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Natural fibre reinforced composites: A review based on additive

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DOI: 10.1016/j.matpr.2022.02.607

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journal homepage: www.elsevier.com/locate/matpr

Natural fibre reinforced composites: A review based on additive

manufacturing routes and biodegradability perspective
Anumoy Ganguly a, Shiv Shankar a, Ashish Das b, Mukul Shukla c, Chetan Swaroop d,⇑, Tarun Bhardwaj e
a
Division of material science and engineering, RWTH Aachen University, 52074, Germany
b
Department of Production and Industrial Engineering, National Institute of Technology Jamshedpur, Jharkhand, India
c
Department of Mechanical Engineering, Motilal Nehru National Institute of Technology Allahabad, Prayagraj, India
d
Department of Mechanical Engineering, United College of Engineering and Research, Prayagraj, Uttar Pradesh, India
e
Department of Mechanical Engineering, Ajay Kumar Garg Engineering College, Ghaziabad, Uttar Pradesh, India

a r t i c l e i n f o a b s t r a c t

Article history: Natural fibres derived from plants, animals, and minerals have been used by humans since the start of
Available online xxxx civilization. Since then, with the changing human needs, these naturally occurring fibres are finding
new applications and uses. Due to their high specific strength, low density, and biocompatibility, these
Keywords: natural fibres have found use as filler materials in advanced composite materials in the 21st century.
Natural fibres In an environment concerned and the energy-hungry world, another notable stride towards sustainable
Polymer engineering is the use of additive manufacturing. Due to its low energy consumption, minimal material
Additive manufacturing
wastage, and easy fabricability of complicated parts, additive manufacturing has gained attention as the
Composites
norm of the future. Hence, there has been increasing popularity to try and manufacture composite rein-
forced with natural fibres through the additive manufacturing route. In this paper, we have tried to sum-
marize the recent developments in the field of additive manufacturing of Natural fibre reinforced
composites. Comprehensive discussions regarding the different kinds of natural fibres, additive manufac-
turing routes, pre-processing of natural fibres and their biodegradability have been included. In the end,
we have drawn some conclusions and have suggested future directions to the research.
Copyright Ó 2022 Elsevier Ltd. All rights reserved.
Selection and peer-review under responsibility of the scientific committee of the International Confer-
ence on Advances in Materials and Mechanical Engineering. (ICAMME-2022).

1. Introduction NFRCs are inexpensive when compared to glass or metal reinforce-

In the wake of the 21st century, the world is becoming increas-
ingly concerned about the environmental impact of all the techno-
logical progress mankind has made. Naturally, mankind has turned
to the scientific community for possible solutions for sustainable
growth. A major portion of this seemingly tough problem is solved
by the use of environmentally friendly materials and processes
used to fabricate them. Hence, researchers all over the world are
trying to develop materials that are biodegradable yet meet the
stringent demands of service. Natural fibre reinforced composites
have hence emerged as a key research area in material research.
Various kinds of matrices have been used to fabricate natural
fibre reinforced composites (NFRCs), among which the ones with
thermo-plastic matrices have gained popularity. Moreover, these
⇑ Corresponding author.
E-mail address: chetanswaroop019@gmail.com (C. Swaroop).
ments and are abundantly available. However, NFRCs are yet to be
incorporated into actual use due to their poor mechanical, thermal,
and physical properties. Hence, more research and innovation are
needed in these domains. Currently, NFRCs are being exclusively
investigated for their lightweight and high stiffness to weight ratio,
biodegradable nature, and functional properties which have made
them a potential candidate for tissue engineering and specific parts
for automotive industries. Moreover, it has been found that NFRCs
are among the most frugal energy consumers during their fabrica-
tion with high energy recovery at the end of their life [1,2].
The global market for these Natural reinforced composites has
grown tremendously in the past decade and is expected to grow
at a constant rate over the next few decades with the construction
and biomedical sector being the largest consumers followed by the
automotive sector. The increasing awareness towards the use of
environmentally friendly materials will push the growth of NFRCs
in the coming decades. Yet, there are several hurdles to overcome

https://doi.org/10.1016/j.matpr.2022.02.607
2214-7853/Copyright Ó 2022 Elsevier Ltd. All rights reserved.
Selection and peer-review under responsibility of the scientific committee of the International Conference on Advances in Materials and Mechanical Engineering. (ICAMME-
2022).

