HDT) of biopolymer composites. The test compliments both mechanical test
methods as well as thermal techniques (DSC and TGA) [128]. The test is usually
performed with ASTM D648, ASTM D5023–15 and measured in Thermal Analysis
Instruments. The elastic response (storage modulus), viscous response (loss modulus)
and damping (tan δ) values of a material are the function of temperatures at 3 °C/min [3].
Incorporation of natural fibers to a biopolymer matrix increases the stiffness and imparts
good stress transfer to the matrix, which further augment the storage modulus of the
composite [128]. The overall dynamic properties are governed by the type of polymer,
plasticizer and reinforcement technique [3]. Oksman et al. [135] prepared flax fibers (30
and 40 wt. %) reinforced PLA composites in a twin-screw extruder by adding triacetin as
plasticizer. The thermal properties were decreased by the addition of plasticizer, but from
the DMTA analysis, it was found that the storage modulus increased and the material
softening enhanced from 50 to 60°C. PLA composites were prepared by reinforcing kenaf
fibers (0 to 40 wt. %) and polyethylene glycol (PEG) (as plasticizer) in a mixer, followed
by compression molding. The incorporation of PEG created plasticizing effect and
decreased the glass transition (Tg) from 63 to 40°C [136]. The qualitative information
of fiber matrix interfacial characteristics can also be obtained by DMTA analysis [128].
Toughness and hardness properties

The toughness and hardness properties depend upon the strength and ductility of
a biopolymer composite. The ability to absorb energy and plastically deform without
fracturing is regarded as toughness of a material. Whereas, the fracture toughness is the
property of a material to resist fracturing by getting a crack [128]. The toughness of
a biopolymer composite can be measured by impact tests, while the fracture toughness is
analyzed by varied techniques like Kahn test and plane strain fracture toughness.
Hardness of a biopolymer composite is its ability to resist the permanent plastic defor
mation when a compression force is applied [128]. It is mostly determined by Rockwell
hardness tester, besides others like indentation, rebound and scratch. The usual indenta
tion hardness scales are Vickers, Rockwell, Brinell and Shore. Several factors like stiffness,
toughness, ductility, plasticity and visco-elasticity affect the hardness of a biopolymer

composite [128].
Creep and fatigue properties

Creep in a biopolymer composite is the tendency to deform slowly but permanently due
to mechanical stress [128]. Even though creep occurs at high-stress levels, because of
long-term stress exposure it will be below the yield strength of material. Unlike brittle
fractures, creep fracture is not instantaneous and is a time-dependent deformation,
where the accumulated strain is due to long-term stress [128]. The creep properties like
creep strength and creep modulus are determined as time and temperature function,
and most of the creep behavior is dependent on time, temperature, relative humidity
(RH) and load [137]. Fatigue is the structural damage due to cyclic loading and
unloading of a material. Similarly like creep failure, fatigue failure takes place within
the yield stress limit. The structure or shape of the biopolymer composite influences the
fatigue properties [128].
Brittleness and ductility properties

If a biopolymer composite under stress, breaks with or without noticeable deformation
then the material could be considered as brittle or ductile. Unlike glass fibers, natural
fibers deform before fracture, and thus have a significant relation with impact proper
ties. Under stress, if the biopolymer composites are ductile, they tend to deform before
complete failure and if the biopolymer composites are brittle, they break. The ductile
biopolymer composites gain more energy before fracture while brittle ones gain
relatively less energy [128]. The brittleness and ductility behavior of the biopolymer
composites are examined along impact tests and usually not determined by any
separate methods. The ductile-brittle transition PLA composites reinforced with
kenaf fibers were investigated by Kaiser et al. [138]. The team explained the sensitivity
of the composite toward mechanical properties to temperature with respect to brittle
and ductile fracture. Since, many studies have revealed that the mechanical properties
of fiber-reinforced biopolymer composites have relatively higher mechanical properties
than unreinforced biopolymer composites. The enhancement in these properties is due
to the use of small-sized fiber particle, surface area and elevated aspect ratio of the fiber,
homogeneous distribution of fiber in the matrix, and strong interaction between fiber
and matrix [1].
Tribological properties
Due to wider production and application of natural fiber-reinforced biopolymer compo
sites it is necessary to understand their tribological properties. Tribology is the study of
friction and wear of two mating surfaces [3]. Many research works have revealed that by
the addition of natural fibers the friction and wear performance of biopolymer compo
sites can be improved [60,139]. A commonly used wear test is “Pinon disc” test proce
dure, which includes sliding wear, with constant contact area. Another test for
determining the friction and wear performance is “Dry sand rubber wheel”, performed
according to ASTM G65 and “Block on ring tribo test”, performed according to ASTM
G77, G137–95 [3]. It is necessary to understand the environmental conditions on
performing tribological tests as each practical application has a different environment.
Application of biopolymer composites

