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Progress Report On Natural Fiber Reinforced Composites: Review

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Review

Progress Report on Natural Fiber Reinforced


Composites

Omar Faruk,* Andrzej K. Bledzki, Hans-Peter Fink, Mohini Sain

This century has witnessed remarkable achievements in green technology in material science
through the development of natural fiber reinforced composites. The development of high
performance engineering products made from natural resources is increasing worldwide day
by day. There is increasing interest in materials demonstrating efficient use of renewable
resources. Nowadays, more than ever, companies are faced with opportunities and choices in
material innovations. Due to the challenges of petroleumbased products and the need to find
renewable solutions, more and more companies are looking at natural fiber composite
materials. The primary driving forces for new biocomposite materials are the cost of natural
fibers (currently priced at onethird of the cost of glass fiber or less), weight reduction (these
fibers are half the weight of glass fiber), recycling (natural fiber composites are easier to
recycle) and the desire for green products. This Review provides an overview of natural fiber
reinfocred composites focusing on natural fiber types and sources, processing methods,
modification of fibers, matrices (petrochemical and renewable), and their mechanical
performance. It also focuses on future research, recent developments and applications and
concludes with key issues that need to
be resolved. This article critically sum-
marizes the essential findings of the
mostly readily utilized reinforced natu-
ral fibers in polymeric composite mate-
rials and their performance from 2000
to 2013.

1. Introduction

Due to the increasing environmental awareness, natural


O. Faruk, A. K. Bledzki fiber composites are becoming more prevalent in use. In
Institut fuer Werkstofftechnik, Kunststoff- und Recyclingtechnik, addition, the materials’ relatively low cost and low density,
University of Kassel, Moenchebergstrasse 3 D-34109, Kassel, acceptable specific properties, ease of separation, enhanced
Germany energy recovery, CO2 neutrality, biodegradability, and
E-mail: o.faruk@utoronto.ca recyclable properties, have focused recent attention on
H.-P. Fink natural fiber use in composites. The materials which are
Fraunhofer Institute for Applied Polymer Research,
durable, reliable, lightweight, and with excellent mechani-
Geiselbergstrasse 69 D-14476, Potsdam-Golm, Germany
cal properties, that are significantly better than those of
A. K. Bledzki
Institute of Material Science and Engineering, West Pomeranian traditional materials are fueling the growing demand for
University of Technology, 19 Piastow Ave 70310, Szczecin, Poland natural fiber in various industries such as automotive,
O. Faruk, M. Sain building, and construction.
Centre for Biocomposites and Biomaterials Processing, University Recent study forecasts that in 2010, total global natural
of Toronto, 33 Willcocks Street, Toronto ON M5S 3B3, Canada fiber composite materials market shipments topped 430.7

Macromol. Mater. Eng. 2014, 299, 9–26


ß 2013 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim wileyonlinelibrary.com DOI: 10.1002/mame.201300008 9
O. Faruk et al.

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million pounds with a value of US$ 289.3 million and the Dr. Omar Faruk completed his B.S. and M.S. in
market is expected to grow to US$ 531.3 million in 2016 Chemistry at the University of Chittagong,
Bangladesh. With a DAAD (German Academic
with an 11% Compound Annual Growth Rate (CAGR) over
Exchange Service) scholarship, he joined at Univer-
the next 5 years.[1] The report also mentioned that sity of Kassel, Germany. He achieved his PhD in
increasing use of natural fiber composites in automotive Mechanical Engineering at 2005. He worked at the
applications is driving the market. Indeed, automotive is Department of Forestry, Michigan State University,
expected to remain the largest market through 2016. USA as a Visiting Research Associate from 2006 to
Several automotive components are now produced using 2009. Since 2010, he is working at the Centre for
Biocomposites and Biomaterials Processing, Uni-
natural composites, which are generally based on polypro- versity of Toronto, Canada.
pylene (PP) resin and fibers such as flax, hemp, kenaf, or
sisal. The automobile models, first in Europe and then in Prof. Andrzej Bledzki studied at the Technical
Universities in Poland and Germany. In 1988 he
North America, featured natural fiber reinforced thermo- took on the professorship of Polymer Processing in
sets and thermoplastics in door panels, package trays, seat the department of Mechanical Engineering at the
backs, and trunk liners. The application of natural fiber University of Kassel. From 1994 on, Prof. Bledzki
composites has increased and is gaining preference over was the head of the endowed professorship
glass fiber and carbon fiber. Because of natural fiber Polymer and Recycling Technology, which was
sponsored by industry and belonged to the
composites excel in most parameters except strength Institute of Materials Engineering of the University
(the strength of glass and carbon fiber is higher compared of Kassel. At present, he continues to work at the
to natural fiber) (Figure 1). The automotive industry’s University of Kassel in the position of a ‘‘Senior
adoption of natural fiber composites is led by price, weight Professor’’ and is also active at the West Pomera-
reduction, recycling, and marketing incentives rather than nian University of Technology, Szczecin, Poland.
Prof. Bledzki has been honoured numerous times.
technical demands. The range of products is no longer He was, inter alia, a scholarship holder of the
restricted to interior and non-structural components such German Humboldt-Foundation (1984/85).
as door panels or rear shelves. The report summarized that
Prof. Hans-Peter Fink studied physics at the
the major drivers of the natural fibers are raw material
University of Rostock and made his PhD thesis
source (natural fiber composites made with easily available (1977) on X-ray scattering of glasses. From 1975 to
renewable sources), properties (lighter weight, low energy 1992 he was employed at the Institute for Polymer
consumption, and low cost product), volatility in oil prices Chemistry in Teltow-Seehof, since 1992 he is
(impacts substitute materials markets and natural fiber working at the Fraunhofer Institute for Applied
Polymer Research in Potsdam-Golm. Since 2006 he
costs less), and environmental advantages with govern-
is the Director of that Institute. His research
ment supports. activities are centered on biopolymers, cellulose
Another trend is also remarkable that the concept of fibers, composites, and on different types of carbon
using biobased plastics as reinforced matrices for natural fibers. Additionally he holds adjunct professorships
fiber composites is gaining more and more approval day by for biopolymer science at the Universities of
Potsdam and Kassel.
day. The developments in emerging biobased plastics are
spectacular from a technological point of view and mirror Prof. Mohini Sain is Dean and professor at Faculty
their rapid growth in the market place. The average annual of Forestry, University of Toronto. He specializes in
advanced nancellulose technology, biocomposites
growth rate globally was 38% from 2003 to 2007. In the
and bio-nanocomposites. He is cross-appointed to
same period, the annual growth rate was as high as 48% in the Department of Chemical Engineering and
Europe. The worldwide capacity of biobased plastics is Applied Chemistry. He is a fellow of Royal Society
expected to increase from 0.36 million metric tonnes (2007) of Chemistry, UK. Besides, he is also an adjunct
to 2.33 million metric tonnes by 2013 and to 3.45 million professor of the Chemical Engineering Depart-
ments at the University of New Brunswick, Canada;
metric tonnes in 2020. The main product in terms of
King Abdulaziz University, Jeddah Saudi Arabia;
production volumes will be starch-based plastics, poly University of Guelph, Canada, University of Lulea,
(lactic acid) (PLA) and polyhydroxyalkanoate (PHA).[2] Sweden, Honorary Professor at Slovak Technical
The growing importance of natural fiber composites is University and Institute of Environmental Science
reflected by the increasing number of publications during at the University of Toronto, and collaborates with
American and European research institutes and
the recent years including reviews, patents, and books.
universities.
Satyanarayana et al.[3] represents the number of publica-
tions and patents on biodegradable lignocellulosic fiber
based composites (1995–2007) found in the ISI database by This paper is mainly the summary of recently published
entering the words ‘‘biodegradable, polymer, fiber’’ and it is comprehensive review paper,[4] which reviewed 525 papers
seen that after year 2000, the number of publications and on natural fibers in polymer composites from 2000 to
patents rose significantly (Figure 2). 2010 and additionally adds very recent results from 2010 to