Please cite this article as: A. Ganguly, S. Shankar, A. Das et al., Natural fibre reinforced composites: A review based on additive manufacturing routes and
biodegradability perspective, Materials Today: Proceedings, https://doi.org/10.1016/j.matpr.2022.02.607
A. Ganguly, S. Shankar, A. Das et al.
for NFRCs especially those manufactured through additive manu-
facturing. For the 3D printed NFRCs to perform under service con-
ditions, good interfacial properties of the natural fibre and the
polymer matrix are required apart from the problems of aniso-
tropy, nonuniform distribution of fibres and varying quality of
fibres obtained from different sources. These problems require us
to delve deeper into the understanding of the underlying mecha-
nism of additive manufacturing as well as composites in general.
2. Types of natural fibres
Natural fibres can be broadly divided into two classes a) Animal
fibre containing keratin b) plant fibre containing cellulose and c)
fibres obtained from minerals. Fibres can further be classified
according to their shape and size (aspect ratio) as long fibres and
short fibres. Long and short fibres play different roles when added
to composites as reinforcements.
2.1. Plant-based fibres
Plant-based fibres can be subdivided according to the part of
the plant they are obtained from. Often the structural entities are
different which leads to different mechanical properties when used
as reinforcements in polymer composites.
2.1.1. Seed fibres
Cotton, kapok, rice husk, almond seed skin, and wheat can be
classified as seed fibres. They are predominantly made up of cellu-
lose and long-chain carbohydrate molecules. These fibres have a
higher degree of polymerization when compared to other naturally
occurring fibres [3]. However, these fibres do not show significant
elongation before failure. Cotton fibre is rarely used as a reinforcing
agent due to its soft nature. Almond skin fibres are used in biomed-
ical implants due to their biocompatibility.
2.1.2. Stem fibres
Stem fibres are obtained from the inner living tissues of the
plant in between the inner cire to the dead bark. Flax, hemp, jute,
nettle, okra, and ramie falls under this category. They are com-
prised almost 70% of cellulose and display high tensile strengths,
hence are being extensively being investigated as reinforcements
in polymer composites. Stem fibres have fibre diameters ranging
from 12 lm to 17 lm.
2.1.3. Leaf fibres
Sisal, abaca and manila leaf fibres are commonly used in NFRCs.
They are especially popular in tissue engineering due to their bio-
compatibility. However, void and pore formation at the interface
and poor bonding with matrix degrade the mechanical properties.
Sisal fibres are hard and stretchy and have diameters from 200 lm
to 400 lm. Sisal fibres are extensively used as reinforcements in
polymer composites [3].
2.2. Animal-based fibres
Animal-based fibres can be classified into three types a) hair
fibre b) wool fibre and c) silk fibre.
Wool fibres are obtained from shearing animals like sheep and
goats. They are extremely durable and have great fatigue tough-
ness. It has been found that wool fibres can flex back and forth
20,000 times before failure and hence are used in polymer compos-
ites requiring high strength. Wool fibres are also fire resistant and
hence can be used in conjecture with asbestos in fire resistance
composites. Wool is being extensively investigated for use in pro-
2
Materials Today: Proceedings xxx (xxxx) xxx
tective gears for military use due to its flexibility, high strength,
and durability [3].
3. Additive manufacturing routes for NFRCs
Additive manufacturing is a technique that uses layer-by-layer
fabrication to build a 3D component from a computer-aided design
fed to it through a computer. The computer model is divided into
horizontal layers and each layer is then fabricated on top of
another. Additive manufacturing has the advantage of being able
to fabricate components of complex geometry in less time with
minimal steps with almost no wastage of materials. Different kinds
of AM processes exist and are used for different products depend-
ing on the material, complexity, desired property, and size [4]. Now
we shall discuss briefly the processes relevant to the manufactur-
ing of NFRCs.
3.1. Different AM techniques for NFRCs
Several AM techniques can be used to fabricate natural fibre
reinforced polymer matrix composites. The selection of the appro-
priate techniques depends on the feedstock materials, geometric
complexity of the desired part, and the kind of natural fibres used.
