Sustainability 15 16171

sustainability
Review
Natural Fiber Composite Filaments for Additive Manufacturing:
A Comprehensive Review
Irshad Ahamad Khilji 1 , Chaitanya Reddy Chilakamarry 2 , Athira Nair Surendran 1,3 , Kunal Kate 3
and Jagannadh Satyavolu 1, *
1 Conn Center for Renewable Energy Research, University of Louisville, Louisville, KY 40292, USA;
irshad.khilji@louisville.edu (I.A.K.); athiranair.surendran@louisville.edu (A.N.S.)
2 Bioproducts LLC, Louisville, KY 40206, USA; c_chilakamarry@bioproductsllc.com
3 Materials Innovation Guild, Department of Mechanical Engineering, University of Louisville,
Louisville, KY 40208, USA
* Correspondence: jagannadh.satyavolu@louisville.edu
Abstract: This research explores the potential and significance of 3D printing natural fiber composite
(NFC) materials. The primary objective is to investigate the mechanical, thermal, and environmental
properties of NFC filaments, mainly focusing on biodegradable, renewable fibers such as jute, hemp,
flax, and kenaf. In addition to studying the properties of NFCs, our research delves into the challenges
associated with processing, including moisture absorption and fiber-matrix interfacial bonding. The
novelty of this work lies in the convergence of traditional composite materials with the versatility of
3D printing technology. NFC filaments offer unique advantages in terms of sustainability, and we
examine their potential contributions to the circular economy. By using eco-friendly NFC materials
in 3D printing, we aim to present a viable, environmentally responsible alternative to conventional
synthetic composites. The importance of 3D printing NFCs stems from the ways their use can align
with sustainability goals. These materials provide the advantages of renewability, reduced carbon
impact, and in some cases, biodegradability. Their applications extend to various industries, such
as automotive, construction, and packaging, where eco-friendly materials are increasingly sought.
Such applications showcase the ways in which NFC-based 3D printing can contribute to a more
Citation: Khilji, I.A.; Chilakamarry,
environmentally responsible and sustainable future. This research explores the mechanical, thermal,
C.R.; Surendran, A.N.; Kate, K.;
and environmental properties of NFC materials, highlighting their unique advantages for 3D printing
Satyavolu, J. Natural Fiber
and the potential to have eco-friendly applications in diverse industries.
Composite Filaments for Additive
Manufacturing: A Comprehensive
Review. Sustainability 2023, 15, 16171.
Keywords: natural fiber composite; additive manufacturing; biodegradability; sustainability; hybrid
https://doi.org/10.3390/ composites
su152316171
Academic Editors: Andrzej Pacana

and Dominika Siwiec
1. Introduction
Received: 18 October 2023 A major paradigm shift in additive manufacturing occurred recently, leading to a focus
Revised: 15 November 2023 on discovering and applying novel materials to expand three-dimensional (3D) printing
Accepted: 16 November 2023 techniques [1]. Natural fiber composite filaments have received considerable interest among
Published: 21 November 2023
these emerging materials due to their unique mechanical properties, eco-friendliness, and
renewable nature [2]. One of the most fascinating developments is the use of natural
fiber composite filaments in AM techniques. This novel approach combines the benefits
Copyright: © 2023 by the authors.
of naturally occurring, sustainable fibers with the adaptability and precision of additive
Licensee MDPI, Basel, Switzerland. manufacturing techniques [3]. Fused deposition modeling (FDM) is becoming popular for
This article is an open access article developing intricate structures using biodegradable polymer composite materials in various
distributed under the terms and industries, including medicine, automotive, sensors, and pharmaceuticals. This approach
conditions of the Creative Commons is known as fused filament fabrication (FFF) [4]. Various additive manufacturing (AM)
Attribution (CC BY) license (https:// techniques have also been used to create prototypes. Due to its low cost, user-friendliness,
creativecommons.org/licenses/by/ and streamlined control, which requires minimal human input and understanding of the
4.0/). process, FFF offers a compelling advantage. Polymers are the primary raw material for
Sustainability 2023, 15, 16171. https://doi.org/10.3390/su152316171 https://www.mdpi.com/journal/sustainability

Sustainability 2023, 15, x FOR PEER REVIEW 2
Sustainability 2023, 15, 16171 2 of 30
understanding of the process, FFF offers a compelling advantage. Polymers are the
mary raw material for FFF, and the finished products are produced sequentially u
FFF, and the finished products are produced sequentially under the direction of G-code
the direction of G-code instructions derived from CAD data [5]. Famous thermopl
instructions derived from CAD data [5]. Famous thermoplastic polymers like acrylonitrile
polymers like acrylonitrile butadiene styrene (ABS), polylactic acid/polylactide (P
butadiene styrene (ABS), polylactic acid/polylactide (PLA), polypropylene (PP), nylon,
polypropylene (PP), nylon, polyamide, and polycarbonate (PC) are extensively
polyamide, and polycarbonate (PC) are extensively used within this framework [6]. Materi-
within this framework [6]. Materials are typically used in the automotive, electrical, m
als are typically used in the automotive, electrical, medical, and architectural industries
ical, and architectural industries based on their inherent strength and processability
based on their inherent strength and processability [7].
While FFF first found applications in manufacturing prototypes with low stres
While FFF first found applications in manufacturing prototypes with low stress re-
quirements, its value is now seen in a more extensive range of applications, includin
quirements, its value is now seen in a more extensive range of applications, including in
toys for
toys for the home [8].the
Thehome [8]. The
creation creation of
of composite composite
filaments from filaments
naturalfrom
fibersnatural fibers like he
like hemp,
flax, and bamboo has advanced significantly as a result
flax, and bamboo has advanced significantly as a result of recent research efforts [9]. These of recent research efforts [9]. T
filaments have improved mechanical qualities, lower environmental impact, and a more and a m
filaments have improved mechanical qualities, lower environmental impact,
comprehensive comprehensive range of [10].
range of applications applications [10]. Investigations
Investigations of natural fiber of natural
compositesfiberascomposites
a
viable alternative to typical polymer-based filaments have gained traction as the globalas the gl
viable alternative to typical polymer-based filaments have gained traction
emphasis on emphasis
eco-friendly on solutions
eco-friendlyandsolutions
reducingand the reducing the carbon
carbon footprint footprint of manufactu
of manufacturing
has grown [11]. The employment of natural fiber
has grown [11]. The employment of natural fiber composite filaments in AM processes composite filaments in AMis process
one of the most exciting advances in this field [12]. This innovative method combines thecombine
one of the most exciting advances in this field [12]. This innovative method
advantages ofadvantages
renewable of andrenewable andnatural
sustainable sustainable
fibersnatural
with the fibers with the and
adaptability adaptability
accuracyand accu
of additive manufacturing processes [13]. The creation of composite filaments fromfilaments
of additive manufacturing processes [13]. The creation of composite natural from n
ral fibers
fibers has advanced has advanced
significantly as a significantly
result of recent as research
a result of recent
efforts research
[14]. These efforts
filaments[14]. These
have improved ments have improved
mechanical qualities,mechanical qualities, lower
lower environmental impact, environmental impact,
and a wider range of and a w
range
applications [9]. of applications
Investigations [9]. Investigations
of natural fiber composites of natural fiber composites
as a viable alternative toastypical
a viable alterna
polymer-based to filaments
typical polymer-based filaments
have gained traction. have gained
Combining traction.
insights fromCombining insights from m
materials science,
rials science, mechanical engineering, and additive
mechanical engineering, and additive manufacturing technologies, this research aims to manufacturing technologies, thi
comprehensively search aimsthis
assess to comprehensively
developing field’sassess this developing
accomplishments, field’s accomplishments,
obstacles, and future pos- obsta
sibilities. Thisand future
review possibilities.
aims to shed lightThisonreview aimsof
the history tonatural
shed light oncomposite
fiber the history of natural fiber c
filaments
by examiningposite filaments
the current by examining
literature and criticallythe current
evaluatingliterature and critically
experimental evaluating
findings, therebyexperime
adding to thefindings, therebydebate
more significant addingon tosustainable
the more significant debate on sustainable
additive manufacturing materialsadditive
and manu
processes. In turing
addition, materials
this workandcontributes
processes. In addition,
to the evolvingthisfield
work ofcontributes to the evolving fie
additive manufactur-
ing by analyzing the synthesis,
additive manufacturingprocessing techniques,
by analyzing theand wide range
synthesis, of applications
processing of and w
techniques,
natural fiber composite filaments (Figure
range of applications of natural1). fiber composite filaments (Figure 1).
Figure 1. Additive
FigureManufacturing Process.
1. Additive Manufacturing Process.
1.1. Natural Fiber-Reinforced Polymer Composites (NFRPC)
1.1. Natural Fiber-Reinforced Polymer Composites (NFRPC)
Researchers are exploring the use of NFRPCs to bridge the gap between sustainability
Researchers are exploring the use of NFRPCs to bridge the gap between sustain
and material performance. Fiber-reinforced polymer (FRP) was initially introduced by
ity and material performance. Fiber-reinforced polymer (FRP) was initially introduce
Owens Corning in 1935, with the first iteration using glass fiber [15]. Composites are
Owens Corning in 1935, with the first iteration using glass fiber [15]. Composites
becoming increasingly important, and their use is expanding in many areas of modern life.
Eco-friendly, lightweight, robust, renewable, inexpensive, biodegradable, and sustainable
composite materials can be made from natural fibers [15]. Compared to traditional synthetic
fibers, natural fibers are preferable due to their superior mechanical characteristics. Thus,
natural fibers have recently attracted the attention of many researchers and scientists for
usage as an alternative reinforcement in polymer composites [16]. They are affordable,
recyclable, renewable, use less energy, pose fewer health risks, are not abrasive to machinery,
and do not irritate the skin. They have thermoplastic and thermosetting properties and
can be employed as a reinforced material. Several thermosetting resins are commonly
employed in composite materials, including epoxy, unsaturated polyester resins, polyester,
polyurethane, and phenolic resins [17]. They have acceptable mechanical characteristics and
are reasonably priced. Natural fibers are gaining increased consideration from academics
and industrial users because they are extremely strong and lightweight as well as being
much more environmentally friendly than regular composites. Natural composites are
being used ever more frequently because they are biodegradable and non-carcinogenic [18].
Ensuring efficient bonding at the fiber-matrix interface is a critical difficulty with
NFRPCs. Recent research has concentrated on fiber-surface treatments that encourage
adhesion. Alkali treatments have been used to improve interfacial bonding by remov-
ing impurities and roughening the surface of fibers. Natural fibers can absorb moisture
and cause composite materials to degrade because they are intrinsically hydrophilic [19].
Hydrophobic coatings and the incorporation of desiccants into the matrix are now being
researched as potential solutions to this problem.
Natural fiber is a relatively economical material that is used in various industries
and applications, including packaging, automotive, building and construction, covering
the interiors of railway coaches, and warehouses. It is also used to replace expensive
glass fiber in various industries. The poor mechanical properties of NFRCs are one of
their drawbacks [20]. The hybridization process is one way to improve the mechanical
performance of NFRCs and broaden their applications. The water-absorption rates for
hemp/flax/epoxy, hemp/jute/flax/epoxy, and hemp/jute/epoxy blends are affected by
the hybridization process, which alters the behavior of hybrid composites. These rates
are 2.8 percent, 3 percent, and 4.5 percent, respectively, when hybridization is done by bi-
directional weaving and hand layup compression [20]. The water-absorption rate of the flax-
fiber composites was discovered to be 12 times higher than that of the glass-fiber composites
via vacuum-assisted resin infusion. The increased moisture absorption of natural fibers
is the main drawback of these materials. Therefore, chemical treatments must mitigate
excessive moisture absorption [21]. Many parameters, including fiber length, fiber aspect
ratio, fiber-matrix adhesion, etc., significantly affect the mechanical properties of natural
fibers after chemical treatment [9]. Through chemical modification using alkaline treatment,
silane treatment, acetylation treatment, benzoylation treatment, and peroxide treatment,
the matrix’s adherence to NFRC is improved and its hydrophilicity is lowered [22].
1.2. Properties of Natural Fibers