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Progress Report on Natural Fiber Composites

www.mme-journal.de

Figure 1. Comparison between natural fiber, glass fiber, and carbon fiber.

till to date. This paper does not include natural fibers from kenaf fibers were extensively researched and employed in
animals (e.g., silk or wool) or cotton or man-made cellulosic different applications. But nowadays, abaca, pineapple leaf,
fibers and also excludes wood fiber. coir, oil plam, bagasse, bamboo, wheat straw, curaua, and
rice husk fibers are gaining interest and importance in both
research and applications due to their specific properties
2. Reinforcing Fibers and availability.
The properties of natural fibers differ among cited works,
The volatility in petroleum oil prices and their resources led because different fibers were used, different moisture
to an increased awareness and our inevitable dependence conditions were present, and different testing methods
on renewable resources has arisen. This century could were employed. The natural fiber reinforced polymer
be called the cellulosic century, because more and more composites performance depends on several factors,
renewable plant resources for products are being discov- including fibers chemical composition, crystalline cell
ered. It has been generally stated that natural fibers are dimensions, microfibrillar angle, defects, structure, physi-
renewable and sustainable, but they are in fact, neither. The cal properties, and mechanical properties, and also the
living plants are renewable and sustainable from which interaction of a fiber with the polymer.
the natural fibers are taken, but not the fibers themselves. The hydrophilic nature of fibers is a major problem for
There are thousands of different fibers in the world and all natural fibers if used as reinforcement in plastics.
in fact only few of these fibers have been studied. Most The range of the characteristic values, as one of the
research has been carried out to study the potential use of drawbacks for all natural products, is remarkably higher
natural fibers for technical applications and this paper has than those of glass-fibers, which can be explained by
only covered the most widely studied and used natural differences in the fiber structure due to the overall
fibers in reinforced composites materials. Among the most environment conditions during growth. The physical
popular natural fibers; flax, jute, hemp, sisal, ramie, and properties of each natural fiber are critical, and include
the fiber dimensions, defects, strength,
and structure. There are several physical
properties that are important to know
about for each natural fiber before that
fiber can be used to reach its highest
potential. A high aspect ratio (length/
width) is very important in cellulose-
based fiber composites as it gives an
indication of possible strength proper-
ties. The fiber strength can be an impor-
tant factor in selecting a specific natural
fiber for a specific application. Fiber
dimensions, defects, strength, variability,
crystallinity, and structure must be taken
into consideration.
Dittenber and GangaRao[5] compiled a
Figure 2. Overview of publications and patents on biodegradable lignocellulosic fiber- cost per weight comparison between
based composites from 1995–2007. natural and glass fibers from several

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radiation. In addition, there are several factors that can