The detrimental increase in the use of conventional plastics has led to the invention of
fully biodegradable alternatives to reduce the environmental pollutions. The natural
fibers have shown their excellence in replacing expensive carbon fibers and glass fibers
over decades. When compared to these synthetic fibers, natural fibers possess lesser
density, and hence are light weight and help in enhancing fuel efficiency [43]. During late
twentieth century, the practical applications of biopolymer composites started [3].
World-wide the natural fibers are commonly used in varied applications such as auto
mobiles and aerospace, sports, medical implant and drug deliveries, textiles, packaging,
infrastructure and building, upholstery and furniture, and many household products
[140]. In the near future, wider applications of biopolymer composites are likely to
increase considerably in industrial markets.
In automobile industries, natural fiber-reinforced biopolymer composites can
impart several advantages over conventional composites, like improved stability,
reduced cost and weight, enhanced acoustic insulation and mechanical properties,
reduced wear of machinery and tools, lesser or no release of toxic/noxious gases,
along with recyclability, renewability, and eco-efficiency [12,34]. The biopolymer
composites prepared from PLA reinforced with natural fibers like kenaf and jute with
good strength and mechanical properties are found to be an excellent application in
interior automotive parts, where strength of composite is a necessity for performances.
Kenaf fibers have also been explored to improve the mechanical properties of structural
elements in automobiles. Cotton and coconut fibers are used to make insulation
materials in automotive sectors. In Germany, the renowned automotive companies
like Bayerische Motoren Werke AG (BMW), Mercedes, Volkswagen, Audi, Opel,
Daimler Chrysler and Ford employ natural fiber reinforced polymer composites for
numerous exterior and interior applications [141]. PROTON Holdings Berhad (PHB)
or Proton, a Malaysian automotive company also engages in natural fiber-reinforced
composites for various applications [140]. Natural fiber-reinforced composites are used
to manufacture components like door panels, cushioned seats, cabin lining, dash
boards, package trays and headliners [11]. FIAT, an Italian automobile manufacturer
employed wood flour filled door panels in Brava, Punto, Marea, and Alfa Romeo
models [142]. From studies it is seen that Daimler-Benz incorporated coconut fibers
in the body parts and Audi A3 used hemp fiber-reinforced composite in the side panels.
Toyota, a Japanese multi-national automotive manufacturer in their first commercial
vehicle employed composites manufactured by reinforcing kenaf fibers in PLA matrix
developed from sugar cane and sweet potatoes in spare tire cover of RAUM 2003 model
[3]. Other automotive applications of biopolymer composites are seen in bamboo and
kenaf fibers reinforced composites in interior components (package shelves, floor mats
and luggage compartment) in Toyota’s Lexus models (CT200h and ES 300, HS), ramie
and kenaf fiber-reinforced PLA composites in translucent roof in Toyota 1/X plug-in
hybrid concept vehicle and bamboo fiber-reinforced PBS composites in headliner/
ceiling material and bamboo fiber-reinforced PLA and PBS composites in preparing car
floor mats in Mitsubishi Motors Corporation [43,74].
As an alternative to aluminum alloys and E-glass/epoxy composites, completely
biodegradable bamboo fiber reinforced PLA composite panels and boards were prepared
possessing excellent mechanical strength [143]. The PLA/PBAT composites developed by
reinforcing surface modified kenaf fiber with 2 wt. % (3-aminopropyl)trimethoxysilane
(APTMS) as compatibilizer in 90:10 wt. % ratio exhibited strong improvement in
toughness, tensile and flexural strength because of good interfacial adhesion between
natural fiber and biopolymers [144]. Dorez et al. [145] prepared PBS based composites by
adding natural fibers along with ammonium polyphosphate (APP) as fire retardant for
designing interior body parts of vehicles. On fire exposure, the APP improved the fire
retardancy property by imparting phosphorylation of natural fibers and hot hydrolysis of
PBS, thus forming as a barrier layer over the composite. Improved mechanical strength of
biopolymer composites fulfills the requirement in designing and engineering applica
tions in automotive industries.
The noticeable characteristics of plant fibers like lightweight, stiffness, good acoustic
insulation, and thermal properties have made them suitable for use in the construction
industry [11]. Plant fibers are usually employed in manufacturing construction materi
als such as internal/secondary structural elements, light-weight structures, partitioning,
surface panels, facade panels, doorframes, and other architectural uses [11,38].
Biopolymer composites have shown their ability to substitute furniture and wood
fittings, fixtures, noise-insulating panels, marine piers, and flower pots [38]. The
wood fiber-reinforced polymer composites are employed in outdoor decking, windows,
and furnitures. The wood-filled polymer composites are composed of about 30–70 %
wood content [11]. The natural fibers have also proved their functionality in wound
healing and drug delivery. The nanofibers prepared from natural fibers were used for
release of vitamins/drugs, as they are compatible with any hydrophobic polymer and
extend the durability and release of vitamins/drugs in a sustained manner [146].
Natural fibers are widely accepted in transdermal drug delivery (TDD) applications,
because of their ease of addition in biological compounds, controlled drug release and
permeation characteristics [146]. In biomedical and electronic application, the nano
fiber structured silk/chitosan composite films prepared by facile solution casting
technique exhibited improved hydrogen bonding interaction, mechanical perfor
mance, and biocompatibility with living cells. The biopolymer composite films can be
potentially employed in biomedical and electronic display screens because of their
strong nanofibril structure [147].
Durability of biopolymer composites