Fiber diameter, fiber length, and cell-wall thickness are three crucial characteristics
of natural fibers. Because of the wide variety in fiber diameters (5–76 µm), fiber bundle
widths (10–1000 µm), and fiber lengths, the properties of polymer composites made with
natural fibers can vary greatly (1.2–300 mm) [23]. Optimizing production processes wherein
natural fibers are used as reinforcement is difficult due to the inherent variances in natural
fibers. Thus, accurate assessment and management of feedstock material is critical to
obtaining the desired results from NFRCs. Cellulose, a natural polymer composed of
three repeating hydroxyl groups, is one of the NFRC’s components [24]. Plants typically
store cellulose as a linear, ribbon-shaped polymer of glucose. Chemical and solution
treatments can degrade cellulose, despite the material’s resistance to hydrolysis, strong
alkalis, and oxidants. Hemicelluloses, which are low-molecular-weight polysaccharides, act
as a matrix for the bonds between cellulose microfibrils, which are the basic constituents of
NFRC cells. Hemicelluloses hydrolyze efficiently in the presence of weak acids because of
their hydrophilicity. A complex hydrocarbon polymer called lignin gives NFRCs strength,
rally polar and hydrophilic due to their abundance of hydroxyl groups. However, most
polymer matrixes are hydrophobic by nature [25].
The properties of the natural fibers that influence those of NFRCs are physical, chem-
ical, geometrical, thermal, and mechanical, as shown in Figure 2. Mechanical properties
Sustainability 2023, 15, 16171 of natural fibers are directly influenced by structural and dimensional changes, 4 ofsuch
30 as
changes in fiber density (cell wall-lumen ratio) and microfibril angle (MFA). Synthetic fi-
bers like E-glass fiber have a tensile strength of about 2000–3500 MPa. These natural fibers,
however, have
facilitates a wide
water range
transport, of resists
and tensilemost
strengths andattacks.
microbial Young’s It ismoduli, with ahydrolyzes
hydrophobic, typical tensile
in concentrated
strength betweenhydrochloric
100 and 1000 acid,
MPa and is easily oxidized. Pectin is a heteropolysaccharide
[26].
that
Thegive flexibility toperformance
mechanical plant cell wallsof and is used as thickener.
a hand-layup NFRCs are
kenaf/polyester naturallywas
composite polarexam-
and hydrophilic due to their abundance of hydroxyl groups. However,
ined by Mohammed et al. to elucidate the effects of layering NFRCs [25]. The influence of most polymer
matrixes are hydrophobic by nature [25].
the variable fiber-volume fraction (5–25%) on the mechanical specifications of kenaf/pol-
The properties of the natural fibers that influence those of NFRCs are physical, chem-
yester
ical, geometrical, was
composites studied
thermal, by Husseinas
and mechanical, etshown
al. Their findings
in Figure demonstrated
2. Mechanical that as the
properties
fiber volumefibers
of natural reached 10%, tensile
are directly strength
influenced increasedand
by structural [27]. In contrastchanges,
dimensional to composites
such as with-
outchanges
filler, Jenish et al. studied Cissus quadrangularis stem fiber /epoxy resin
in fiber density (cell wall-lumen ratio) and microfibril angle (MFA). Synthetic fiberswith various
concentrations
like E-glass fiberof coconut-shell
have a tensile ash powder.
strength The2000–3500
of about tensile and MPa.flexural
Thesestrength values for
natural fibers,
however,
Cissus have a wide range
quadrangularis stem of tensile
fiber stem strengths and Young’s
fiber/epoxy moduli,
composite with
with a typical
five tensile coco-
wt. percent
strengthash
nut-shell between 100 and 1000inferred
particulate-were MPa [26].to be 110.31 and 136.11 MPa, respectively [28].
Figure 2. Significance
Figure 2. SignificanceofofDistinctive PropertiesofofNatural
Distinctive Properties Natural Fibers
Fibers for for NFRCs
NFRCs.
The mechanical
1.3. Advantages performance
and Challenges of aNatural
of Using hand-layup
Fiberskenaf/polyester
in Composites composite was ex-
amined by Mohammed et al. to elucidate the effects of layering NFRCs [25]. The in-
Material and product development relies heavily on considerations like biodegrada-
fluence of the variable fiber-volume fraction (5–25%) on the mechanical specifications of
bility and recyclability.
kenaf/polyester The was
composites advantages
studied byofHussein
naturaletfibers over
al. Their synthetic
findings fibers inthat
demonstrated terms of
technology,
as the fibereconomy, and ecology
volume reached are displayed
10%, tensile in Figure
strength increased 3. Carbon
[27]. and
In contrast to glass fibers, two
composites
common
withouttypes
filler, of synthetic
Jenish fibers used
et al. studied as quadrangularis
Cissus reinforcement,stemhavefiber
the central
/epoxy problem
resin withof not
being biodegradable
various concentrations orofrecyclable when
coconut-shell ashthey endThe
powder. their useful
tensile andlives. Their
flexural processing
strength values also
for Cissus quadrangularis stem fiber stem fiber/epoxy composite with five
carries risks of harm to human health [29]. The focus of scientific inquiry has recently wt. percent
coconut-shell
shifted ash particulate-were
from single-component inferredtotocomposites
materials be 110.31 and 136.11 MPa,
reinforced respectively
with [28]. The
natural fibers.
fact1.3.
that plant fibers
Advantages do not increase
and Challenges of Usinggreenhouse
Natural Fibersgas emissions is remarkable. It is widely
in Composites
Material and product development relies heavily on considerations like biodegrad-
ability and recyclability. The advantages of natural fibers over synthetic fibers in terms
of technology, economy, and ecology are displayed in Figure 3. Carbon and glass fibers,
two common types of synthetic fibers used as reinforcement, have the central problem
of not being biodegradable or recyclable when they end their useful lives. Their process-
ing also carries risks of harm to human health [29]. The focus of scientific inquiry has
recently shifted from single-component materials to composites reinforced with natural
fibers. The fact that plant fibers do not increase greenhouse gas emissions is remarkable. It
is widely believed that carbon dioxide (CO2 ) emissions from burning materials made from
lus values include curauá, sisal, and ramie. However, many factors, including those envi-
ronmental and processing circumstances already mentioned, can affect their behavior,
[31]. One such aspect is the large variability in fiber quality, which leads to high variation
in material properties. Therefore, more research on these characteristics is required with
Sustainability 2023, 15, 16171 respect to methods of fiber preservation. Another critical factor is that it is difficult 5 ofto
30 com-
pare the results of different investigations due to the absence of specific information re-
garding experimental testing methodologies for single fibers. Tensile strength is calcu-
petroleum-based
lated products
using the entire are the primary
cross-section cause of the
of the sample, andgreenhouse effect
even a small and, consequently,
measurement error can
of climate change [30].
have a significant impact on the results [32].
Figure 3. Advantages
Figure 3. AdvantagesofofUsing
UsingNatural FibersininComposites.
Natural Fibers Composites.
MoreFiber
1.4. Natural cellulose-rich
Types fibers with higher tensile strength and values for Young’s modulus
values include curauá, sisal, and ramie. However, many factors, including those environ-
Natural fibers are fibers that are free of dyes, artificial additives and synthetics. Plants
mental and processing circumstances already mentioned, can affect their behavior [31]. One
andsuch
animals
aspectboth
is theproduce naturalinfibers.
large variability Natural
fiber quality, fibers
which come
leads from
to high both renewable
variation in material and
nonrenewable resources.more
properties. Therefore, Natural fibers
research on are hair-like
these raw materials
characteristics derived
is required directly
with respect to from
vegetables, plants, animals, or minerals. These raw materials are converted
methods of fiber preservation. Another critical factor is that it is difficult to compare theinto nonwo-
venresults
fabrics
of and usedinvestigations
different as compositedue components.
to the absenceTheofclassification of natural
specific information fibers into
regarding
experimental
plant, animal, and testing methodologies
mineral for singlein
fibers is depicted fibers.
Figure Tensile strength
4. The primaryis calculated
difference using
between
the entire cross-section of the sample, and even a small measurement error
animal and plant fibers is that animal fibers are composed primarily of protein, whereas can have a
significant impact on the results
plant fibers are promarily cellulose. [32].
Plant
1.4. fibers:
Natural FiberPlant
Typesfibers consist primarily of cellulose fibers. Plant fibers are divided
into primary and secondary fibers, depending on their purpose. The fibers of primary
Natural fibers are fibers that are free of dyes, artificial additives and synthetics. Plants
plants
and are usedboth
animals to cultivate secondary
produce natural plants.
fibers. NaturalThese fibers
fibers comecanfrom beboth
further categorized
renewable and as
seed fiber (fibers from the seed and seed case, e.g., cotton and kapok),
nonrenewable resources. Natural fibers are hair-like raw materials derived directly from leaf fiber (leaves,
e.g.,vegetables,
agave, abaca,
plants,henequen,
animals, or pineapple fiber,raw
minerals. These and sisal), skin
materials fiber (the
are converted skin
into or bast that
nonwoven
surrounds
fabrics andtheused
stemas of a plant components.
composite (e.g., flax, ramie, jute, banana,
The classification hemp,fibers
of natural kenaf,intorattan,
plant, vine
animal, and mineral fibers is depicted in Figure 4. The primary difference between
fibers, soybean fiber, and banana fibers), and fruit fiber (coconut (coir) fiber) [33]. Fibers animal
fromandstalks,
plant fibers
cane, is that animal
grass, and reedsfibersare
arefrom
composed primarily
original naturalof sources
protein, (e.g.,
whereas plant ba-
bamboo,
fibers are promarily cellulose.
gasse, sabai, communis, and phragmites).
Plant fibers: Plant fibers consist primarily of cellulose fibers. Plant fibers are divided
Animal fibers: Animal fibers are derived from wool, silk, hair/fur, alpaca fiber, and
into primary and secondary fibers, depending on their purpose. The fibers of primary
avian fiber.
plants are used to cultivate secondary plants. These fibers can be further categorized as
Mineral
seed fibers:from
fiber (fibers Mineral fibers
the seed andcan
seedbecase,
found orcotton
e.g., modified minimally
and kapok), leaf to become
fiber (leaves,asbes-
tos,e.g.,
ceramic
agave,fiber,
abaca,orhenequen,
metal fiber. pineapple fiber, and sisal), skin fiber (the skin or bast that
surrounds the stem of a plant (e.g., flax, ramie, jute, banana, hemp, kenaf, rattan, vine
fibers, soybean fiber, and banana fibers), and fruit fiber (coconut (coir) fiber) [33]. Fibers
from stalks, cane, grass, and reeds are from original natural sources (e.g., bamboo, bagasse,
sabai, communis, and phragmites).
Animal fibers: Animal fibers are derived from wool, silk, hair/fur, alpaca fiber, and
avian fiber.
Sustainability 2023, 15, x FOR PEER REVIEW