The most popular among these are the FFF, SLS, BJ, SLA, and DW
techniques.
The FFF process is the most extensively used technique to man-
ufacture polymer-based composites. It uses a feedstock in form of a
thin filament which is partially melted using a heat source,
extruded through the nozzle and deposited onto the substrate fol-
lowing the designated path specified by the CAM model. The pro-
cess is hence fast with the advantage of being able to use multiple
filaments of different materials. Usually, two filaments is used, one
that of the primary filler material and another composed of the
support material (which is then removed manually or by dissolu-
tion). However, the accuracy of FFF is not satisfactory for geomet-
rically intricate structures, where methods such as Selective laser
sintering are used.
Another process very similar to FFF is Direct writing (DW).
Direct writing is often referred to as inkjet 3D printing because it
uses a viscous solution contrary to ink in printing. The viscous liq-
uid is deposited with the help of a nozzle and allowed to harden. A
post-fabrication treatment may be used where heating, UV ray, or
reactive feedstock may be used to harden the deposited solution.
The advantage of DW is that complex composites with a
functional and compositional gradient can be manufactured.
The quality of the product obtained largely depends on the quality
of the solvent.
In the Selective laser sintering process, metal powders are sin-
tered using directed energy beams (laser or electrons). SLS is
extensively used to manufacture semicrystalline polymers which
do not require a separate support structure. The quality of the pro-
duct depends on the quality of the powder quality and hence pre-
cise control has to be exercised over the molecular structure [5]. In
the case of NFRCs, the fibre can be blended with the feedstock to
create an in-situ NFRC composite, but the non-uniform distribution
of these reinforcements remains a problem. However, even with
the advantage of being able to deliver intricate structures, only cer-
tain kinds of polymer (with low viscosity, high IR absorption, and
low surface tension) [5] are found to be suitable for SLS manufac-
turing because of the complex phenomenon of incipient fusion
involved.
Binder jet additive manufacturing is very similar to SLS except
for using a binder to hold the feedstock powder. The binder is
printed on the powder bed with the help of a printer according
to the CAD-CAM model and immediately heated by a heat source
A. Ganguly, S. Shankar, A. Das et al.
from beneath to dry off the binder. The sequential and timely exe-
cution of drying steps is of utmost importance for the geometrical
integrity of that layer and the structure as a whole. After all the lay-
ers have been solidified, the excess supporting powder is blown off.
The final product may require post-manufacturing treatments to
harden the binder (by heating) and initiate polymerization using
UV rays. A binder of suitable viscosity and a low spreading ten-
dency is essential for the geometrical accuracy of the fabricated
part. The advantage of this process is that a very wide range of
polymers may be fabricated by the BJ process if they are available
in powdered form and a suitable binder is available [6]. Properties
of the powder such as its size distribution, morphology, and rheol-
ogy directly influence the quality of the product (see Fig. 1).
3.2. Pre-processing of natural fibres
For sound mechanical and physical properties of the manufac-
tured composite, the distribution of fibres within the polymer
matrix and the fiber–matrix adhesion. However, it has been found
that most natural fibres do not bound well with the polymer
matrix because of the hydrophilic nature of most natural fibres
and the hydrophobic nature of the polymer matrix. Hence, the nat-
ural fibre has to be treated to modify its surface properties before
being incorporated as reinforcements [10].
3.2.1. Washing
Natural fibres such as jute, hemp, cotton, and fleece may have
been waxed to reduce friction while machining. The wax sticks
Fig. 1. Schematic representation of different AM technologies used to fabricate polymer and polymer composites (a) FFF [7] (b) DW [8] (c) SLS [7].
3
Materials Today: Proceedings xxx (xxxx) xxx
to the surface and may reduce the adhesion between the matrix
and reinforcements. Hence, all-natural fibres are washed thor-
oughly. Often cleaning agents like detergents are used to remove
grease and oils from natural fibres derived from animals.
3.2.2. Chemical treatments
As mentioned before, natural fibres are found to be hydrophilic