Natural weathering conditions like humidity, temperature, rain, and UV radiation
negatively affect the characteristics and properties of biopolymer composites [38]. Thus
determining durability of biopolymer composites is an essential factor to understand the
application and performance of the materials for a longer run. The durability of biopo
lymer composites is governed by many factors like moisture absorption, thermal stability,
flame retardancy, UV resistance and biodegradability of natural fiber, biopolymer as well
its composites.
Moisture absorption
Moisture exposure of biopolymer composites always negatively affects the performance
of the composites. Water has the tendency to plasticize the natural fiber and biopolymer
and thereby reduces the stiffness of the composite. Differential expansion between
natural fiber and biopolymer lead to the permanent damage of the fiber–matrix interface
[38]. When the natural fibers absorb moisture and get saturated, they swell, shrink and
lose their physical characteristics, which leads to the entry of moisture to the fiber-matrix
interfacial region [6]. The swelling of fibers leads to poor dimensional stability, and as the
moisture enters to the fiber–matrix interface delamination occurs. The fiber-matrix
debonding is actuated by osmotic pressure development at the surface of the fiber due
to leaching of water-soluble substances from the fiber [148]. A pictorial representation of
moisture absorption of biopolymer composites is summarized in Figure 3. Research has
also stated that moisture absorption increases with increase in fiber volume fraction [38].
The biopolymer composites manufactured with hydrophilic biopolymers (like cellulose
and starch) show greater moisture absorption when compared to composites prepared
with hydrophobic biopolymers (like PHB and PHBV) [38]. From studies, when hemp/
cellulose acetate and sisal/MaterBi-Y (derived from cellulose and starch) biopolymer
composites exposed to water immersion and high humidity, there was 70% and 30–50%
loss in tension modulus and flexure modulus, respectively [149–151]. It is stated that
even though hydrophobic matrices absorb less moisture, they retain more permanent
damage than their hydrophilic counterparts due to moisture absorption. This is because
of the high internal stress in stiffer materials leading to cracking, caused by swelling of
fibers in the biopolymer composites. Christian and Billington [149] demonstrated that
there was remarkable cracking and less recovery of mechanical properties for hemp/PHB
composites when compared to hemp/cellulose acetate composites on drying.
Thermal stability
Even though, each material has its own innate decomposition temperature, the physical
characteristics and decomposition temperature of the material change if it is blended or
Figure 3. Effect of moisture absorption on biopolymer composites.