Mineral 6 of 31
fibers: Mineral fibers can be found or modified minimally to become asbestos,
ceramic fiber, or metal fiber.
Figure4.4.Classification
Figure Classificationof
ofnatural
naturalfibers.
fibers.
The
Thetrajectory
trajectoryofofNFRPC
NFRPCresearch is is
research shifting from
shifting basic
from understanding
basic to optimization
understanding to optimiza-
and application. As methodologies to enhance interface adhesion and reduce
tion and application. As methodologies to enhance interface adhesion and reduce moisture
mois-
sensitivity mature, NFRPCs are poised to become a mainstay in sustainable materials.
ture sensitivity mature, NFRPCs are poised to become a mainstay in sustainable materials.
2. Additive Technologies for Natural Fiber Composites
2. Additive Technologies for Natural Fiber Composites
2.1. Polymer-Based Fused Deposition Modeling (FDM)
2.1. Polymer-Based Fused Deposition Modeling (FDM)
Fused deposition modeling is an additive manufacturing technique that utilizes com-
Fused deposition
pact desktop-sized modeling
machines to is an additive
produce rapidmanufacturing
prototyped 3D technique
printed that utilizes com-
structures. This
process uses polymer filaments heated to a molten state and extruded through aThis
pact desktop-sized machines to produce rapid prototyped 3D printed structures. nozzlepro-
cess uses ranging
typically polymerin filaments
size from heated
0.2 mm to ato molten
1.0 mm state
and and extruded
made through
of brass. a nozzle
First, a model typi-
is
cally ranging
designed on a CADin sizesoftware
from 0.224.2.mmNext, to 1.0the mm 3Dand made
printer of brass.slices
software First,the
a model
3D model is designed
into 2D
on a CAD
layers stackedsoftware
on top24.2.
of eachNext, the making
other, 3D printer software slices
a layer-by-layer the(G-code),
code 3D modelwhich into 2D layers
supplies
stacked on top of each other, making a layer-by-layer code
the instructions to the printer head to control all of the printing parameters. The slicer (G-code), which supplies the
instructions to the printer head to control all of the printing
supports the 3D model if any structures are overhanging or unstable. A spool of polymer parameters. The slicer sup-
ports the typically
filaments 3D modelmade if any structures
from polylactic areacid
overhanging or unstable.
(PLA) is loaded onto theA spool of polymer
3D printer, and
filaments
the filament typically
is loaded made from polylactic
between two gearsacid that(PLA)
guide is the
loaded onto the
filament from3Dtheprinter,
spooland the
to the
filamenthead.
extruder is loadedThere, between two gears
the filament is heated thattoguide the state
a molten filament
and from
extrudedthe from
spoolthe to nozzle.
the ex-
truder
The head. There,
extruder and heaterthe filament is heated
are attached to an to axis
a molten state and
that moves in extruded
the x, y and from the nozzle.
z directions,
The extruder and heater are attached to an axis
facilitating material deposition in complex shapes and structures [34]. that moves in the x, y and z directions,
facilitating
There are material
printingdeposition
parameters in complex
to consider shapes
when and structures
designing a 3D[34].
printing model. The
most There
criticalare printing parameters
parameters are print speed, to consider when designing
print temperature, a 3D printing
and layer height. Printmodel. The
speed
ismost
the critical
speed at parameters
which theare printdeposits
printer speed, print temperature,
material onto theand build layer height.
plate and is Print speed
typically
is the speed
measured at which
in mm/s. Printthetemperature
printer deposits material ontoatthe
is the temperature whichbuildtheplate andisisextruded,
filament typically
and layer height
measured in mm/s. is the
Printthickness of each
temperature is layer of the part.atThe
the temperature speed
which theand temperature
filament is extruded, can
be different for the first layer than
and layer height is the thickness of each layer for the rest of the printed part because good
part. The speed and temperature can adhesion
between
be different the first layer
for the andlayer
first the build
than for platethe needs
rest toof be
theestablished
printed part forbecause
a good-quality printed
good adhesion
part.
betweenThe manufacturer
the first layergives and athe print
build temperature
plate needs for to
thebefilaments,
established but this
for avalue can also
good-quality
be obtained
printed part.from
Thethermal-stability
manufacturer gives analysis.
a print Thetemperature
optimal layer forheight depends but
the filaments, on the thisnozzle
value
diameter;
can also bea obtained
good layer fromthickness is about 50–60%
thermal-stability analysis.of The
the nozzle
optimaldiameter.
layer height Thisdepends
thickness on
facilitates proper adhesion between the layers to maintain the
the nozzle diameter; a good layer thickness is about 50–60% of the nozzle diameter. This properties of the printed part.
Optimal
thicknessprocess conditions
facilitates proper can be obtained
adhesion between by the
analyzing
layers to themaintain
properties theofproperties
the filaments. of the
printed part. Optimal process conditions can be obtained by analyzing the properties of
the filaments.
Other than the abovementioned parameters, other physical parameters of each layer
affect the characteristics and properties of printed parts: air gap, perimeter, and raster.
Other than the abovementioned parameters, other physical parameters of each layer
affect the characteristics and properties of printed parts: air gap, perimeter, and raster. The
air gap is the distance between a raft, a support that can be printed as the base for a part,
and the bottom of the model. Raster width is the width of a single line of material deposited,
and raster angle is the angle at which the infill is printed [35]. The number of perimeters
and thickness of the perimeter also make a difference in the print quality of the end product.
Gebisa et al. studied the effect of printing parameters on the tensile properties of high-
performance ULTEM 9085 using complete factorial design of experiments and found that
the raster or infill angle has the greatest effect on tensile strength and strain [8]. Sanatgar
et al. investigated the effects of print temperature, print speed, and build-plate temperature
on the adhesion properties of polymers (PLA, nylon, PA66) and nanocomposites (carbon
nanotubes and PLA: CNT/PLA; carbon black and PLA: CB/PLA) in textiles [36]. Build-
plate temperature had little effect on the adhesion properties when it was lower than the
glass-transition temperature. Linear and quadratic correlations were found between print
temperature and print speed, respectively, and adhesion properties. Wang et al. studied
the process parameters of printing glass fiber (GF) and carbon fiber (CF) composite with
polyetheretherketone (PEEK) [37]. Print temperature, build-plate temperature, print speed,
and layer height were investigated and related to mechanical and microstructural properties
of the GF/PEEK and CF/PEEK. The ideal layer height and print speed for composites were
1 mm and 5 mm/s, and all mechanical parameters of the composites decreased as print
speed and layer height increased. Tensile and flexural strength increased at higher print
and build-plate temperatures, but these two factors had no effect on impact strength.
Materials Compatibility and Natural Fiber Composites in FDM

The limitation of FDM is the need for a thermoplastic polymer to be used in the 3D
printing process. The raw materials needed for FDM printers are filaments that must be
molten. This can be a challenge for 3D printing of natural fiber composite because natural
fiber decomposes at a lower temperature compared to thermoplastic polymers, making the
composite challenging to manufacture. Examples of thermoplastic polymers typically used
in the FDM technique are polylactic acid (PLA), acrylonitrile butadiene styrene (ABS),
polyamide (PA)/nylon, polyethylene terephthalate glycol (PETG), and elastomers. PLA is a
biodegradable polymer typically made from fermented plant-based starch that breaks down
into lactic acid over time, making it a safe and cost-effective choice for 3D printing filaments.
However, PLA’s degradability and poor mechanical strength makes it a poor choice for 3D
printing structures that need to withstand high temperatures or force. ABS, by contrast,
exhibits good thermal stability, making it a good filament with which to print functional
parts, but it produces styrene gas when subjected to high print temperatures. Similarly, PA
is also typically used to print functional parts because of its excellent mechanical properties
and thermal stability. PETG is one of the best materials for printing because of its superior
chemical, mechanical and heat stability, but it is typically more expensive than other 3D-
printing filaments. Thermoplastic polyurethane, copolyester and elastomers are elastic
filaments used for printing parts that require high impact resistance, but the elastic nature
of these filaments make them challenging to control and feed into the nozzle. Other than
that, complex overhanging structures are not suitable for manufacture with elastic filaments
and require support structures.
Findings in the literature have shown that natural fibers improve the properties of
some of the abovementioned polymers. Kamarudin et al. investigated the properties of
up to 5 wt.% alkali-pretreated kenaf fiber in a PLA matrix with the addition of epoxidized
jatropha oil as a plasticizer [38]. There was a slight increase in flexural strength and up
to a tenfold increase in impact strength for treated kenaf-fiber composites. Adding the
plasticizer decreased water absorption and retention, and it was concluded that the fiber
pretreatment improved fiber-polymer adhesion. Agaliotis et al. studied the tensile proper-
ties of 3D-printed PLA-henequen fiber-flour composites and showed similar mechanical
properties with the addition of 1% fiber flour [39]. However, there is an increase in ultimate
tensile strength and strain in specimens with maleic anhydride. Duigou et al. reported a
study of using continuous flax fiber coated with PLA for 3D printing, which is a different
approach compared to mixing short-natural-fiber composites using high torque and tem-
perature [40]. These biocomposites contained 35 wt.% flax fiber and exhibited significantly
higher tensile strength and modulus compared to short-fiber printed composites. Ahmad
et al. developed ABS-oil palm-fiber composite filaments in which 5 wt.% of natural fiber
was added to the composite mixture [41]. The values of Young’s modulus and tensile
strength for the composite printed parts increased at the expense of flexural strength, which
is acceptable because of the higher stiffness of fiber-reinforced composites. There is little
literature on composites of nylon and natural fibers because of the high thermal stability of
nylon, which makes it incompatible with natural fibers, which have much lower thermal
stability. However, extensive research has been done to examine composites of carbon or
glass fiber and nylon [42–45]. The mechanical properties increase significantly with the
addition of carbon fiber to nylon. Balla et al. 3D printed up to 35 wt.% of soybean-hull
fiber mixed with TPC to test the mechanical properties and water uptake of the resulting
material [14,46]. They discovered that sulfuric-acid pretreatment increased the mechanical
properties of soy-hull-reinforced 3D-printed composites and that water uptake is lower at
lower percentages of natural fibers. Zhou et al. studied high loading of lignin in TPU for 3D
printing composites and found that the mechanical properties peak at 50 wt.% lignin [47].
They further investigated the addition of carbon fiber and showed a 67% improvement
in tensile strength, which is more than the tensile strength exhibited by a composite with
20 wt.% kenaf fiber.
2.2. Resin Based Stereolithography (SLA)