influence fiber quality in each stage, and there are several
different stages of production, as shown in Table 2.[5] The
fiber quality is affected by the plant species, the crop
production, the location, and the climate at the plant
growth stage.
Baillie et al.[7] illustrated the properties of natural fibers
(strength, thermal degradation, biological degradation,
moisture absorption, and UV degradation) to their depen-
dence on chemical constituents of the natural fibers
(Figure 5). In all plant-based fibers, the basic chemical
Figure 3. Cost per weight comparison between glass and natural structure of cellulose is similar but they have different
fibers. degrees of polymerization. The cell geometry of each type of
celluloses varies with the fibers and these factors contribute
published papers shown in Figure 3. The variation of to the diverse properties of the natural fiber.
price for natural and glass fibers are depend on sources
of geographic area.
It is also studied the comparison between the specific 3. Modification of Natural Fibers
modulus of glass and natural fibers, a favorable comparison
for several types of natural fibers, and additionally the wide The main disadvantages of natural fibers in respective
range each type of fiber may have for the specific modulus composites are the poor compatibility between fiber and
obtained from published stiffness and density values matrix and their relatively high moisture absorption.
(Figure 4). It is mentioned that most used natural fibers Therefore, natural fiber modifications are considered
potential specific modulus are higher than glass fibers. leading to a change of the fiber surface properties to
There are many positive reasons to use natural fibers as improve their adhesion with different matrices. An
reinforcing component in polymers, at the same time there exemplary strength and stiffness could be achieved with
are also several disadvantages, when preparing composite a strong interface that is very brittle in nature with easy
materials with these fibers. Aragones[6] summarized the crack propagation through the matrix and fiber. The
pros and cons of selection of natural fibers for composite efficiency of stress transfer from the matrix to the fiber
materials (Table 1). could be reduced with a weaker interface.
The variation of properties of natural fiber relates to the Extensive research was carried out and reported in the
lack of consistency of fiber qualities, which related to the literature, showing the importance of the interface and
location and time of harvest, processing conditions, as well the influence of various types of surface modifications
as their sensitivity to temperature, moisture, and UV on the physical and mechanical properties of natural
fiber reinforced composites. The observed
trend indicate a preference for the
chemical modification (alkaline, silane,
acetylation, benzoylation, acrylation and
acrylonitrile grafting, maleated coupling,
permanganate, peroxide, and isocyanate
treatment) compared to physical modifi-
cation (corona and plasma treatment).
It has also been shown that maleated
and silane treatment is becoming
a choice method due to beneficial
results.[8–10] Additive suppliers improved
the additives with higher amounts of
anhydride functional groups than previ-
ous grades (used in 1980s and 1990s),
which create more sites for chemical
links, resulting in significant perfor-
mance improvement at low additive
Figure 4. Comparison of potential specific modulus values and ranges between natural contents. Using coupling agents reduced
fibers and glass fibers. the water absorption of the composites

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Progress Report on Natural Fiber Composites

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Table 1. Pros and cons of selection of natural fibers for composite material.

Pros Cons

Physical- Low density, thus low weight Fibers absorb moisture that causes swelling
mechanical Higher specific strength and stiffness than glass Lower strength properties than glass fiber
composites, particularly impact strength
Good thermal and acoustic insulating properties Odor generation due to degradation process
Processing Non-abrasive effect aver screws and other The maximum processing temperatures are
metaLtic parts limited, especially in relation to glass fiber
Nan-harmful processing, no tool wear and no Some fibers need to be pelletized in order to
skin irritation increase the apparent density
Environmental It is a renewable resource, and is therefore an Relatively low durability, due to fungus
inexhaustible supply attack, weathering, etc.
Production energy is only 1/3 of that for glass Relatively large price fluctuations due to
fibers harvest results or agricultural politics
The amount of CO2 that the plants absorb Variable quality, depending on unpredictable
during their growth is the same as that given off influences such as weather
when they are decomposed

but has not resulted in decreased long-term performance. performance. In addition, enzyme technology could be cost
The use of enzyme technology is becoming increasingly effective, improved product quality compared to mostly
substantial for the processing of natural fibers. Currently, use maleated and silane modification.
the use of enzymes in the field of textile and natural
fiber modification is also rapidly increasing.[11] A major
reason for embracing this technology is the fact that 4. Matrices for Natural Fiber Composites
the application of enzymes is environmentally friendly. The
reactions catalyzed are very specific and have a focused The composites’ shape, surface appearance, environmental
tolerance, and overall durability are dominated by the
Table 2. Factors effecting fiber quality at various stages of matrix while the fibrous reinforcement carries most of the
natural fiber production. structural loads, thus providing macroscopic stiffness and
strength. The polymer market is dominated by commodity
Stage Factors effecting fiber quality plastics with 80% consuming materials based on non-re-
newable petroleum resources. Governments, companies,
Plant growth Species of plant
and scientists are driven to find an alternative matrix to the
Crop cultivation conventional petroleum-based matrix through public
Crop location awareness of the environment, climate change, and limited
Fiber location in plant
Local climate
Harvesting stage Fiber ripeness, which effects:
-Cell wall thickness
-Coarseness of fibers
-Adherence between fibers
and surrounding structure
Fiber extraction stage Decortication process
Type of retting method
Supply stage Transportation conditions
Storage conditions
Figure 5. Properties of cellulose fibers and their dependence on
Age of fiber chemical constituents.

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fossil fuel resources. Therefore biobased plastics, which (ii) Some bioplastics have a lesser performance factor
consist of renewable resources, have experienced a renais- when compared to petroleum-based plastics
sance in the past decades. (iii) The manufacturing process of bioplastics still relies
on petroleum based energy
(iv) Studies have shown that various bioplastics
4.1. Petrochemical Based
manufacturing varies in its environmental impact
The effects of the incorporation of natural fibers in (v) There are concerns that sustainable bioplastics will
petrochemical-based thermoplastics and thermoset ma- upset existing recycling methods
trixes were extensively studied. PP, polyethylene (PE), (vi) Since the production of bioplastics as market is
polystyrene (PS), and polyvinyl chloride (PVC) were used for fairly new, the manufacturing price tag is not as cost
the thermoplastic matrixes. Polyester, epoxy resin, phenol effective as the fossil fuel plastic production; this is
formaldehyde, and vinyl esters were used for the thermoset based on existing price of oil.
matrices and are reportedly the most widely used matrices
for natural fiber reinforced polymer composites. The effects of reinforcing polylactide (PLA) and poly(3-
hydroxybutyrate-co-3-hydroxyvalerate) (PHBV) bio-
polymers and petrochemical PP on the mechanical
4.2. Biobased
performance of man-made cellulose, abaca and jute fiber
Many new polymers were developed from renewable composites were studied.[12] Figure 6 illustrates that
resources, such as starch, which is a naturally occurring biobased polymer composites exhibited higher tensile
polymer that was re-discovered as a plastic material. Others strength and modulus compared to petrochemical-based
are PLA that can be produced via lactic acid from composites. It is also seen that PLA based man-made
fermentable sugar and PHAs, which can be produced from cellulose, abaca and jute fiber composites showed
vegetable oils next to other biobased feed stocks and these higher properties in comparison with PHBV and PP-
are the mostly used biobased polymers in natural fiber based composites.
reinforced composites. Other biobased polymers such Bledzki et al.[13] investigated the tensile properties of
as soy-based biodegradable resin (polyol derived from mostly used petroleum based polymer PP and biobased
soybean oil), polycaprolactone (PCL) and polybutylene
succinate (PBS) is also studied with natural fibers.
Though biobased polymers experiencing positive accep-
tance in composites area, but biobased polymers have their
own advantages as well as drawbacks. The pro and contras
of using biobased polymers are summarized below.