combined with another material [1]. To ensure that there is no change in chemical and
physical properties of biopolymer composite, it is necessary to know and monitor the
thermal stability of materials. Thus the thermal stability of natural fiber and biopolymer
determines the thermal activity of the composite. The thermal stability of biopolymer
composites is usually determined by DSC, TGA and DMTA. By TGA, the degradation of
composite material at high temperatures is analyzed and it is used for manufacturing and
fire exposure of composites. While the degradation at lower temperatures is useful for the
comparison of thermal stability in specific service ranges [148]. The analysis help to
determine the maximum heat required to degrade the biopolymer composite and to
evaluate the residue left behind after degradation. Besides, it is possible to determine the
weight loss of the biopolymer composites with increase in temperature [1].
Many studies reported that by fiber incorporation the thermal insulation properties or
thermal stability of biopolymer composites can be improved. Recently, the thermal
stability of PBAT/PLA composites reinforced with varied natural fibers, wood fibers,
wheat husk, rice husk, and textile waste fibers was analyzed by TGA. From the experi
ment, it was observed that by the addition of natural fibers, the initial degradation
temperature decreased [152]. The effect of reactive compatibilization on thermal stability
of miscanthus/PHBV biopolymer composites prepared by extrusion and injection mold
ing was determined by Muthuraj et al. [153]. It was found that, by the incorporation of
natural fiber and dicumyl peroxide (DCP) there was significant reduction in the onset
degradation temperature, along with improvement in tensile and flexural strength of the
composites. Similar results on thermal stability was observed in miscanthus fiber-
reinforced PBAT composites [154]. Hence, natural fiber-reinforced biopolymer compo
sites can be employed in manufacturing interior parts of aircraft and automobiles.
Modification of natural fibers by acrylonitrile grafting and acetylation has demonstrated
improvement in thermal stability [38].
Flame/fire retardancy
When biopolymer composite materials are chosen for thermal insulation applications or
as building materials, it is mandatory to determine the flammability and flame retardancy
property of composites by flame retardancy tests. Since natural fibers alone are highly
flammable, it is more likely to ignite and combust exothermically and burn itself
vigorously on combustion. Several factors influence the flammability of biopolymer
composites, like type of natural fiber and biopolymer, type of reinforcement, adhesion
between reinforcement and matrix, and the structure of the composite [155]. As the
chemical composition and microstructure differs from one fiber to another, the flamm
ability also varies accordingly. At elevated temperature, the major fiber components,
cellulose, hemicelluloses, and lignin markedly behave in different ways and thus the
composition of a natural fiber greatly influences the composite performance [38]. The
flammability of natural fibers increases with increase in cellulose content, and its decom
position emits flammable volatiles, noncombustible gases and tars leading to char for
mation. Lignin content is also responsible for char formation and it acts as a protection of
the underlying biopolymer composite integrity by serving as an insulation layer. The
natural fibers having high crystallinity and low polymerization are less flammable [38].
Usually, the flame retardancy test for natural fiber-reinforced biopolymer composites is
performed in a vertical Bunsen burner test, according to Federal Aviation Regulation