2.2.1. Photopolymerization Mechanisms
Stereolithography is a rapid prototyping method wherein an ultraviolet (UV) spectrum
light source is used to cure photosensitive polymeric resin to produce 3D-printed structures.
The resin contains photo initiators that undergo a chemical reaction when exposed to UV
light and bond monomers and oligomers into a polymer. SLA printers are designed as
upside-down printers, where the build plate moves vertically into a vat of photosensitive
resin and the bottom of the vat is clear. There is a small distance between the build plate
and the bottom of the resin-filled vat, and the material is cured by the UV light from under
the vat. When a layer is finished, the build plate moves up by the height of a layer to allow
liquid resin to go between the bottom of the vat and the top of the previous layer. After
printing, the part is post-processed by further UV curing under visible light or under UV
light for a faster curing time.
The printing parameters to consider that affect dimensional accuracy in SLA printing
are layer height, exposure time, build angle, and support density. Badanova studied the
effects of SLA-printing parameters on castable wax and found that build angle plays the
most important role in dimensional accuracy. A zero-degree build angle and a 0.25 µm
layer height were optimal for castable wax [48]. The effects of post-curing processes used
with SLA, namely, treatment in a microwave, conventional oven, and UV chamber, on the
mechanical properties of printed parts were studied. The parameters investigated were
build angle, solidification factor, and curing time. The microwave and UV post-curing was
found to lead to an increase in mechanical strength, while the heat from the conventional
oven led to overcuring and a decrease in strength [49]. A study on the effects of UV
SLA in increasing solids loading and the printability of ceramics was performed wherein
combinations of dispersant, photo initiator, plasticizer, monomer, and alumina powder
were prepared with varying loading of alumina powder. With this method, the highest
flexural strength was found at 52 vol.% solids loading. Sintered part density increased
while shrinkage decreased with increasing solids loading. Rheological results showed a
significant increase in viscosity with increasing solids loading [50]. Hu investigated the
3D printing of Mn-Zn ferrite ceramics using an SLA technique wherein the layer height,
print speed and laser power were varied. They concluded that the optimal parameters to
print Mn-Zn ferrite ceramic parts were 2 µm layer height, 2500 mm/s print speed, and
laser power of 240 mW. These paramets produced the best dimensional accuracy and the
least shrinkage [51].
2.2.2. Formulation of Photopolymerizable Resin with Natural Fibers

Although SLA is the oldest form of 3D printing, research around natural fiber compos-
ites based on SLA is limited, possibly due to the poor compatibility and bonding between
thermoset resins and natural fibers. Another reason could be that natural fiber may hinder
or slow the photopolymerization process by blocking the UV light from reacting with the
polymer matrix. SLA printing is normally used for printing parts with a smooth finish and
rarely exhibits good chemical or mechanical properties for most applications. However,
researchers have been trying to add other substances to the mixture of photopolymer and
natural fibers to help with bonding and curing. Palaganas extracted cellulose nanocrys-
tals (CNCs) from hydrolyzed abaca-pulp fibers and mixed up to 1.2 wt.% of CNCs with
polyethylene glycol diacrylate (PEGDA) and a photo initiator to create a hydrogel pre-
cursor. There were no significant differences in elastic modulus at different CNC loading
wt.%, but adding 0.3 wt.% CNC loading resulted in a 100% increase in tensile strength,
110% increase in elongation and 300% improvement in fracture energy. Adding 1.2 wt.%
loading of CNC increased the tensile strength, elongation, and fracture energy by 33%,
40%, and 100%, respectively. This study provides a potential formula for a biocompati-
ble 3D-printed CNC resin that can be used in tissue engineering. Using lignocellulosic
natural fibers [52]. Romero-Ocana tested 5 wt.% loading of wheat-straw and rice-straw
composites with photosensitive resin for SLA 3D printing. The fibers were milled and
sifted to <45 µm, <125 µm and <250 µm to investigate the effects of particle size of the
two cereal straws on mechanical properties. Both straw composites with <45 µm fibers
showed higher elastic modulus compared to clean resin. Tensile strength and elongation
decreased significantly for all composites with straw fiber added [53]. Feng studied the SLA
printing of lignin-coated CNCs mixed with methacrylate resin and the effect of loading
0.1, 0.5 and 1 wt.% CNCs on the thermal and mechanical properties of the composite.
Loading of lignin (1 wt.%) CNCs resulted in the worst performance in terms of mechanical
and thermal properties. CNC-loaded (0.1 wt.%) post-cured composites showed a small
increase in tensile strength and deformation and a drastic increase in tensile modulus,
while a 0.5 wt.% addition resulted in a significant improvement in tensile strength and
modulus, with a small decrease in deformation. Adding 0.1 and 0.5 wt.% CNCs improved
the thermal stability by increasing the critical temperatures of the composites, making them
more resistant to heat [54].
2.3. Powder-Based Sintering and Deposition Processes

2.3.1. Selective Laser Sintering (SLS)
Selective laser sintering converts powder into complex and functional structures by
melting thermoplastic with a laser beam. The powder reservoir is filled with a thermoplastic
powder such as nylon, then packed in a thin and uniform layer by a rotating roller. The
layer of powder is heated to a point close to the melting temperature to facilitate laser
sintering and prevent warping from a large temperature gradient. A high-powered laser
beam is directed onto a mirror, where a galvo motor focuses the beam to selectively heat
regions on the powder layer. This heating fuses the powder particles to form a solid part
layer. The particles that make up the powder are round, smooth, uniform, and less than
100 µm in diameter. Once a layer is sintered, the next layer is filled with powder and the
process repeats. Unheated powder surrounds printed layers and also acts as a support for
the printed part. Wang et al. investigated the relationship between SLS process parameters
and shrinkage using a neural network model [55]. Their study suggests that shrinkage ratio
decreases with increasing layer thickness, interval time, and laser power, while it increases
with increasing scanning speed and hatch spacing. The surrounding temperature increases
shrinkage from 82–85 ◦ C and results in a rapid decrease at temperatures higher than 85 ◦ C.
2.3.2. Binder Jetting (BJ)

Binder jetting is a mechanism similar to SLS and 2D printing wherein a layer of powder
is deposited onto a bed and a binder jetting head deposits a binding agent where the layer
needs to be solidified. Unlike SLS, BJ does not use heat or a laser, which allows for any
material to be the feedstock. Depending on the material and binding agent, some printed
parts need to be post processed by heat or chemicals. The printed part can undergo a
debinding process wherein excess binding agent left on the printed part is removed using
heat or solvent. The final step is sintering the printed part at a high temperature to solidify
and improve the properties.
2.3.3. Natural Fibers in SLS and BJ

Natural fibers are rarely used in composites created using SLS and BJ because of
the high operating temperature, which degrades most biomaterials. However, there has
been work on modifying natural fibers to incorporate them into composites made by these
techniques. Idriss examined how the processing parameters of sisal fiber-polyether sulfone
(SFPC) composites (weight percentage ratio of 1:5 for sisal fiber:polyethersulfone) affect
the mechanical properties of printed parts. Tensile and flexural strength increased with
increasing preheating temperature and laser power and decreasing scan speed. The results
were compared to wood-fiber composites, and sisal-fiber composites showed an increase
of over 100% in flexural strength and an increase of 50% in tensile strength [56]. In a
technique similar to SLS, Coelho manufactured a composite of gypsum and sisal fiber
using binder jetting technology. Samples were tested with and without fibers and with
and without post-processing adhesive infiltration. Adding fibers increased porosity by 4%
due to poor fiber-gypsum interfaces, which decreased the tensile strength of green parts
with fibers. However, the strength of fiber-impregnated samples increased by 41% with
post-processing, possibly due to the presence of curing resin in the available pores [57].
Evdokimov investigated the characteristics of five wood types, namely beech, oak, larch,
alder, and pine wood for creating fibrous composites with binder jetting and concluded that
pine-wood fibers were the most suitable because of their elasticity, length, lower energy
requirements, and small particle size [58]. Adjary et al. mixed alkali lignin and polyamide
12 (PA12) at a ratio of 40:60 wt.% to prepare 3D-printed composites with the SLS technique.
Addition of lignin decreased mass loss from 97% for pure PA12 to 77% for composite and
Sustainability 2023, 15, x FOR PEER REVIEW
increased porosity by 14% but also increased Young’s modulus by 16% [59]. Figure 5 11 of 31
shows
a summary of 3D-printing techniques and the typical matrices used.
Figure5.
Figure 5. 3D
3D Printing
Printing techniques
techniques with
withmatrices.
matrices.
3. Mechanical, Thermal, and Chemical Properties of Natural Fiber Composites

3.1. Tensile Strength, Flexural Strength, and Impact Resistance
Natural fibers have been proven to improve mechanical properties and provide rein-
forcement to the filaments and printed parts. The mechanical properties are inherently
3. Mechanical, Thermal, and Chemical Properties of Natural Fiber Composites

3.1. Tensile Strength, Flexural Strength, and Impact Resistance
Natural fibers have been proven to improve mechanical properties and provide re-
inforcement to the filaments and printed parts. The mechanical properties are inherently
influenced by the cellulose content of the fibers and the spiral angle formed by the mi-
crofibrils in relation to the fiber axis in their inner structure. Factors like the source of
the fibers, their age, and other variables influence both properties and structure [60]. The
attributes of natural fiber composites are influenced not only by the inherent qualities of
the natural fibers, but also by various testing parameters, such as fiber length, test speed,
temperature, etc. Introducing fibers into a polymer matrix is an important step because it
significantly enhances the composite’s mechanical properties. Readily available natural
fibers can provide reinforcement through fiber alignment, and fiber pretreatments help to
increase contact with the polymer matrix, which improves the mechanical properties of
the composite [14,61]. This phenomenon aligns with the Rule of Mixture theory, which has
been employed to approximate composite moduli, enabling the adjustment of properties to
various levels [62].
Nonetheless, it is crucial to emphasize that variances in mechanical properties are
a common occurrence, and these deviations can be ascribed to a multitude of factors,
including differences in process parameters, manufacturing techniques, fiber treatments,
and the wide-ranging sources of both fibers and polymer matrices. An overview of the
tensile strength, flexural strength, and impact strength of natural fiber composites is given
in Table 1. Investigations into the effects of fiber volume fractions and pretreatments on
hemp fiber with a polylactic acid (PLA) matrix provided valuable insights. Elastic moduli
increased with the addition of hemp fibers, regardless of fiber weight percentage and
pretreatments. However, increasing fiber volume decreased tensile strength and modulus.
Pretreatment of hemp fibers and weight-percentage loading showed little to no effect on
the flexural modulus, but alkali and silane pretreatment resulted in high flexural strength
for both 30% and 50% hemp fiber-loaded composites [63].
In the pursuit of creating 100% bio-based, biodegradable and sustainable composites,
various ratios of abaca fibers and bio-polyethylene (bioPE) have been employed, including
20/80, 30/70, 40/60, and 50/50 wt.%. The volume fraction of abaca fibers contributed al-
most linearly to the composites’ tensile strength, with maximum tensile properties achieved
at 50 wt.% fiber loading. Moreover, it has been observed that the measures of mechanical
properties increased in tandem with the weight fraction of abaca fibers and that the use of
maleic acid as a coupling agent further improved these properties [64]. The development of
bast-fiber composites by compression molding and chemically pretreating jute fibers with
amino-silicone oil has been explored. The experimental design varied molding temperature,
compression pressure, and pressure time. Box-Behnken design (BBD) response-surface
methodology (RSM) was utilized to predict tensile, flexural, and impact strengths. as well
as optimize compression molding conditions to provide the best composite mechanical
properties. Table 1 shows some other work related to optimization of natural fibers with
matrix material.
Table 1. Mechanical Properties of Natural fibers.
Tensile Flexural Impact