4.2.1. Advantages

(i) Sustainable bioplastics will help to reduce our


dependency on oil
(ii) Sustainable bioplastics are made from renewable
sources
(iii) Many of the bioplastics are biodegradable
(iv) Bioplastics are used and promoted for recycled
products
(v) Product costs are getting more competitive due to the
increased oil prices
(vi) Continued research will lead to improved production
techniques and products that are more environment
friendly.

4.2.2. Disadvantages
Figure 6. a) Tensile strength and b) tensile modulus of PLA, PHBV,
(i) There is a limited shelf life for some of the sustainable and PP composites with man-made cellulose, abaca, and jute
bioplastics fibers.

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Progress Report on Natural Fiber Composites

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Figure 7. Tensile properties of abaca reinforced PP, PLA, and PA 6.10 composites.

polymer PLA and PA 6.10 with natural fiber abaca day, there is great interest in developing natural fiber
(Figure 7). The biobased polymer composites clearly composites with a thermoplastic rather than thermoset
show better tensile strength and modulus than the matrix, mainly due to their recyclability. Also the choice of
petroleum-based PP abaca composites. In comparison a thermoplastic matrix fits well within the eco-theme of
between biobased PLA and PA 6.10, it is observed that biocomposites, but there are some important limitations
PLA exhibits higher strength and modulus compared to on the recyclability and mechanical performance of
PA-abaca composites. thermoplastics. Generally, the mechanical properties of
Kim et al.[14] performed the total volatile organic thermosets are higher than the thermoplastics (lower
compound (TVOC) emissions from natural fiber (pineapple modulus and strength). In addition, a dramatic loss in
flour and cassava flour) reinforced biopolymer (PLA and properties is observed above the glass transition temper-
PBS) composites and compared to mostly used synthetic ature, which leads to decrease in other thermally sensitive
polymer PE and PP (Figure 8). It is observed that natural fiber properties such as creep resistance. On the contrary,
reinforced PLA and PBS composites exhibit significantly thermoplastics show greater fracture toughness than
lower odor emissions, which is favorable for automotive thermosets and thus are more useful in resisting impact
interior components. loads. Another remarkable change was the introduction of
Ganster and Fink reviewed[15] the PLA for the production biopolymers in recent years with the aim of decreasing
of bio- and nanocomposites. Attempts to improve PLA reliance on petroleum-based thermoplastics. The avail-
properties by reinforcing with lignocellulosic fibers ability and outstanding mechanical properties of bio-
(both wood and natural fibers) and man-made cellulosic polymer PLA has led to this matrix system being one of
fibers (rayon) are outlined. The mechanical properties of the most thoroughly investigated in the biocomposites
composites obtained from melt compounding are mainly research area.
considered, because this is the most industrially relevant
properties.
Till to date, the petroleum derived thermoplastics PP 5. Processing Techniques
and PE are the two most commonly employed thermo-
plastics in natural fiber reinforced composites. Day by Generally, natural fiber reinforced plastic composites
are manufactured by using traditional manufacturing
techniques (designed for conventional fiber reinforced
polymer composites and thermoplastics). The processing
techniques include compounding, mixing, extrusion, injec-
tion molding, compression molding, LFT-D are suitable
and investigated for natural fiber reinforced thermoplastic
composites. On the other side, resin transfer molding
(RTM) and SMC are implemented with thermosets
matrix. Besides these processes, nowadays thermosets
compression molding and pultrusion are investigated with
natural fiber composites. Till to date, above mentioned
techniques have been well developed and accumulated
Figure 8. Emission factor for the PLA and PBS-natural fiber experience has proofed their successability for producing
composites, LDPE and PP (PLA-P: PLA with pineapple flour, PLA- composites with controllable quality. Innovative techno-
C: PLA with cassava flour, similar for PBS). logies and process solutions should be intensively