(FAR). Other horizontal and vertical fire tests are also employed to evaluate the flame
retardancy. By using tests with UL-94 horizontal and UL-94 vertical standards in
accordance with DIN EN 60,695–11–10, the ignitability and flame spreading rates
could be determined [3]. The fire testing instrumentation methods like Ohio State
University (OSU) rate of heat release apparatus technique, limiting oxygen index,
pyrolysis combustion flow calorimetry and cone calorimetry are also used [155]. All
these analyses correlate each other with the results of Bunsen burner test, horizontal and
vertical fire tests, thermo-mechanical analysis methods (DSC and TGA), spectroscopic
methods (FTIR and XRD), TGA-FTIR coupled systems and microscopic methods (SEM
and TEM) [155].
Jang et al. [2012, 156] by commingled yarn method prepared plasma-treated
coconut fibers reinforced PLA composites and investigated the flammability perfor
mance via loss on ignition (LOI) method. They reported that even though no
remarkable difference between the LOI values for the coconut fibers/PLA composites
was found, it was above 20 vol. % which indicates a non-flammability characteristic.
The tensile strength and Young’s modulus of the reinforced composite also
improved. The flame retardancy of ammonium polyphosphate (APP) added thermo
plastic starch (TPS) composites were analyzed and found that APP enhanced the
flame retardancy of the biopolymer composites. Also, a similar trend was noticed
when keratin fibers replaced 20 of 30 % of APP [157]. The fire resistance of
biopolymer composites can be increased by decreasing the flammability of the
components of composites [158]. To improve the flame resistance, various agents/
additives like dispersion and fire retardant agents and coupling are used in biopo
lymer composites. The addition of flame retardants reduce or avoid the combust
ibility in composites. The flame retardants by addition of filler and endothermic
process, cool and thins the flammable materials in gaseous or solid phase, and
isolate the material from fire source by forming a protective film coating over
biopolymer composites [42]. The composites can also be protected by intumescent
systems painted on its surface. On fire exposure, the systems char and expand, and
create a surface layer for limiting the access and permeation of oxygen and
heat [158].
In a study with commercial biodegradable blend kenaf/E-PHBV composites the
flame retardancy performance was assessed. The E-PHBV was composed of PBAT
and PHBV. To this composite, metal oxide (Sb2O3) and a phosphate-based additive
were added as flame retardants. The cone calorimetry test demonstrated that heat
release rate (HRR), peak/maximum heat release rate (PHRR) and fire spread indices
decreased by the addition of flame retardants. From the SEM analysis of the char
obtained from cone calorimetry tests, it was noted that the dense and porous
structure in the residue is due to the OH group rich kenaf fibers which stood as
a carbonizing agent that formed as a network of cavities and holes by pyrolysis gases
release [159]. The researchers at the Council of Scientific and Industrial Research
(CSIR) engaged in a project by collaborating with AIRBUS, a European multi-national
aerospace corporation for developing natural fiber-reinforced thermoset panels for
aircraft applications. They developed aqueous-based flame retardant treatments for
flax fibers to confirm that the composite panels follow the regulations of Federal
Aviation Airworthiness (FAA). Non fibrous natural silicate was also incorporated as
a fire-resistant material along with primary fire retardants in the composites. Finally,
the manufactured composites exhibited superior toxicity, smoke and flammability
properties for the aforementioned purpose [160]. Since gluten-based composites are
susceptible to fire, the fire retardancy can be improved by adding lasonol [161]. In
a study by Zainuddin et al. [162] on bacterial grade PHBV, the fire retardancy is
increased by incorporation of halloysite nanotube as a fire-retardant agent. But by
halloysite nanotube addition the mechanical properties of composite reduced. There
are numerous fire retarding agents employed in biopolymer composites, but most of
them possess some limitation or implement some concerns like hindering the
mechanical properties of the composites. So there is a need to discover newer fire
retarding agents that are compatible with composites without any effect in properties
and performance.
Ultraviolet resistance
Photodegradation occurs when the biopolymer composites are exposed to UV radiation.
In natural fibers, lignin is more susceptible to photodegradation and this results in
imparting a yellow color discoloration to the composites [38]. And as the lignin degrades
gradually, the cellulose which is less prone to UV degradation develops on the surface of
the composites [42]. When the biopolymer composites are exposed to solar radiation, the
radiation cleaves the covalent bonds in organic polymers, and further causes, discolora
tion, surface roughening, degradation of mechanical properties, and embrittlement
[148]. Campos et al. [163] in their experiment found that thermoplastic like sisal/starch
and sisal/PCL composites on UV exposure led to the decrease in mechanical properties,
holes in the surface, embrittlement and discolouration of the composites. In the labora
tory setup, the biopolymer composites are not just alone exposed to UV radiation, but
they are exposed to a combination of moisture, temperature and UV source intended to
simulate actual conditions at an accelerated rate. To an extent, the UV degradation can be
overcome by bonding chemicals to the cell wall polymers that decreases the lignin
degradation and also by adding polymers to the cell matrix to keep the degraded fibers
structure together [42].
Biodegradability
The microbial growth on biopolymer composite depicts the biodegradation ability of the
material. The presence of lignin in natural fibers makes them resistant to microbial
degradation. While, less lignified natural fibers are prone to microbial degradation of
cellulose and hemicelluloses [6]. Also, moisture exposure and absorption promote
bacterial growth [148]. The mechanical strength of biopolymer composites are reduced