Natural Fiber wt.% Loading Matrix Material References
Strength (MPa) Strength (MPa) Strength
Kenaf 30–40 PLA 50–61 58–62 15–48 kJ/m2 [65]
40 PP 90 50 - [66]
30 PLA 36.18 64.90 116.6 J/m [38]
Jute 50 Epoxy 39.52 89.62 2.22 J [67]
26.9 Epoxy 70.4 84 - [68]
33 PP 27.49 43.33 25.54 kJ/m2 [69]
Flax 37.9 Epoxy 95.4 95 - [68]
20 PLA/PCL (70:30) 49–60 - 3.3–6 kJ/m2 [70]
22 PLA - 160–185 - [71]
Hemp 50 Epoxy 22.43 57.11 1.25 J [67]
30–50 PLA 39–65 51–113 - [63]
30 Polybenzoxazine 52 122 4.23 kJ/m2 [72]
0.040–0.048
Abaca 10–30 PP 22–30 46–54 [73]
kJ/m2
20–50 BioPE 26.64–47.73 - - [64]
30 HDPE 33.13 - - [74]
0.040–0.055
Coir 10–30 PP 24–30 48–57 [73]
kJ/m2
Melamine-Urea-
84–90 Formaldehyde (MUF) 3.05–4.4 2.099–5.149 - [75]
Biopolymer
5–30 Bakelite resin - 53–61 - [76]
3.2. Thermal Stability and Thermal Conductivity

Natural fibers exhibit biodegrade relatively rapidly, which contributes to the flamma-
bility of composites containing them. The decomposition of these natural fibers occurs at an
accelerated pace in a polymer matrix. It is essential to recognize that decomposition unfolds
at varying temperatures: cellulose undergoes decomposition first, followed by hemicellu-
lose, and eventually, lignin. Some factors that influence the thermal properties of natural
fiber composites are the fiber type, surface pretreatment, type of polymer matrix, other ad-
dition of fillers, and fiber content and orientation [77]. The thermal stability of natural fiber
composites can be quantified by thermogravimetric analysis (TGA), wherein the sample is
subjected to various temperatures in a controlled environment [78,79]. The specific temper-
ature and thermogravimetric method vary from one composite to another, but a starting
guideline can be obtained by implementing ASTM E2250. The typical decomposition
pattern for lignocellulosic biomass consists of three stages. Stage one involves the removal
of water from the natural fiber (60–100 ◦ C). Stage two entails the breakdown of the primary
components of the fibers, including hemicellulose, cellulose, and lignin (200–500 ◦ C). The
final stage results in the formation of ash, which remains as a residual substance.
Several researchers have employed thermogravimetric analysis to assess the thermal
stability of natural fiber composites. For example, a composite of bamboo fiber and
epoxy resin exhibited first-stage weight loss at temperatures under 155 ◦ C. Second-stage
decomposition occurred from 199–399 ◦ C and signified the degradation of cellulose and
hemicellulose, while the final stage occurred from 364–499 ◦ C, signifying the degradation of
lignin [80]. In another study, sugar-palm fibers were mixed with phenolic resin at a 30 wt.%
loading. TGA results revealed that the initial weight loss occurred from 30–200 ◦ C, when
moisture is lost. The second stage involves hemicellulose, cellulose, and lignin degradation
and occurred between 300 ◦ C and 400 ◦ C. The final phase occurred at 300–400 ◦ C, which
corresponds to losing small groups and water bonds in the chains of the chemical structures.
The chemical treatment negatively affected the thermal stability of the composite [81]. Bessa
investigated the thermal characteristics of benzoxazine resin composites reinforced with
Arundo donax L. (ADL) fibers. It was shown that the second and third stage of decomposition
occurred at 200–300 ◦ C and 350–500 ◦ C, respectively [82]. Fique fibers are typically grown in
the South American Andean region and have been used as structural reinforcement material
for polymer composites. At 60–100 ◦ C, moisture evaporation occurred; at 250–350 ◦ C,
hemicellulose decomposed; at 350–600 ◦ C, cellulose degraded. Incorporating fique fiber
into the LLDP matrix decreased the time to onset of degradation and the peak degradation
temperature compared to pure LLDP composite. For the epoxy resin composite, fiber
incorporation increased the time to the onset of degradation and the peak degradation
temperature compared to the pure epoxy [83].
Epoxy is a resin commonly used in natural fiber composites due to its inherent thermal
stability and pose good thermal compatibility to various natural fibers. Sisal and hybrid
fibers have been investigated as reinforcements for epoxy. Investigations involving sisal
and hybrid fibers as reinforcements for epoxy composites revealed that hybridizing sisal
with curauá fiber and ramie fiber enhanced the composites’ thermal stability compared
to pure sisal composites [84]. Similarly, hybridizing epoxy composites with jute fiber and
oil-palm fiber increased the maximum degradation temperature compared to pure oil-palm
fiber composites [85]. However, in the case of banana and jute fibers, hybridization had a
lesser impact compared to the fiber content. Increasing the fiber content decreased in the
thermal diffusivity and specific heat capacity of the jute/banana hybrid composite [86].
PLA is another common matrix used in natural fiber composites due to its biodegrad-
ability and compatibility with natural fibers, which arises from its low glass-transition
temperature. Similarly to epoxy resin, PLA composites are influenced by hybridization
with flax and basalt natural fiber. The hybrid composite exhibited an increased temperature
of degradation onset compared to the flax + PLA composite, with the addition of basalt
fiber contributing to improved thermal stability. The addition of basalt fiber also increased
the thermal stability of the composite [87]. Jute and PLA are recognized as a promising
combination for natural fiber composites. Initially, weight loss in jute-PLA composites can
be attributed to water evaporation, which is followed by the thermal decomposition of
jute fiber at approximately 250 ◦ C. In contrast, the PLA matrix experiences degradation at
around 340 ◦ C, with the composite decomposing most rapidly at approximately 390 ◦ C.
During this stage, there is noticeable and significant weight loss due to the degradation of
cellulose and the release of volatile compounds produced by PLA, such as carbon monoxide
and dioxide [88]. Table 2 describes the range of weight loss associated with decomposition.
Table 2. Material with temperature range for decomposition.
Material Temperature (◦ C) Weight Loss during Decomposition Reference