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researched to get the high strength engineering composites Based on final product, suitable manufacturing processes
required by new applications area. must be utilized to transform the materials to the final
There are some factors; such as fiber type, fiber shape without causing any defect of products. The product
content, fiber orientation, moisture content of fiber, size is a dominating factor for the preliminary assessment
which influence significantly the processing of natural on a suitable type of manufacturing processes to be used.
fiber composites as well as the properties of final From the literature review, it is observed that for small to
product. Therefore to select a suitable process to fabricate medium sized components, injection, and compression
natural fiber composites, design, and manufacturing moldings are preferred due to their simplicity and fast
engineers would mainly focus on numbers of criteria processing cycle. In the case of large structures, they are
including desired properties, size, and shape of resultant typically manufactured by open molding.
composites, processing characteristics of raw materials
(both fibers and polymers: biobased or petroleum based),
the production speed and the manufacturing cost. In 6. Performance of Natural Fiber Composites
addition, based on processing techniques, semi-finished
product manufacturing; mat production, slivers, fiber Tensile, flexural, and impact properties are the most
yarns, fiber preparation (opening, mixing, and carding), commonly investigated mechanical properties of natural
and granule production are the important steps, which fiber reinforced plastic composites. Impact strength is
should be taken in account to production of natural one of the undesirable weak points of these materials
fiber composites. in terms of mechanical performance. Besides these
The influence of compounding processes (mixer- tensile, flexural, and impact properties, the long-term
injection molding, mixer-compression molding, and direct performance (creep behavior), dynamic mechanical
compression molding) on the mechanical properties of the behavior, compressive properties are also investigated
abaca fiber reinforced PP composites was investigated.[16] for natural fiber composites.
It represents that mixer-injection molding processes lead Ramesh et al.[17] has developed sisal-jute-glass fiber
to higher tensile and flexural strength values compared reinforced polyester composites and compared their
to the other processes. It is also notable that direct mechanical properties with sisal-glass fiber and jute-
compression process exhibits higher strengths compared glass fiber reinforced polyester composites. It is seen
to mixer-compression process. It seems that due to the that the incorporation of sisal and jute fiber with glass
agglomeration, the fiber breaks into lower length what fiber can improve the properties and used as an alternate
plays a role in the compression molding process. It is material for glass fiber reinforced polymer composites.
also observed that after agglomeration (mixing) and Figure 9 illustrates the load versus the displacement
injection molding process, composites showed very graph for above-mentioned composites. It is observed
significant higher odor values compared to other process- that the displacement increases with the increase of
es. Compression molding process showed relatively load and above 14.2 mm displacement, there is a breaking
lower odor concentrations, which is favorable for exists. Based on the interfacial properties, internal cracks,
the automotive sector. It seems that injection molding and internal structure of the composites, it is indicated
process decomposes the composite materials more than that sisal-jute-glass fiber reinforced composites showed
compression molding process what results in higher better performance than the other type of composites
odor concentration. tested.
To date, injection molding, extrusion, compression
molding, sheet molding, and RTM are the major
manufacturing processes for natural fiber reinforced
plastic composites. But new downstream and auxiliary
equipment has been designed. Such as: unique heating
and single or dual venting systems for in-line drying,
high-intensity spray-cooling tanks, a variety of new
configurations of feeding (gravimetric or vertical crammer)
systems, combinations of extrusion-injection molding
or extrusion-compression molding as well as screw, die,
and mold design. Although the majority of natural
fiber composites are produced today by the processes
mentioned above, the manufacturers are improving
the feasibility of using other processes like pultrusion Figure 9. Comparison of load vs. displacement of sisal-glass fiber,
and so on. jute-glass fiber, and sisal-jute-glass fiber reinforced composites.

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Progress Report on Natural Fiber Composites

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Figure 10. Flexural modulus of the PLA and PHB composites with Figure 11. Shore D hardness of pure PLA and PHB, and their
lyocell and kenaf fibers (Box-whisker diagram with confidence composites (Box-whisker diagram with confidence intervals).
intervals, different letters mean significant differences between
the test samples,  means normal distributed).
compression molded natural fiber composites such as
other kenaf, sisal, and coir reinforced thermoplastics. With
Kenaf and lyocell (man-made cellulose) fiber reinforced the aid of the elastic modulus data, it was also possible to
PLA and poly(3-hydroxybutyrate) (PHB) composites were compare the economic benefits of using kenaf composites
produced by compression molding process.[18] The use of instead of other natural fibers and E-glass. The manufac-
different matrices leads to variable composite character- tured kenaf maleated PP composites have a higher
istics and provides a comparison of the mechanical modulus/cost than sisal, coir, and even E-glass (Figure 12).
characteristics of compression-molded 30% lyocell and Thus, they provide an option for replacing existing
40% kenaf fiber reinforced PLA and PHB. The tensile and materials with a higher strength, lower cost alternative
flexural test showed that 30% lyocell-PLA composites that is environmentally friendly.
reached the highest tensile and flexural strength with 89 Hybrid of kenaf/glass fiber reinforced epoxy composites
and 148 N  mm2, respectively. The 30% lyocell-PLA com- was manufactured to enhance the desired mechanical
posites also exhibited the highest tensile modulus with properties for car bumper beams as automotive structural
9.3 GPa. The highest flexural modulus was measured components.[20] Hybrid composites, which is fabricated
for 40% kenaf-PHB composites with 7.1 GPa (Figure 10). by modified SMC method is tested and compared with
The best impact strength was observed for lyocell-PHB a typical car bumper beam material (GMT-glass mat
composites with 70 kJ  m2, whereas lyocell-PLA compo- thermoplastic). Tensile strength and modulus of hybrid
sites exhibited with 52 kJ  m2. The investigation of the composites exhibited higher values than typical car
Shore D hardness resulted in a higher
value for the PLA matrix with 81.5 and
PHB achieved a hardness of 67.5. Due to
the addition of fiber, the Shore D hardness
increased up to 83.6 for lyocell-PLA
composites and 73.1 for kenaf-
PHB composites (Figure 11). Density
measurements showed lower densities
for the composites with higher fiber loads
(kenaf-PLA and kenaf-PHB) in compari-
son to the theoretical density, which
relates to a higher proportion of air
inclusion in the composites. Thus results
a negative effect to the mechanical
composite characteristics.
Zampaloni et al.[19] found that com-
pression molded kenaf-PP composites
have superior tensile and flexural
strength when compared to other Figure 12. Comparison of modulus/cost for various natural fibers and glass fibers.