by cellulose degradation via dehydration, hydrolyzes and/or oxidation [42]. From labora
tory studies, it is found that natural fiber-reinforced biopolymer composites from PHB,
PBS and PLA, biodegrade by anaerobic digestion and/or enzymatic degradation
[164,165]. The soil burial tests of sisal/Mater Bi-Y composites shows that the microbial
load in soil biodegrades the biopolymer composites by creating holes and cracking over it
and thereby reducing its mechanical properties [166]. Barkoula et al. [167] in their work
stated that flax fiber-reinforced PHB matrix composite showed noticeable reduction in
tensile strength in the initial stage of biodegradation study, but later it was more gradual
in the next stages of degradation. In a study, a series of composite boards were prepared
from varied mixtures of bamboo/PLA and chemical, physical, mechanical and biological
properties were analyzed. The samples were exposed to three different wood-decaying
fungi for 60 days and observed that all the species degraded all the composites expect
pure PLA composite. After 1500 h of biological exposure, the biopolymer composite
samples showed nearly zero water absorption and swelling thickness. The study showed
that PLA composites has the ability to remain water resistant, but more research is
needed to confirm the durability of these composites [168].
The natural fibers can be protected from biodegradation by making them less
hygroscopic and less susceptible to enzymes [6]. Other way is the surface modifica
tion of natural fibers by chemical treatment and thereby reduces the moisture
content below microbial requirement for growth. Biodegradability of biopolymer
composites can also be delayed by harsh chemical against microbes and to slow
down biological attack [42]. One main issue governing the durability of biopolymer
composites is that how easily and rapidly the resistance of the composite materials
could be evaluated for biodegradation study [6]. Several groups like European
Standardization Committee (CEN), American Society for Testing and Materials
(ASTM), International Organization for Standardization (ISO), Italian
Standardization Agency (UNI), German Institute for Standardization (DIN),
Institute for Standards Research (ISR), and Organic Reclamation and Composting
Association (ORCA) made different techniques for biodegradability assessment
under varied environment [6]. However, a single standard method for determining
the biodegradability of biopolymer composites has not been stated. The lack of
standardization leads to testing of different polymers and conditions suitable for
optimizing the composite materials. Ultimately, the methods to control the biode
gradability of biopolymer composites should be developed to use these eco-friendly
materials as an alternative to petrochemical-derived counterparts.
One of the feasible ways to conduct durability management of biopolymer composite
is to wisely choose the function and application of each raw material, so that the required
performance is met by controlling the weakness and taking the advantages of the
strengths of these materials [38]. So while designing a biopolymer composite, the most
essential things to consider are the thermal stability, dispersion, and surface attachment
qualities of fibers in biopolymer matrices. Due to thermal decomposition/degradation of
natural fibers, the compounding temperature is confined to max. 200 °C [169], as natural
fiber mostly starts to degrade around 240°C [35]. The fiber volume fraction also should
be considered while designing a biopolymer composite, as increase in the fraction can
have both merit and demerit, as it give rise to improved mechanical performance and
moisture-related damages, respectively [38].
Hybrid composites
Hybrid composites are the composites developed by reinforcing two or more natural
fibers to a matrix. Researchers in their studies have selected the best combination of
natural fibers to obtain the best possible result to utilize the combined benefits of
fibers and reduce the negative aspects [5]. Mixing different fibers enhances the tensile
properties of the composites [128]. Hybridization of fibers with different diameter
increases the fibers matrix adhesion effective area for uniformly transferring the
stress. For instance, even though a fiber having low elongation is used, the mechanical
properties can be maintained by transferring the stress to another fiber with high
elongation in the composite [4]. Usually, reinforcement methods in hybrid compo
sites are by mixing two types of short fibers prior the addition of matrix, or by adding
each fiber alternatively by layering in the matrix [5]. The strength of the hybrid
composites depends on the length of individual fiber, fiber properties, aspect ratio of
fiber content, orientation of fiber, extent of intermingling of fibers, fiber-matrix
interfacial bonding and arrangement of both the fibers and failure strain of individual
fibers [7].
Bax and Müssig [170] in their study found that the rigidity and strength of the PLA
composite was remarkably improved by reinforcing the composite with man-made
cellulose, abaca, and jute fibers. Depending on the fiber type, the mechanical proper
ties of the composites varied. By solution casting procedure, a blend of 90% PVA and
10% cellulose nanofiber (from varied sources like hemp, flax, kraft pulp or rutabaga)
was prepared to make nanofiber-reinforced composite film. It was observed that the
Young’s modulus increased four to five times greater than pure PVA film [171]. PLA
composites were prepared by reinforcing sisal and banana fiber by twin-screw extru
sion and injection molding. Prior to composite processing the sisal fibers were
subjected to alkali treatment with 6% benzoyl peroxide and acetone solution for
30 min at 70°C. The study reported that by chemical modification of natural fibers,
the tensile, flexural, and impact strength of the hybrid composites improved [172].
The properties of hemp, kenaf, cotton, and lyocell PLA composites was observed and
the study revealed that kenaf and hemp/PLA composite exhibited great tensile
strength and Young’s modulus and the cotton/PLA composite showed good impact
strength [173].
Recyclability of biopolymer composites