Bamboo Fiber and Epoxy Resin 60–155 Moisture loss
199–399 Cellulose and hemicellulose [80]
364–499 Lignin
Sugar Palm Fiber and Phenolic Resin 30–200 Moisture loss [81]
300–400 Hemicellulose, cellulose, lignin
300–400 Small groups and water bonds
in the chemical structures
Arundo donax L. (ADL) Fibers and 200–300 Second stage of decomposition [82]
Benzoxazine Resin Composite 350–500 Third stage of decomposition
Fique Fiber and LLDP Matrix 60–100 Moisture evaporation [83]
250–350 Hemicellulose
350–600 Cellulose
Epoxy Resin Composites with
Sisal and Hybrid Fibers Varies Improved thermal stability in [84]
hybrid composites
Epoxy Composites with Jute and Varies Increased maximum degradation [85]
Oil Palm Fiber temperature in hybrid composites
Jute and PLA Composite Water evaporation at Water evaporation, jute fiber [86]
lower temperatures decomposition, PLA matrix
4. Tribological Properties
Tribological properties describe the behavior and characteristics of a material when it
interacts with other materials, especially in terms of friction, wear, and lubrication. These
properties are crucial to evaluating the compatibility of materials in a system with me-
chanical parts. Factors that can quantify tribological properties include frictional and wear
resistance and lubrication effectiveness [89]. The wear resistance of composite materials
varies depending on the orientation of the reinforcing fibers. In jute fiber-reinforced epoxy
composites, there is a hierarchical trend in wear resistance, with the anti-parallel orientation
surpassing the parallel and normal orientations in terms of the sliding direction and applied
force. In the anti-parallel orientation, the mats were strategically arranged to align parallel
to the direction of the applied force while remaining perpendicular to the sliding direction.
Under experimental conditions characterized by a load of 30 N and a sliding velocity of
3 m/s, the anti-parallel-oriented mat exhibited a maximum volume loss of merely 10 mm3
when subjected to an extensive 11 km sliding distance against a stainless steel surface [90].
In a comparison of white and brown coconut fibers, the brown fiber-reinforced com-
posite displayed better wear resistance due to the greater hardness and porosity and lower
median pore diameter of the brown fibers. Interestingly, an NaOH treatment had no ob-
servable effect on wear resistance, but aligning the fibers perpendicularly to the direction
of rubber disc had a small effect [91]. Another study explored hybridizing sisal fibers and
coconut sheath with polyester as the polymer matrix. In single-fiber composites, both mass
loss and specific wear rate (SWR) consistently increased with sliding distance. Conversely,
hybrid composites exhibited a unique trend: mass loss and SWR initially increased up to
1800 mm of sliding distance and then declined. This shift can be attributed to the hybrid
composites having lower porosity and void content compared to single-fiber composites.
Regardless of the type of composite, the coefficient of friction (COF) consistently increased
as sliding distance increased. This effect is due to increased contact between the polymer
surface and abrasive grit as the sliding distance increases [92]. Liu investigated the in-
fluence of mixing silane-treated corn-stalk fiber with nitrile butadiene rubber-modified
phenolic resin on the wear resistance of the composite. The different weight percentages
(1–13 wt.%) of fibers loaded in the composite samples had minimal effect on the COF, which
increased up to 150 ◦ C. The COF decreased at temperatures higher than 150 ◦ C, possibly
due to composite degradation [93].
5. Applications of Natural Fiber-Reinforced Polymer Composites in Various Industries
Natural fiber composites are a viable option for several applications due to their low
production cost [94]. Possible applications include car bodies and interiors, storage devices,
walls and ceilings in commercial and industrial spaces, and even false ceilings. Figure 6
depicts many applications in the automobile, transportation and aerospace, construction
and building, electronics, sports, residence construction, and material handling and storage
industries. The ever-increasing size of aircraft wings and wind-turbine blades is contin-
uously testing advanced materials, designs, and fabrication techniques. Composites will
be made with processed fiber and resin as fillers [95]. Research efforts focus on using
high-quality components and streamlined production procedures. When weight-bearing
ability is a primary concern, NFPCs can be used instead of glass in several contexts. The
superior mechanical characteristics and lower cost of fiber-reinforced composites make
them superior to polymer resins for structural applications.
Commercial aircraft use composites in construction: 50% in the Boeing 787 Dreamliner,
53% in the Airbus A350 53%, and 25% in the Airbus 380. Fuel efficiency can be significantly
enhanced by using lighter materials. Using composites reinforced with natural fibers allows
for a 35% reduction in aircraft weight. The Mercedes Benz E-class was the first to employ
NFRCs for the inner door panel, combining flax and sisal with epoxy polymer, achieving
weight savings of 20% [96].
Commercial aircraft use composites in construction: 50% in the Boeing 787 Dream-
liner, 53% in the Airbus A350 53%, and 25% in the Airbus 380. Fuel efficiency can be sig-
nificantly enhanced by using lighter materials. Using composites reinforced with natural
fibers allows for a 35% reduction in aircraft weight. The Mercedes Benz E-class was the
Sustainability 2023, 15, 16171
first to employ NFRCs for the inner door panel, combining flax and sisal with 15 of 30
epoxy pol-
ymer, achieving weight savings of 20% [96].
Figure 6. Applications
Figure 6. ApplicationsofofReinforced NaturalFiber
Reinforced Natural Fiber Composites
Composites in Industrial
in Industrial sectors.
sectors.
Numerousnew
Numerous newapplications
applications forforbiofiber
biofibermaterials
materials have emerged,
have emerged, including window
including window
frames and decking, dashboards and parcel shelves, door panels,
frames and decking, dashboards and parcel shelves, door panels, seat cushions, seat cushions, and back- and
rests, and cabin linings. More industries, such as the automotive, aerospace, marine,
backrests, and cabin linings. More industries, such as the automotive, aerospace, marine,
electrical and electronics, sports, recreation equipment, and machinery office-equipment
electrical
sectors, and electronics,
are switching sports,
to NFCs fromrecreation equipment,
petroleum-based fibers,and machinery
as are office-equipment
the automobile and con-
sectors,
struction industries, because of its low-cost processing, excellent comparative mechanical and
are switching to NFCs from petroleum-based fibers, as are the automobile
construction
properties, industries, becausecorrosion
ability to withstand of its low-cost processing,
and fatigue, excellent comparative
and recyclability. Many companies mechan-
icaluse
properties, ability
natural fibers. Fortoinstance
withstand corrosion
Daimler Benz and fatigue,dashboards,
constructed and recyclability. Many com-
center-armrest
consoles,
panies and seatfibers.
use natural shells out
Forofinstance
natural fibers.
Daimler Volkswagen utilized natural
Benz constructed fibers tocenter-arm-
dashboards, create
rest consoles, and seat shells out of natural fibers. Volkswagen utilized natural and
the boot-lid finish panel, seatback, boot lining, and door panel for the Passat, A4, Golf, fibers to
Bora.the
create The use of cellulose
boot-lid fibers like
finish panel, flax and
seatback, abaca
boot increased
lining, and NFC
dooruse in several
panel vehicles
for the Passat, A4,
by about 98% over older models [97].
Golf, and Bora. The use of cellulose fibers like flax and abaca increased NFC use in several
The European Commission issued directives in 2000/53/EC mandating that 85% of
vehicles by about
the weight 98% over
of products, older models
particularly [97].be recyclable by 2005. By 2015, manufac-
vehicles,
Thewere
turers European Commission
to achieve a recyclingissued directives
rate of 95%. in 2000/53/EC
Automakers mandating
must incorporate that in
biofibers 85% of
thecomposites
weight of to products, particularly vehicles,
balance sustainability and cost [98]. be recyclable by 2005. By 2015, manufactur-
ers were to achieve
Biofibers are a recycling
used rate of
extensively in 95%. Automakers
the production mustpanels,
of door incorporate biofibers
dashboards, in com-
parcel
shelves,
posites seat cushions,
to balance backrests, and
sustainability andcabin
cost linings.
[98]. More industries, such as the automotive,
aerospace, marine, electrical and electronics, sports, recreation equipment, and machinery
office-equipment sectors, are switching to natural fibers from petroleum-based fibers [99].
The automotive manufacturing applications of natural fiber-reinforced polymer composites
are depicted in Figure 7. Natural fibers were used by Opel’s other producers on the
instrument panel, headliner panel, door panels, and pillar-cover panel of models such
the Astra, Vectra, and Zafira. The Citroën C5 model included interior door-paneling
components made from natural fibers. The Raum, Brevis, Harrier, and Celsius Toyota
models included door panels, seat backs, floor mats, and spare tire covers made from
natural fiber. Mitsubishi (Space Star, Colt Cargo) used natural fibers for flooring, instrument
panels and door panels. Rear parcel shelves made from natural fibers used by Renault
(Clio, Twingo), and Volkswagen (Golf A4, Passat, Variant, Bora) includes natural fiber in
the door panel, seat back, boot-lid finish panel, and boot liner. The Lotus Eco Elise model
includes body panels, spoilers, seats, and interior carpets made from natural fibers [100].
Hybrid polymer-based composites increasingly use synthetic fibers, including glass,
carbon, and aramid, for their superior stiffness and strength. Biodegradability, high ini-
tial processing costs, non-recyclability, high energy consumption, machine abrasion, and
potential health risks are some of the main disadvantages of using these fibers [101].
fiber in the door panel, seat back, boot-lid finish panel, and boot liner. The Lotus Eco Elise
model includes body panels, spoilers, seats, and interior carpets made from natural fibers
[100].
Hybrid polymer-based composites increasingly use synthetic fibers, including glass,
Sustainability 2023, 15, 16171
carbon, and aramid, for their superior stiffness and strength. Biodegradability, high16initial
of 30
processing costs, non-recyclability, high energy consumption, machine abrasion, and po-
tential health risks are some of the main disadvantages of using these fibers [101].
Figure 7. Natural
Figure7. Natural Fiber-Reinforced
Fiber-ReinforcedPolymer
PolymerComposites
CompositesUsed
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inVarious
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Automobiles.
Some
Somechallenges
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composites are
aretheir relatively
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and flammability.
high flammability. Additionally,
Additionally,variability
variabilityininfiber
fibercharacteristics
characteristics
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properties contributes
contributes toto large
large scatter
scatter in
in the
the properties
properties ofofNFRCs.
NFRCs. Certain
Certain fibers
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are
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not compatible with certain polymer matrices and may be susceptible to damage from
compatible with certain polymer matrices and may be susceptible to damage from
insects
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and fungi. Productperformance
fungi. Product performanceand andreliability
reliabilitydepend
dependononwhether
whether thethe natural
natural fi-
fiber causes higher moisture absorption (swelling), and variation in natural
ber causes higher moisture absorption (swelling), and variation in natural fiber character- fiber charac-
teristic features/quality
istic features/quality depends
depends onon
thetheconditions
conditionsofofcultivation
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weather, aa complex
complex
supply chain, and geographical availability. NFRCs exhibit low thermal
supply chain, and geographical availability. NFRCs exhibit low thermal conductivity conductivity
compared
compared to to glass
glass fiber-reinforced
fiber-reinforced composites,
composites, but but natural
natural fibers
fibers exhibit
exhibit poor
poor wettability,
wettability,
resulting
resulting in weak fiber-matrix interfacial bonding and worse mechanical properties. They
in weak fiber-matrix interfacial bonding and worse mechanical properties. They
are also subject to fluctuations in price and supply due to weather and crop production,
are also subject to fluctuations in price and supply due to weather and crop production,
as weather and crop yield can significantly affect both prices and supplies. NFRCs have
as weather and crop yield can significantly affect both prices and supplies. NFRCs have a
a service temperatures lower than 200 ◦ C, so they can be used only for non-structural
service temperatures lower than 200 °C, so they can be used only for non-structural com-
components [11].
ponents [11].
The fundamental drawback of incorporating NFRCs into a polymer matrix is the
absence of interfacial interaction between the two components, which results in a less
ideal end product. Chemical modifications such as alkaline treatment can strengthen the
bond between the NFRC and the matrix. Morphological examination demonstrates that
when non-cellulose materials are removed from the surface of alkali-treated particles, the
interfacial adhesion between the particles and matrix is improved [12].
The mechanical characteristics and dimensional stability of composites are reduced by
humidity and aging. Matrix materials like polyester are quickly hydrolyzed by moisture,
lowering the molecular weight of the polymer. Temperature and humidity affect how
quickly materials decompose through hydrolysis [102]. Salem et al. examined the effects
of fiber loading (10 to 40) wt percent) on the ability of a kenaf/polyester composite’s to
absorb water at room temperature. Because of the high hydrophilicity of NFRCs, natural
fiber composites typically absorb 2% of their weight in moisture within 24 h, 5% within a
week, and up to 22% after many months [103]. Moisture-exposed composites have different
surface morphologies than their dry counterparts, with increased permeability, swelling,
gaps, adsorption in cracks, and fissuring around the NFRCs. Between 215 and 310 degrees
Celsius, most natural fibers undergo around 60 percent thermal degradation has been
found [104]. Solar ultraviolet (UV) radiation causes the breakdown of covalent bonds
in organic polymers, leading to consequences such as yellowing, discoloration, weight
loss, surface roughening, deterioration in mechanical properties, embrittlement, and a
pronounced decline in the thermal stability of natural fiber composites [105].
Natural fibers often have their surfaces treated to improve their properties before
they are used to make composite materials. Surface modification improves fiber-matrix
interfacial bonding, roughness, and wettability, hence decreasing the fibers’ moisture
absorption. The resulting composites have enhanced mechanical properties. Hybrid
composites benefit from fiber treatment because of this enhanced performance [18].
Physical treatment: Adhesion among the fiber surface and the polymer matrix can be
enhanced by applying physical treatments that affect the fiber surface and increase fiber
strength. The interfacial bonding between the NFRC and the matrix is improved through
physical treatment, which reinforces the interface without affecting the chemical properties
of the fiber [106]. Plasma, corona, electron radiation, ultraviolet, heat treatments, and fiber
beating are used to modify the surface of natural fibers. Gassan and Gutowski showed that
Corona treatment modifies cellulose fibers’ surface energy, making them more amenable to
incorporation into the NFRC. This technique employs high voltage at low temperatures
to generate plasma at atmospheric pressure. In plasma therapy, the gas type, rate of gas
flow, gas pressure, and gas concentration are controlled [107]. The NFRCs are heated
to a temperature close to their degradation point during heat treatment. However, this
treatment affects the NFRC’s physical, mechanical, and chemical characteristics, including
their chemical composition, fiber strength, and cellulose crystallinity. These processes affect
the fibers’ surface characteristics without changing their structural makeup, enhancing the
bond between the fiber and the matrix. When comparing chemical and physical treatments,
the primary difference is the cost of the equipment for physical treatments [108].
Chemical treatment: Enhancing adhesion to the fiber matrix through chemical bonding
or mechanical interlocking at the interface, as is done in many chemical treatments, is
a common way to reduce the fibers’ water absorption [109]. Compounds used for this
purpose include acetic acid, benzoyl chloride, sodium hydroxide, silane, malleated coupling
agents, peroxides, isocyanates, and stearic acid. Sumrith et al. used water-hyacinth fibers
treated with NaOH and silane to form reinforced bio-epoxy-based composites by casting.
The results show that hyacinth fibers can be used with bio-epoxy polymer as a reinforcement
material to produce biobased, eco-friendly composites with lightweight structures [110].
Chemical methods result in better enhancement of properties than physical methods.
Mechanical and thermal properties are enhanced by chemical concentration and are de-
pendent on exposure time. Sometimes, the mechanical and thermal properties resulting
from combined treatment with two chemicals were superior to those resulting from either
treatment used alone [111].
Improvements in fiber-matrix interfacial adhesion, roughness, and wettability were
observed in chemically and physically modified natural fibers. Most treatments also lessen
natural fibers’ hydrophilicity and their propensity to absorb moisture. Depending on
fiber, matrix, filler, and other factors, fabric polymer composites can exhibit improved
mechanical and thermal properties. Fiber content, aspect ratio, and fiber orientation are
important characteristics of composites. The manufacturing process and the techniques
used to create the fiber (cylindrical, spherical, or rectangular cross-sectioned prisms or
platelets) are significant as well [112].
The matrix contributes significantly to the composite’s shear properties, compression,
and transverse modules (mechanical properties). Matrix properties like curing temperature,
duration, viscosity, and fiber-bonding behavior influence the manufacturing strategy [113].
The matrix in composites binds the fibers and distributes loads between them. Aims in-
clude the optimum orientation and location of the fibers, shielding them from damaging
environmental factors such as temperature, humidity, chemicals, and abrasion, and sup-
porting interlaminar shear. The matrix enhances the composite’s transverse properties [114].
Limited shrinkage, dimensional consistency, chemical resistance, reduced coefficient of
thermal expansion, decreased water absorption, resistance to damage from significant
temperature increases, elasticity for load transfer to the fiber, excellent flow characteristics
that allow the matrix to penetrate fiber bundles and remove voids during compacting, and
the ability to be easily shaped into the final composite form are highly desirable properties
of a composite matrix [115]. The fiber/matrix employed and the composite’s intended use
will determine the best technique for fiber modification. To use NFRCs and hybrid compos-
ites, it is crucial to understand the interfacial properties and bonding mechanisms of the
fiber-matrix interaction, which necessitates extensive research [116]. Inadequate adhesion
between the fibers and the matrix will lead to inefficient load distribution, reducing the
composite materials’ mechanical properties (such as tensile, flexural, and impact strength).
Obtaining the correct mechanical and thermal properties in composites involves finding
the right fiber/matrix combination [117].
The matrix protects the reinforcement fibers from wear and tear caused by mechanical
and chemical abrasion, keeps the fibers in their proper positions, and transfers stress
adequately between them.
Matrix types include ceramic, metallic, and polymeric matrices. There are two broad
categories of polymer matrix: thermosets and thermoplastics. Polymeric (thermoset or
thermoplastic) matrices are most typically utilized to make hybrid natural fiber composites
because they can be produced at low temperatures and are lightweight. Thermoplastic poly-
meric matrices include nylon, cellulose acetate, polylactic acid, polycarbonate, polyethylene,
polypropylene, polystyrene, polyvinyl chloride, polylactic acid, and polyether-ether ke-
tone, while thermoset polymeric matrices include epoxy, phenolic, polyester, polyamide,
polyurethane, and ester vinyl chloride. Epoxy and unsaturated polyesters are the primary
thermoset resins used in hybrid natural composites [118]. Epoxy resins are resistant to
environmental deterioration and have high mechanical strength. Epoxy resins are known
for their strong adhesive properties and are simple to use and cure. A crucial advantage of
epoxy resins over phenolic, polyester, and vinyl ester resins is that no volatile substances
are created during curing. Additionally, compared to polyesters, epoxy resins experience
less shrinkage [119]. The relative brittleness of epoxy resins, which has serious negative
effects on the interlaminar characteristics of the matrix and the fiber reinforcement, is a
disadvantage. Epoxy resin undergoes a catalytic chemical reaction when it cures from a
liquid to a solid, forming strong bonds that are difficult to undo or reform. This reaction
results in this matrix material having superior performance compared other matrices, but
recycling this material is still difficult. Most natural fibers become unstable at temperatures
above 200 ◦ C, and matrices that call for high processing temperatures are ineffective for
producing NFRCs or hybrid natural fiber composites [120].
5.1. Automotive Industry