while polymers are hydrophobic, resulting in poor interfacial
bonding. Plant fibre is mostly comprised of cellulose which has
open hydroxyl groups in its structures. These hydroxyl groups form
a polar bond with neighbouring hydroxyl groups from other mole-
cules as well as moisture in the air. To inhibit these hydroxyl
groups, chemical reagents are used to replace the active hydroxyl
group. Nuno et al [9] has used a two-step process where diiso-
cyanate was used to mask the hydroxyl groups and in the second
step, polyol was added to form polyurethane moieties which
resulted in superior interface binding and improved mechanical
properties in the composite. A common practice is to add acetate
group to replace active hydroxyl group to improve the hydropho-
bicity. Heli cellulose and lignin another class of fibres found in ani-
mal and plant-based natural fibre are often treated with NaOH
followed by mildly acidic reagents to decompose the lignin and
hemicellulose and thus improve the reinforcement-matrix bonding
[11]. Acha et al [12], in their studies, have used lignin as a compat-
ibilizing agent to improve the interfacial bonding properties of
jute-fibre and polypropylene and observed improvement in several
parameters such as stiffness, tensile behaviour and impact proper-
ties (see Fig. 2).
A. Ganguly, S. Shankar, A. Das et al.
Fig. 2. Schematic representation of chemical modification of bamboo fibres [9].
4. Recycling and biodegradability of NFRCs
One of the main reasons for the popularity of NFRCs is their
biodegradable nature. Scientists and engineers have always been
looking for composites that are stable during their service but
can be easily degraded in appropriate conditions. Natural fillers
that are hydrophilic and more biodegradable increase the adhesion
of microorganisms to the composite material and facilitate degra-
dation. Cellulose-based natural fibres which form the bulk of the
NFRCs are highly hygroscopic and come under bacterial attack
[13]. However, this feature also makes them susceptible to degra-
dation during their service, hence the fraction of polymer matrix
and degradable reinforcements should be carefully tuned. The
large surface area at the matrix–reinforcement interface represents
a zone of weakness that can restrict the use in some applications
since the interface can act as an access site for degrading agents,
but it also acts as a pathway for their eventual degradation [14].
In another similar study [15], Polypropylene (PP) and Polyethylene
(PE) which are extensively used in commercial and household
activities were manufactured with saw-dust and wheat-flour fibres
as reinforcements. The biodegradability was found to improve
remarkably under conditions of microbial attack and chlorinated
environment. Such development also hints at developing special-
ized treatment plants and composting grounds with suitable
degrading environments, where degradation of these composites
can take place.
5. Conclusion
In the coming years as the world seeks its redemption from
environmental degradation, we are bound to look for natural mate-
rials for engineering use. In an energy-hungry and resource-
depleted world manufacturing techniques such as additive manu-
facturing is bound to change the manufacturing landscape. We can
assume that natural fibre reinforced composites are a potential
candidate for next-generation materials. Research labs all over
the world have already started prototyping these materials for
their extensive testing. The excellent biocompatibility, biodegrad-
ability, mechanical properties, thermal properties, and surface
properties are some of the reasons that today’s additive manufac-
turing is adopting this at a larger scale for the production of func-
tional and structural composites in engineering and medical fields.
4
Materials Today: Proceedings xxx (xxxx) xxx
The animal fibre by the biomedical engineering fields where the
preparation of biomedical scaffolds can be performed by the rein-
forcement of the animal fibres in biodegradable thermoplastics.
However, more scientific insights need to be collected with the
adoption of suitable standards for testing, service parameters and
degradation of such composites. Systematic research and planning
for setting up treatment and composting facilities for degradation
and reuse of NFRCs need to be put in place.
Declaration of Competing Interest
The authors declare that they have no known competing finan-
cial interests or personal relationships that could have appeared
to influence the work reported in this paper.
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