The end of life scenarios of polymers and polymer matrix composites receive
increasing attention, since a huge amount of plastics is simply being mismanaged.
The “circular economy” vision for plastics is far from being within reach, with the
industry talking about “thermal recycling”, a gross misnomer for “incineration”.
Ngaowthong et al. [174] studied the recycling of sisal fiber-reinforced PP and PLA
composites and found that 4 rounds of recycling did not affect the stability of the
PP composite, whereas the PLA-based material showed strong degradation.
Increasing the bio-based carbon content of products can reduce their carbon
footprint. In any case, a circular economy approach where plastics composites and
plastics in general are used more than once is to be targeted. Feedstock recycling is
one option, another one cascaded use, apart from established collection and remold
ing in less demanding products as for thermoplastics. Out of all polymers, thermoset
recycling is more challenging. The huge varieties of composites express great
difficulties to meaningfully recycle the materials. So standardization could help
increase recycling rates.
Limitations and future trends of biopolymer composites

Besides advantages, there are some noticeable limitations in biopolymer composites. The
poor moisture resistance, dimensional stability, thermal decomposition temperature, fire,
UV, and biological resistance of biopolymer composites when compared to conventional
plastics limit the growth of its potential applications [38,42]. The use of natural fibers
improves the impact strength of the biopolymer composite, and it increases with increase
in fiber content. But, as the amount of fiber increases the ductility, water absorption
tendency and undesirable odor is increased in the composite [15]. Another notable
limiting factor for utilization of biopolymer composites in heavy load-bearing, interior,
and non-structural applications is the limited compatibility of natural fibers and biopo
lymers [3]. The extent of compatibility between natural fibers and biopolymers influence
the mechanical properties, durability, and performance of the composites. The long-term
characteristics like creep and fatigue behaviors, durability and lifetime prediction of
biopolymer composites is precisely unknown and is a major concern [175]. So some
new methods and experimental techniques should be adopted to study the performance
of biopolymer composites over its lifetime. It is also noted that for commercial produc
tion, the biopolymer composites are engineered through fiber treatment, biopolymer
blending, plasticizer, and other filler addition, coating and other advanced processing
methods. In spite of the fact that natural fibers and biopolymers are cost-effective than
synthetic counterparts, some processing methods demand a good amount of capital
investment and energy requirement [38]. So to combat these limiting factors, some
critical aspects and recommendations to be noted in future researches on biopolymer
composites are:
● Exploration, identification, and characterization of new natural fibers are essential

for the wider application of natural fibers to replace hazardous synthetic fibers.
Studies on animal fibers reinforced biopolymer composites are still minimal, even
though animal fibers are known to possess better mechanical properties than plant
fibers.
● Among currently used fiber extraction methods, no extraction technique has been
identified as standard method for a specific type of fiber. It is also very well observed
that there is no specific standard method for manufacturing biopolymer composites.
Establishing standard procedures for composite preparation saves optimization
time, energy and raw material utilization.
● For application of biopolymer composites in various fields like automotive and
construction sectors, it is necessary to perform quality assurance and develop
optimized natural fibers due to its widely dispersed resources and variable
properties.
● It is also important to study more about the effect of reinforcing modified natural
fibers to biopolymer composite to predict the suitable application and also to foresee
its potential performance. And also, innovations in surface modification techniques
need to be explored to adopt methods which are more cost-effective and eco-
friendly.
● Even though natural fiber-reinforced biopolymer composites have shown its applic
ability in automotive, aerospace, electronic and biomedical applications, more
research is needed in medical scaffolds for wound healing process and tissue
engineering. In automotive sectors, biopolymer composites have made substantial
commercial markets for value-added products. Likewise, value addition in other
fields need to be focused and promoted.
● One major drawback of bio-based materials is the difficulty in understanding its
durability. The unpredictable durability along with limited mechanical strength is
a major limiting factor for the use of biopolymer composites in automotive sectors.
Most of the knowledge about the durability of biopolymer composites is based on
laboratory-scale experiments. The in situ behavior of composites has not been
greatly analyzed to validate the laboratory results and findings. New experimental
techniques should be explored to monitor, evaluate and control the durability and
biodegradability of biopolymer composites.
● The research should also focus one major area, that is, load-bearing characteristics
of biopolymer composites. Developing load-bearing biopolymer composites widens
the use of biopolymer composites for various structural applications.
● The long-term performance of biopolymer composites need to be improved and
monitored to its extensive use in construction sectors. New techniques to conduct
performance evaluation in biopolymer composites are necessary to understand the
effect of environmental conditions in thermal, mechanical, and durability of
composites.
● Hybridization is an effective technique that needs more attention to develop novel
and efficient biopolymer composite products. It is an advantageous method to
combine natural fibers of varied characteristics to produce composites with excel
lent strength and properties.
● Recyclability of composites is a promising area to explore. Future studies on the
recyclability aspects of biopolymer composites is needed to reuse the composites in
way or the other, rather than subjecting it for biodegradation after its specified use.
● Since biopolymer composite is a product of synergism of properties of natural fibers
and biopolymers, the invention and development of component-dependent and
non-dependent blending system is a major area need to be focused.
● The use of nanotechnology has shown numerous opportunities for enhancing
characteristics of biopolymer composite products. Studies have reported that the
nanocrystalline cellulose is stiffer than aluminum and stronger than steel. So devel
opment of nanofibers from natural fibers is a promising field for structural applica
tions of biopolymer composites.
Conclusion
Since last few decades, there is gradual increase in the industrial interest in biopolymer
composites. Natural fibers on modification have shown its ability to overrule synthetic
fibers with its abundant availability, low cost and eco-friendly characteristics. Out of all
natural fibers, kenaf fiber has shown its sturdy mechanical properties and jute fiber has
exhibited maximum strength and excellent compatibility with biopolymers. Since natural
fibers are used for composite preparation and other purposes, it promotes farming and
sericulture, thereby reduces air pollution by reducing greenhouse effect and also helps in
improving soil fertility. Biopolymer composites are renewable, non-corrosive, eco-friendly,
biodegradable, lightweight, easily manufactured, and also possess high specific strength and
stiffness that is amenable to be tailored to satisfy varied performance requirements. The
performance of biopolymer composites depends upon numerous factors such as chemical
composition, physical properties of fiber and biopolymer, fiber modification techniques,
fiber volume fraction, amount of additives and plasticizers, method of reinforcements,
geometry and orientation of fiber in matrix, structural defects, interaction between fiber
and biopolymer, and environmental condition of the composites. Another widely accepted
composite development technique is by combining different types of fibers in a single
matrix to develop highly valued hybrid biopolymer composites. The studies revealed that
the biopolymer composites are compatible with automotive, aerospace, construction,
biomedical, and food industries, and proved to have versatile applications. In near future,
further researches on biopolymer composites have the potential to substitute the conven
tional petroleum based plastics. There is possibility in the development of new markets
when these biopolymer composites become more durable with improved performance.
Few characteristics need to be noted whenever a natural fiber is reinforced to a biopolymer
matrix, is to know the purpose, final design, and environmental condition that the material
is exposed to. Continuous exploration on performance and life-cycle assessment is neces
sary to find out more applicability of the biopolymer composites.
Acknowledgments
The authors wish to thank Dr. Shijin A, veterinary surgeon, Akhila P P and Zahle Khan for their
constant support.
Disclosure statement
No potential conflict of interest was reported by the authors.
Notes on contributors
Basheer Aaliya is a researcher scholar in Food Science and Nutrition, Department of Food Science
and Technology, Pondicherry University. Her research interest is the isolation, modification and
characterization of non-conventional starch.
Kappat Valiyapeediyekkal Sunooj is an assistant professor in Department of Food Science and
Technology, Pondicherry University. His doctoral research was on meat science from Defence
Food Research Laboratory (DFRL), DRDO. Currently Dr. Sunooj is widening his research on
starch modification, plasma technology and biopolymer science.
Maximilian Lackner earned his Ph.D. from Vienna University of Technology. From 2004 to 2011,
he worked in the polymer industry in Austria and China in several senior leadership positions. In
2013, he founded a company actively involving bioplastics trading, development and consulting.
Dr. Lackner is a lecturer at The University of Applied Sciences FH Technikum Wien.
ORCID
Basheer Aaliya http://orcid.org/0000-0002-3353-109X
Kappat Valiyapeediyekkal Sunooj http://orcid.org/0000-0002-7269-4473
Maximilian Lackner http://orcid.org/0000-0002-2673-7495
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International Journal of Biobased Plastics