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Sobczak et al.[22] analyzed the mechanical performance


profiles of various natural fiber reinforced PP composites
considering them for a variety of potential applications,
which compete with mineral reinforced (talc), short glass
fiber (sgf), long glass fiber (lgf), and short carbon fiber (scf)
reinforced PP property profiles of the latter materials are
also included in the analysis. Figure 15 illustrated various
natural fiber composites tensile strength and modulus
comparing with talc, glass fiber, carbon fiber, and even with
wood fiber reinforced composites. Natural fiber composites
outperform PP-talc composites. Glass fiber composites
(both sgf and lgf) clearly showed higher performance than
natural fiber composite. Unusually, short carbon fiber
composites for both in scientific investigations and for
commercial products fall significantly, which might be
Figure 13. Tensile properties of hybrid (kenaf/glass) composites short of rule of mixture.
and GMT composites.
To improve their performance to the desired level, still
much work is to be done considering fiber processing, non-
bumper beam (Figure 13), which led to the potential linear behavior, fiber-matrix adhesion, fiber dispersion,
utilization of hybrid natural fiber in some car structural composite manufacturing with optimized processing
components such as bumper beams. parameters.
Alves et al.[21] demonstrated the use of natural fiber
composites, which is produced in developing countries,
have presented several social, environmental, and eco- 7. Developments and Applications
nomical advantages to design green automotive compo-
nents. A structural frontal bonnet of an off road vehicle There are several major areas of interest behind the
were manufactured with jute fibers to a replacement development of natural fiber composites, which provide
of glass fibers and through LCA method demonstrates the potential economic impacts, environmental impacts,
the possibility to use natural fibers considering social, and the ability of natural fiber composite to meet social,
environmental, economical, and technical advantages economic, and material needs all over the world. The
(Figure 14). It is clearly observed that jute composites advanced natural fiber reinforced polymer composite
related to the four aspects, present the better overview contributes to enhancing the development of biocompo-
performance than glass composites except technical sites in regards of performance and sustainability. There
aspects. are numerous research is going on all over the world, which
reflects in recent enormous review papers focusing on
overall performance of natural fiber composites,[23–27]
influence of natural fibers on biodegradable polymers
and their biodegradation,[28–31] chemical treatments of
natural fibers and performance of chemically treated
natural fiber composites,[32–35] mechanical and physical
properties of natural fiber composites,[36] tensile proper-
ties,[37] tribology properties,[38] flame retardancy,[39] me-
chanical behavior of natural fiber woven composites,[40]
natural fiber hybrid composites,[41] aspects of fatigue
analysis of natural fiber composites,[42] and applications
in automotive sector.[43] There are review papers also
published on individual natural fibers and their suitability
in composite materials, such as abaca/banana fiber,[44]
oil palm fiber,[45] oil palm empty fruit bunch,[46] kenaf
fiber,[47] hemp fiber,[48] bamboo fiber,[49] coir fiber,[50]
bagasse fiber,[51] and cellulosic nanofibers.[52–54] Summer-
scales et al. has published a series of review papers on
Figure 14. Comparison between jute and glass composites based bast fibers and their composites with illustrating the
bonnet’s aspects. natural fibers as reinforcements,[55] influence and their

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commercial construction and consumer


goods, composites need to achieve high-
quality performance, serviceability, du-
rability, and reliability standards.
Besides automotive sector, recent re-
search is also focusing on natural fiber
composites in construction sector. Build-
ing materials based on renewable resour-
ces like natural fibers and their reinforce-
ment in cement based materials are
evaluated. Reinforcement suitability
of jute fiber,[59–61] coir fiber,[62–64] corn
stalk,[65] flax fiber,[66] and hemp fiber[67]
were investigated in fiber cement
composites. Pacheco-Torgal and Jalali
reviewed the natural fiber reinforcement
in cementitious building materials focus-
ing on fiber characteristics, properties
and the description of the treatments
that improve their performance, compat-
ibility between the fibers and the cement
matrix, influence of natural fiber on
cement properties, and the properties
and durability performance of cementi-
tious materials reinforced with natural
fibers.[68]
Kalyankar and Uddin[69–71] studied the
manufacturing and structural feasibility
of natural fiber-reinforced polymeric
structural insulated panels for panelized
construction, mainly focuses on the
manufacturing feasibility and structural
characterization of natural fiber rein-
forced structural insulated panels (NSIPs)
using jute fiber reinforced polypropylene
(NFRP) laminates as skin. The natural
fibers were bleached before their use as
reinforcement.
Figure 15. Ashby plot presenting the tensile strength vs. the Young’s modulus of various
Another major advancement lies with-
PP compounds.
in the establishment of nanotechnology
(i.e., reinforcing as well as producing
nanocrystalline cellulose from natural
performance in composite materials,[56] and statistical fibers). Natural fibers consist of approximately 30–40%
models which already have been applied to natural fiber cellulose and about half of that is crystalline cellulose. The
reinforcements for composite systems.[57] nanocrystalline cellulose may be only one-tenth as strong
Last 13 years natural fiber composites have created as carbon nanotubes but it costs 50–1 000 times less to
substantial commercial markets for value-added products produce.
especially in automotive sector. The automotive compo- Zainuddin et al.[72] treated kenaf fibers with NaOH,
nents with natural fiber reinforced composites can be bleached with sodium chlorite and acetic buffer solution,
expected to increase steadily with increased model and subsequently acid hydrolyzed to obtain cellulose
penetration. All major vehicle manufacturers around the nanocrystals (CNCs). CNCs obtained after acid hydrolysis
world now use natural fiber composites in various were characterized by TEM images (Figure 16). It is seen
applications such as those listed in Table 3.[58] However, that CNCs are in needle-like shapes and some were
in order to be able to expand into other markets, such as still agglomerated. It is found that the diameter of

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Table 3. Automotive models, manufacturers, and components using natural fiber composites.