Natural fiber composites have made a positive impact in the automotive industry due
to their light weight and desirable mechanical properties. Their light weight decreases the
overall weight of the vehicle, hence decreasing fuel consumption, which makes the vehicles
more sustainable. Natural fibers have been investigated for potential automotive appli-
cations by several authors in the literature. The structural design of a bonnet containing
flax-fiber composite was investigated through impact-damage analysis. The structure was
first manufactured using resin-transfer molding. Steel panel and flax-vinyl ester panels
were compared in compression and impact tests, and it was concluded that the composite
resulted in a 31.7% weight reduction with similar mechanical properties compared with the
steel panels [121]. Another composite investigated for automotive applications, especially
for the front cabinet, body sheet and lighting frames, is caryota fiber and polyester with 40%
weight fiber loading. A 50 mm fiber length and 40% weight of fiber loading had the best
mechanical properties [122]. Nachippan investigated the impact strength of automotive
bumpers and bodies using glass fiber, natural fiber (hemp), and hybrid composites mixed
with epoxy. They concluded that hybrid composites possess better impact strength and can
protect the vehicle body and passengers better than glass-fiber composites [123]. Another
study investigated the applications of composites of alkali-treated sugarcane bagasse and
palm-sheath fibers in an epoxy matrix in automobile dashboards. A matrix: fiber ratio
of 60:40 with a hybrid combination of treated 40% palm and 60% bagasse showed the
highest tensile strength, Young’s modulus, elongation, flexural strength, impact strength
and hardness, making it a superior composite for dashboard applications [124]. Another
investigation subjected Desmostachya bipinnata fibers to silane treatment to fabricate
brake-pad composites. The pretreatment increased hydrophobicity, hardness and shear
strength, and the wear rate of treated fiber-composite brake pads was lower. This result
shows that pretreated Desmostachya bipinnata fibers are suitable for use in brake pads
because of their wear resistivity and high coefficient of friction [125].
Vehicle manufacturers have started using natural fibers, especially lignocellulosic
biomass waste, in their vehicles. Mercedes Benz, one of the leading automobile manu-
facturers from Germany, included jute and flax fibers in an epoxy matrix in their A- and
E-class models, mainly in their sunroof, gearbox and door panels. The sunroof frame was
developed using 70% renewable materials, mostly sourced from natural fibers such as jute
ad sisal. and offers up to 50% reduction in weight compared to a traditional metal sun
roof frame [126,127]. Before Mercedes Benz, BMW had been one of the first car companies
to use natural fibers in their cars, where flax and sisal were used in the car door lining
and some of the vehicle panels, which increased the vehicles’ impact resistance. BMW
also incorporated wood fiber and cotton for a high-quality sound system and as filler
for car seats, and this method has been used in many car manufacturers after them [128].
Additionally, Audi used flax and sisal fibers in their door panels, with the polymer matrix
being polyurethane (PU) [129]. In the 2003 Toyota RAUM, the spare-tire cover was made
out of sustainable composites based on kenaf fibers reinforced with sugarcane- and sweet
potato-based PLA [130].
5.2. Aerospace Industry

Even though research is being done into developing sustainable composite materials
for the aerospace sector, the composites currently used in aircrafts are mainly made from
carbon fiber, aluminum, and titanium due to their high strength-to-weight ratio. The
widely available Boeing 787 Dreamline and Airbus 350 XWB include some composite parts,
including but not limited to turbine housing, wing panels and stabilizers. This choice
has shown to increase passenger comfort and noise cancellation, while reducing weight
and fuel consumption [131]. Other common applications include interior parts such as
seating, cabin dividers, restrooms panels, overhead bins, flooring, and wall coverings [132].
Within the aviation sector, critical objectives include reducing aircraft weight, enhancing
fuel efficiency, increasing payload capacity, and improving aircraft maneuverability [133].
These objectives can be effectively achieved by employing NFRP composites, which not
only contribute to heightened aircraft efficiency through reduced fuel consumption and
emissions but also offer remarkable strength and stiffness, facilitating the fabrication of
intricate aerodynamic shapes. NFRP composites exhibit excellent fatigue resistance and
corrosion resilience [132,134].
More than 200 aircraft components are crafted from NFRP composites, encompassing
elements such as cabin furnishings, sidewalls, and propulsion systems [133,134]. This
significant shift towards NFRP composites in aviation has been supported by the European
Union through initiatives like the Cayley project, a collaborative effort involving Boeing
Research and Technology, Invent GmbH, Aimplas, and Lineo. The aim of this project is
to develop environmentally friendly interior panels for aircraft by utilizing flax fiber and
recycled thermoplastic sheets [135]. Another EU-funded project, known as Eco-Compass,
is dedicated to the development of eco-friendly composites derived from bioresources and
recycled materials for aviation applications. The primary focus of this project is to explore
alternative ways to reduce the use of carbon- and glass-reinforced polymer composites in
aircraft by incorporating bioresins, natural fibers, or recycled carbon fibers in secondary
structural and interior applications. Flax and ramie fibers have demonstrated potential for
incorporation into NFRP composites for aircraft, offering improvements in tensile strength
and flame-retardant properties [136,137].
Similar to the Boeing 787 and the Airbus 350 XWB mentioned earlier, the Boeing
737 aircraft also used natural fiber composites, namely flax/epoxy sandwich composites
in the sidewall panels, with the flax fabrics treated to be halogen-free and fire-retardant.
These flax/epoxy panels are not only 35% lighter than carbon/epoxy composites, but also
have a structure similar to that of glass/epoxy unidirectional composites [132]. Beyond
epoxy, phenolics and engineering thermoplastics such as polyphenylene sulfide, polyether
ether ketone, polyamide (PA), and polycarbonate (PC) have garnered significant attention
in the aviation industry. This attention is primarily due to their excellent fire resistance,
aligning with the stringent flame, smoke, and toxicity regulations applicable to aviation
materials [138]. For instance, polyether ether ketone (PEEK) was reinforced with chopped
glass and carbon fiber by Victrex Europa GmbH, who developed VICTREX® PEEK for
aircraft applications. This composite exhibits mechanical strength and dimensional stability
comparable to those of metal alloys, withstanding high temperatures and displaying
resistance to corrosion, chemicals, wear, and abrasion [131].
5.3. Medical Industry

In the biomedical industry, lignocellulosic fibers rarely are used, except for in recent
novel regenerative studies, but the wearable technology sector has taken this opportunity
to utilize biomass waste to develop a strain sensor for biomedical applications. The sensor
was constructed from a conductive and flexible composite in which carbonized walnut shell
powder was blended with polydimethylsiloxane (PDMS). The composite demonstrated
exceptional sensitivity in detecting human body movements. The potential applications
for this innovative sensor are boundless, with the tantalizing prospect of it evolving into a
versatile and adaptable technology for wearable, flexible sensors that enhance our daily
lives [139,140].
Animal-based fibers such as silk and chitosan and cellulose-based nanoparticles have
been studied. with promising results. Silkworm- and spider-produced silk have been
applied in medical components such as sutures, sponges, and films [141–144]. The allure
of silk lies in its distinctive usefulness as a scaffold biomaterial, in particular because of
its ability to degrade gradually. This unique feature aligns perfectly with the demands of
biomedical applications, offering a material that seamlessly integrates with the body’s nat-
ural processes. One particularly striking advantage of employing animal-based fibers like
silkworm silk and spider silk in medical implants and bone repairs is the elimination of the
need for a secondary surgical procedure to remove metallic implants. This groundbreaking
advancement not only enhances patient comfort, but also reduces the associated risks and
costs, revolutionizing the field of medical interventions [143,145].
Steering our focus towards the world of advanced technology and biosensors, we
encounter an exciting development in the form of nanocomposites. These nanocomposites,
designed to encapsulate gold nanoparticles with the aid of camphorsulfonic acid (CSA)
surfaces, have applications in electrical devices and biosensors. The nanocomposites
showed high solubility in water and select organic solvents, rendering them exceptionally
versatile for an array of applications [146]. Another noteworthy innovation is a self-cleaning
and antimicrobial hybrid system. This ingenious system is based on a foundation of
polybutylene succinate (PBS) and polybutylene adipate-co-terephthalate (PBAT), fortified
with the inclusion of lignin and zinc nanoparticles. The result is a material with the
remarkable capability to repel dirt and hinder the growth of harmful microbes. This
development not only had immediate implications for maintaining cleanliness and hygiene,
but also holds significant promise for various sectors that demand durable and hygienic
surfaces [147].
5.4. Construction Industry