ISSN: (Print) (Online) Journal homepage: www.tandfonline.com/journals/tbbp20

Biopolymer composites: a review

Basheer Aaliya, Kappat Valiyapeediyekkal Sunooj & Maximilian Lackner

To link to this article: https://doi.org/10.1080/24759651.2021.1881214

© 2021 The Author(s). Published by Informa

Published online: 05 Feb 2021.

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Biopolymer composites: a review

ABSTRACT ARTICLE HISTORY

CONTACT Kappat Valiyapeediyekkal Sunooj [email protected] Department of Food Science and

Classification of natural fibers

Extraction and processing techniques of natural fibers

Mechanical or green retting

Figure 1. Water retting process.

Figure 2. Mechanical retting process.

Chemical and surfactant retting

Protein and enzyme retting

Chemical composition of natural fibers

Physical properties and characterization techniques of natural fibers

Drawbacks of natural fibers

Modification methods of natural fibers

wettability, insulation, tribological properties, and biocompatibility of fibers with the

composite applications are sustainability, cost effectiveness, lightweight characteristics,

Processing techniques of biopolymer composites

Table 1. Improved properties of various biopolymer composites prepared by different processing

Characterization of biopolymer composites

(ISS), Auger electron spectroscopy (AES), X-ray photoelectron spectroscopy (XPS),

Mechanical properties of biopolymer composites

Dynamic mechanical thermal properties

Toughness and hardness properties

toughness, ductility, plasticity and visco-elasticity affect the hardness of a biopolymer

Creep and fatigue properties

Brittleness and ductility properties

Application of biopolymer composites

Durability of biopolymer composites

Figure 3. Effect of moisture absorption on biopolymer composites.

performed in a vertical Bunsen burner test, according to Federal Aviation Regulation

Recyclability of biopolymer composites

Limitations and future trends of biopolymer composites

● Exploration, identification, and characterization of new natural fibers are essential

Maximilian Lackner http://orcid.org/0000-0002-2673-7495

20. Vijay R, Singaravelu DL, Vinod A, et al. Characterization of alkali-treated and

86. Yu T, Ren J, Li S, et al. Effect of fiber surface-treatments on the properties of poly(lactic

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