Model Manufacturer Components

A2, A3, A4, A4 Avant, A6, A8, Audi Seat back, side and back door panel, boot lining, hat
Roadstar, Coupe rack, spare tire lining
C5 Citroen Interior door paneling
3, 5, 7 series BMW Door panels, headliner panel, boot-lining, seat back,
noise insulation panels, molded foot well linings
Eco Elise Lotus Body panels, spoiler, seats, interior carpets
Punto, Brava, Marea, Alfa Fiat Door panel
Romeo 146, 156
Astra, Vectra, Zafira Opel Instrumental panel, headliner panel, door panels,
pillar cover panel
406 Peugeot Front and rear door panels
2000 and others Rover Insulation, rear storage shelf/panel
Raum, Brevis, Harrier, Celsior Toyota Door panels, seat backs, floor mats, spare tire cover
Golf A4, Passat Variant, Bora Volkswagen Door panel, seat back, boot-lid finish panel, boot-liner
Space star, Colt Mitsubishi Cargo area floor, door panels, instrumental panels
Clio, Twingo Renault Rear parcel shelf
Mercedes A, C, E, S class, Trucks, Daimler-Benz Door panels, windshield/dashboard, business table,
EvoBus (exterior) piller cover panel, glove box, instrumental panel
support, insulation, molding rod/apertures,
seat backrest panel, trunk panel, seat surface/backrest,
internal engine cover, engine insulation, sun visor,
bumper, wheel box, roof cover
Pilot Honda Cargo area
C70, V70 Volvo Seat padding, natural foams, cargo floor tray
Cadillac Deville, Chevrolet General Motors Seat backs, cargo area floor
TrailBlazer
L3000 Saturn Package trays and door panel
Mondeo CD 162, Focus, freestar Ford Floor trays, door panels, B-piller, boot liner

individual CNCs was 12  3.4 nm and the length was the highest stiffness compared to other treated kenaf fiber
between 70 and 190 nm with an aspect ratio (L/D) of 13.2. reinforced composites and it was 326.1 MPa at 6 wt.% CNCs
The above-mentioned CNCs from kenaf fiber were then content. It is also notable that aggregates of CNCs in the
mixed with cassava starch to develop biocomposites using matrix contributed to this phenomenon and hence
a solution casting method. Figure 17 represents the tensile restricted fiber content reinforcement.
modulus values as a function of reinforced fiber content. It is Eichhorn et al.[53] provided a comprehensive overview of
observed a clear tendency of increasing stiffness for all of recent progress made in the area of cellulose nanofiber
the composites with increasing fiber content. Generally, the and their composites. The isolation methods of cellulosic
significant increase was attributed to the similarity nanofibers (nanowhiskers, nanofibrils) with details of
between the chemical structures of cellulose and starch. their structure are given. The processing and characteriza-
An increasing trend in the elastic modulus of the films was tion of cellulose nanocomposites and new developments
observed with the addition of nanocellulose regardless in the area, with particular emphasis on applications
nanocellulose content. CNCs reinforced composites showed were described. The review paper highlighted the use

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materials and their boundary conditions are evaluated


(Figure 19). A frontal bonnet of vehicle were manufactured
with jute fiber reinforced composites and its boundary
conditions is the entire life cycle of the bonnets made
of composite materials and their influence for whole
vehicle, from the extraction of raw materials, over
production processes, and the use phase to the end of
life of the vehicle. The boundaries of LCA include all of
needed transports as well as the infrastructure to apply
the treatments at jute fibers and to produce the bonnets
even to dispose them.[21]
Le Duigou et al.[73] investigated the environmental
impact and simplified LCA of flax fiber reinforced PLA
composites and compared their properties to conventional
glass fiber reinforced polyester composites. Their analysis
was based on four steps: Goal and Scope definition, Life
cycle Inventory (LCI), Life Cycle Impact Assessment (LCIA),
and Interpretation. The evaluation of greenhouse gas
emissions in kg of CO2 equivalent are lower for the
biocomposite as carbon dioxide is trapped during photo-
synthesis (for both flax fibers and the maize used to
produce PLLA). The environmental indicators were calcu-
lated with the CML 2000 method and it is illustrated
that the biocomposites appear to be an attractive alterna-
tive to conventional glass/polyester composites. The
natural fiber reinforced composites reduced the majority
of the environmental impact indicators, such as global
warming (70%), photochemical oxidation (60%), and
human toxicity (80%). On the contrary, natural fiber
Figure 16. TEM micrographs of CNCs from kenaf under different composites result in a transfer of pollution from global
magnifications: a) 13 000 and b) 35 000.
to local impacts [eutrophication (þ50%) and fresh water
toxicity (þ20%)].
of cellulose nanowhiskers for shape memory nanocompo- The application of life cycle assessment (LCA) methodo-
sites, analysis of the interfacial properties of cellulose logy in order to explore the possibility of improving
nanowhisker and nanofibril-based composites. It also the eco efficiency of glass fiber composite materials by
covered the applications and new advances of cellulose replacing part of the glass fibers with hemp mats were
nanofibers to reinforce adhesives, to make optically investigated.[74] Besides the exploration of eco-efficiency
transparent paper for electronic displays, to create DNA- of biocomposites, it is also provided the LCI data on
hybrid materials, to generate hierarchical composites composites. LCA was performed of two different elbow-
and for use in foams, aerogels, and starch nanocomposites fittings made of glass fiber/epoxy vinylester resin
and the use of all-cellulose nanocomposites for enhanced composite and hybrid (glass fiber-hemp)/vinylester resin
coupling between matrix and fiber. composite considering human health, ecosystem quality,
Sustainability assessment methodology, such as Life resources, global energy requirement, global warming
Cycle Analysis (LCA) has been developed to evaluate the point, and agricultural land occupation and significant
environmental effect of parameters such as raw materials, environmental benefits of using hemp mats were found.
energy consumption, and ultimate disposal or recycling According to their Life Cycle Costing (LCC), which was
characteristics. Several researchers have attempted to carried out from cradle to grave, the material costs
quantify the environmental improvements natural fibers reduction was significant for the hemp fiber reinforced
offer over synthetic fibers. Akil et al.[47] represented the elbow formulation.
life cycle of all biocomposites (Figure 18) and for further Figueirõdo et al.[75] investigated the life cycle assess-
assessment of natural fiber composites, LCA should be ment of cellulose nanowhiskers which was extracted
done for all products. from unripe coconut fiber and cotton fibers. Nowadays
Natural fiber composite’s LCA was performed to it is really important to know the LCA of cellulosic
find environmental impacts related to the composite nanofibers, which needs many chemical processes to