Geopolymer materials have attracted significant interest for their remarkable technical
characteristics, which closely resemble those of conventional Portland cement-based materi-
als, all while significantly mitigating carbon dioxide (CO2 ) emissions and minimizing their
overall environmental footprint. Furthermore, integrating natural fibers, including but not
limited to bamboo, flax, hemp, and jute, within the geopolymer matrix is a compelling
avenue of exploration. These natural fibers serve as a reinforcing component, enhancing

the tensile and flexural strength while reducing material density, creating lightweight
construction materials. Another advantage of using these natural fiber composites on the
interior of buildings include improved thermal insulation, which leads to energy efficiency
and better soundproofing.
Different aspects of natural fiber-reinforced geopolymers have been studied in the
literature. One of the important factors in choosing materials for construction is flame-
retardation properties, which allow the building material to act as a flame retardant in case
of a fire. Silva studied the fire-resistance and head-absorption capabilities of a jute fiber-
reinforced pozzolan-based geopolymer. The samples demonstrated an impressive ability
to absorb nearly 65% of the heat generated by the flames, with minimal degradation [148].
Other common properties sought after by the construction industry are high mechanical
strength and hydric properties. Bast-hemp fibers were investigated with and without
sodium hydroxide pretreatment at 3% weight loading in diatomite geopolymer, and the
composite showed an almost 100% increase in compressive strength and a 35% increase in
flexural strength while maintaining thermal conductivity [149]. Flax linen, cotton and abaca
fibers also showed an increase in compressive strength after being mixed with geopolymer.
Alkali treatment of the abaca fiber facilitated fiber bonding with fly ash and increased the
flexural strength of the composite [150]. When untreated cotton- and flax-based linens
were investigated for use in fly-ash composite, the compressive and flexural strength of
the composites increased, but the flexural strength of the linen-fly ash composite increased
significantly, by 60% [45,151].
With a rising global emphasis on sustainable materials, recent breakthroughs in FFFs
have broadened their usefulness across numerous domains. Material innovation has wit-
nessed the development of novel hybrid resins for DLP 3D printing of biocompatible
scaffolds using renewable resources [152], extrusion methods for high-performance ther-
moplastics derived from recycled materials [153], and laser-sintering techniques for silicon
carbide-based ceramics utilizing post-industrial waste [154]. Process improvements in-
clude adaptive process control for laser powder bed fusion [155] AM to optimize material
usage, in situ monitoring using computer vision to minimize material consumption, and
multi-material AM systems with extrusion-based approaches that facilitate the effective
integration of sustainable materials [156]. Personalized orthotics and prosthetics made of
recyclable and biocompatible materials, aerospace parts like rocket engines and aircraft
parts made of lightweight, sustainable materials, and medical devices like implants and
surgical guides that are made with biocompatibility and sustainability in mind are just
a few of the numerous applications of additive manufacturing (AM) [157,158]. These
developments highlight AM’s revolutionary potential to promote a circular economy and
advance environmentally friendly manufacturing techniques, opening the door for more
ground-breaking discoveries in the years to come.
6. Challenges and Opportunities

Additive manufacturing and the incorporation of natural fibers in different additive
manufacturing technologies may have great benefits for many industries by improving
composite properties. The new materials have similar or better characteristics compared to
synthetic fibers, with a smaller carbon footprint. However, there are challenges and aspects
of this sector that need to be explored and better understood.
First, because natural fiber composites emerged only recently, there are limited data on
the durability, safety and recyclability of NFCs. Although PLA is a commonly used polymer
composite matrix and is commonly derived from bio-based sources, the recyclability of
NFCs remains uncertain. Some composites may contain precursors and chemical agents
based on formaldehyde, which can emit volatile compounds that may pose a safety concern.
In outdoor applications of composites, the durability of the composites is relevant. In
addition, some composite additives can seep out when subjected to moisture, high humidity
or rain, which can potentially cause chemical leakage into the water system.
The development of NFCs is gaining momentum and holds promise as a sustainable

source of material for various new applications. More work needs to be done to overcome
the challenges associated with the development of NFCs at a large scale, such as cost
and the constraint of technological adaptation. NFCs inherently exhibit relatively inferior
mechanical properties due to the incompatibility between natural fibers and the polymer
matrix and the inherently weaker nature of natural fibers compared to their synthetic
counterparts. A potential solution to address these drawbacks involves the modification of
natural fibers through physical, chemical or biological means. For instance, alkalization al-
ters the fibers’ structures, substantially reducing the fibers’ capacity for moisture absorption
and thereby enhancing the interfacial adhesion between the fibers and the polymer matrix.
Despite these limitations, the use of NFCs is growing, especially in the automotive sector.
There, long fibers like hemp, kenaf, and flax are increasingly being integrated into various
automotive components. The adaptability of wood-plastic composites for construction
highlights the diverse uses of NFCs. Additionally, these materials have been successfully
used in electrical devices and sporting goods, highlighting their potential for a significant
market presence.
Future directions for NFCs should be include development of new composite materi-
als; improving fiber-matrix interfacial properties, fiber homogeneity and alignment and
interlayer bonding; addressing porosity issues; and improving printability. One drawback
of natural fibers is their vulnerability to fluctuations in supply, price and quality with
different seasons, climates and temperatures, which can significantly affect the production
and properties of NFCs. One potential solution to this problem can include hybridization,
whether between natural fibers or natural fiber and synthetic fiber, which can optimize
the properties of the resulting composites. Future research can also focus on ensuring
the long-term stability of NFCs in outdoor applications where the composite parts are
subjected to weather changes, UV radiation and humidity.
7. Conclusions
In conclusion, the development of additive manufacturing has ushered in a new phase
in materials science that is marked by investigations into natural fiber-reinforced polymer
composites. The creation of unique composite materials that can resist structural failure
while being environmentally sustainable has been made possible by the collaborative
fusion of traditional materials-science paradigms with state-of-the-art manufacturing tech-
niques. This approach has produced groundbreaking results. The progress made in 3D
printing highlights a broad area of study in material science and opens hitherto unexplored
possibilities for developing sustainable solutions.
A vital component of this development is a dedication to environmental sustainability,
as demonstrated by the purposeful inclusion of natural fiber-reinforced polymer com-
posites in 3D printing, which is a significant paradigm shift. The combination of these
compositional ingredients with additive manufacturing techniques has created materials
with increased mechanical strength and improved biodegradability, substantially reducing
the carbon footprint associated with traditional manufacturing methods. Therefore, the
combination of natural fibers and polymers with additive manufacturing is a revolutionary
partnership that paves the way for the development of materials that are resilient to harsh
mechanical demands and consistently environmentally responsible. This revolutionary
finding highlights the potential of additive manufacturing to become a leader in the produc-
tion of sustainable materials, and it calls for more scholarly investigation and discussion in
the context of modern materials science, with the following specific focus points.
Material Diversity: Natural fibers such as jute, flax, hemp, and kenaf have been
successfully integrated into polymer matrices. These composites exhibit unique mechanical
and thermal properties, often on par with those of their synthetic counterparts.
Enhanced Properties: Advancements in fiber treatments and matrix formulations
have optimized fiber-matrix adhesion, leading to improved tensile strength, rigidity, and
durability of the composites.
Hybrid Systems: Recent studies have showcased the promise of hybrid composites,
which combine natural fibers with synthetic ones, resulting in materials that harness the
benefits of both.
Processing Techniques: Enhanced FFF methodologies specific to natural fiber com-
posites have been developed to address challenges like moisture absorption and ensure
uniform fiber distribution.
Natural fiber-reinforced polymer composites present a two-fold advantage. Envi-
ronmentally, they promote sustainability through biodegradability and reduced carbon
footprints. Economically, they offer the potential for cost reductions, leveraging abundantly
available natural resources. As industries globally grapple with mounting environmental
concerns, the adoption of such sustainable materials is both viable and imperative.
A new age of materials research has begun with FFF, especially concerning the enor-
mous potential of natural fiber-reinforced polymer composites. Innovative discoveries
have been made possible by the fusion of conventional materials science with cutting-edge
production techniques, leading to the development of composite materials that are both
strong and ecologically friendly.
The research presented in this publication makes a substantial contribution to the fields
of sustainable manufacturing and materials science. This paper provide helpful answers to
environmental problems and improves our knowledge of natural fiber-reinforced polymer
composites. Eco-friendly materials are essential to reducing the size of our carbon footprint
and protecting the environment for coming generations, and this research is a vital first
step toward a more sustainable and ecologically conscious industrial sector.
Author Contributions: Conceptualization, formal analysis, investigation, resources, data curation,

original draft preparation, writing and editing: I.A.K., C.R.C. and A.N.S.; Review: K.K. Visualization;
supervision: J.S.; project administration: J.S.; funding acquisition: J.S. All authors have read and
agreed to the published version of the manuscript.
Funding: This research is funded by the United States Department of Agriculture, grant number
2021-67021-34768.
Data Availability Statement: Data available with the corresponding author.
Acknowledgments: The authors are thankful to the University of Louisville and Bioproducts for
their valuable support and equipment provided during this research.
Conflicts of Interest: Author C.R.C. was employed by the company Bioproducts LLC. The remaining
authors declare that the research was conducted in the absence of any commercial or financial
relationships that could be construed as a potential conflict of interest.
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sustainability

Academic Editors: Andrzej Pacana

Sustainability 2023, 15, 16171. https://doi.org/10.3390/su152316171 https://www.mdpi.com/journal/sustainability

Sustainability 2023, 15, 16171 2 of 30

1.2. Properties of Natural Fibers

Sustainability 2023, 15, x FOR PEER REVIEW

Materials Compatibility and Natural Fiber Composites in FDM

2.2. Resin Based Stereolithography (SLA)

2.2.2. Formulation of Photopolymerizable Resin with Natural Fibers

2.3. Powder-Based Sintering and Deposition Processes

2.3.2. Binder Jetting (BJ)

2.3.3. Natural Fibers in SLS and BJ

3. Mechanical, Thermal, and Chemical Properties of Natural Fiber Composites

3. Mechanical, Thermal, and Chemical Properties of Natural Fiber Composites

Table 1. Mechanical Properties of Natural fibers.

Tensile Flexural Impact

3.2. Thermal Stability and Thermal Conductivity

Table 2. Material with temperature range for decomposition.

Material Temperature (◦ C) Weight Loss during Decomposition Reference

5. Applications of Natural Fiber-Reinforced Polymer Composites in Various Industries

5.1. Automotive Industry

5.2. Aerospace Industry

5.3. Medical Industry

5.4. Construction Industry

avenue of exploration. These natural fibers serve as a reinforcing component, enhancing

6. Challenges and Opportunities

The development of NFCs is gaining momentum and holds promise as a sustainable

Author Contributions: Conceptualization, formal analysis, investigation, resources, data curation,

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