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suggested further research to improve


the environmental performance of nano-
fiber production systems before scaling
up the results from the laboratory to
industry with emphasize focusing
on improving yield efficiency, reducing
energy and water use during the extrac-
tion of nanowhiskers, and recovering
substances from effluents possessing
market value.
As technology improves for biocom-
posites reinforced with natural fibers to
provide enhanced material and product
characteristics, the products will be-
come more diverse and enter markets
that as of yet are unexplored. Today
natural fiber reinforced biocomposites
are found extensively in automotive
sectors. By the time, natural fiber
composite materials and associated
design methods are sufficiently mature
to allow their widespread use, e.g., as
construction materials. The develop-
ment of methods, systems, and stand-
ards could see natural fiber composite
materials at a distinct advantage over
traditional materials. There is a signifi-
cant research effort underway to
develop natural fiber composite materials
and explore their use as construction
materials, especially for load bearing
applications.

8. Focusing on Future
Research
Figure 17. Effects of fiber treatments on tensile modulus of kenaf fiber reinforced starch
composites.
In the future, natural fiber composites
will see increased use in structural
extract the nanofibers from different natural fibers. applications. Various other applications depend on their
This study focused on the environmental performance further improvements. But there are still a number of
of cellulose nanowhiskers production processes and the problems that have to be solved before these composites
product systems encompassed fiber, electricity, and become fully competitive with synthetic fiber composites.
chemical production processes. LCA was performed con- Natural fiber composites are sustainable and could be fully
sidering the environmental aspects: such as, energy, recyclable, but could be more expensive if fully biobased
water, and emissions present in liquid effluents [chemical and biodegradable and they are extremely sensitive to
oxygen demand (COD), biological oxygen demand moisture and temperature. If a proper matrix is used,
(BOD), total nitrogen, nitrate, total phosphorus, phenols, natural fiber composites could be 100% biodegradable,
furfural, and hydroxymethylfurfural (HMF)] and life but their biodegradation can be difficult to control.
cycle impact was also assessed for climate change, Natural fiber composites exhibit good specific properties,
water depletion, eutrophication, and human toxicity but there is high variability in their properties. Their
impact categories. Figure 20 illustrated the system weaknesses can and will be overcome with the develop-
boundary of extraction nanowhiskers from unripe ment of more advanced processing of natural fibers
coconut fiber based on their production process. They and their composites. However, fully environmental

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Figure 18. Life cycle of natural fiber composites.

superiority of natural fiber composites compared to (iii) Overcome moisture absorption related to long term
synthetic fiber composites is still questionable because durability (temperature, humidity, and UV radia-
of their relatively excessive processing requirements, tion), fiber and matrix modification, fire resistance,
which in turn consume more energy. Therefore, future properties and durability, hybridization, and
research should be focused on the following issues: manufacturing and processing optimization subject
to specific final products
(i) Fiber extraction should provide more elemental (iv) Biodegradability and life cycle assessment (LCA)
and technical fibers for effective embodiment into should be thoroughly researched
composite matrix to avoid the fiber variability (v) Composites, matrix (thermoplastic and thermosets),
(ii) The improvement of the interfacial properties additives, coupling agents made from renewable
between the fiber and the matrix should be resources should be developed. Search for new and
achieved improved biopolymers to replace petroleum-based

Figure 19. Boundary conditions of the LCA of a frontal bonnet (manufactured with jute fiber reinforced composites).

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Figure 20. System boundary of extraction of cellulosic nanowhiskers from unripe coconut fibers.

polymers should be continued to fully meet with biodegradation, and volatile organic compounds and
future environmental goals even flame resistance. The use of nanocrystalline cellulose
(vi) Multidisciplinary research, involving agricultural, is being explored for a variety of uses since it is stronger
biotechnology, polymer, and composite manufactur- than steel and stiffer than aluminum. Nanocrystalline
ing aspects should be carried out cellulose reinforced composites could soon provide ad-
(vii) Composite manufacturing technologies should be vanced performance, durability, value, service-life, and
developed and adopted with new biobased polymer utility while at the same time being a fully sustainable
(viii) Current trend and expansion of nanocomposites, technology.
extensively research could be focused on cellulosic Green composite materials could be the material
nanofibers as well as inorganic nanofillers (e.g., revolution of this century focusing on sustainability,
nanoclays) incorporation in natural fiber reinforced ‘‘cradle-to-grave’’ design, industrial ecology, eco-efficiency,
composite materials. and green chemistry, which may guide the development of
a new generation of green materials. The success of natural
fiber reinforced polymeric composites will be dependent
9. Conclusion upon on appropriate processing techniques, modification
of fibers to improve the adhesion between fiber and the
The uses of natural fiber as reinforcing agent in polymeric biopolymer, matrix modification and after treatment to
composites were reviewed from the point of view of improve performance as well as long-term durability and
status, structure, performance, surface treatments, and fire retardancy.
applications. The field of natural fiber reinforced compo-
sites research has experienced an explosion of interest,
particularly with regard to its comparable properties to Received: January 7, 2013; Revised: March 19, 2013; Published
glass fibers within composites materials. It should be online: June 19, 2013; DOI: 10.1002/mame.201300008
mentioned that natural fiber reinforced composite materi-
Keywords: biocomposites; biopolymer; natural fiber; thermoplas-
als are gaining increasing importance in automotive, tic; thermosets
construction, aerospace, and other industrial applications
due to their lighter weight, competitive specific strength
and stiffness, improved energy recovery, carbon dioxide
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