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School of Chemical Sciences, Mahatma Gandhi University, Priyadarshini Hills P.O., Kottayam, Kerala 686 560, India
Received 14 February 2007; received in revised form 22 May 2007; accepted 24 May 2007
Available online 10 June 2007
Abstract
This review deals with a recent study of the literature on the various aspects of cellulosic bres and biocomposites. Cellulosic bre
reinforced polymeric composites are nding applications in many elds ranging from construction industry to automotive industry.
The pros and cons of using these bres are enumerated in this review. The classication of composites into green composites, hybrid
biocomposites and textile biocomposites are discussed. New developments dealing with cellulose based nanocomposites and electrospinning of nanobres have also been presented. Recent studies pertaining to the above topics have also been cited. Finally, the applications
of cellulosic bre reinforced polymeric composites have been highlighted.
2007 Elsevier Ltd. All rights reserved.
Keywords: Biocomposite; Biober; Green composite; Textile; Hybrid
Corresponding author. Tel.: +91 481 2730003; fax: +91 481 2561190.
E-mail addresses: sabut@sancharnet.in, sabut552001@yahoo.com (S.
Thomas).
0144-8617/$ - see front matter 2007 Elsevier Ltd. All rights reserved.
doi:10.1016/j.carbpol.2007.05.040
main components of natural bres are cellulose (a-cellulose), hemicellulose, lignin, pectins, and waxes.
Cellulose is a natural polymer consisting of D-anhydroglucose (C6H11O5) repeating units joined by 1,4-b-D-glycosidic linkages at C1 and C4 position (Nevell & Zeronian,
1985). The degree of polymerization (DP) is around
10,000. Each repeating unit contains three hydroxyl
groups. These hydroxyl groups and their ability to hydrogen bond play a major role in directing the crystalline packing and also govern the physical properties of cellulose.
Solid cellulose forms a microcrystalline structure with
regions of high order i.e. crystalline regions and regions
of low order i.e. amorphous regions. Cellulose is also
formed of slender rod like crystalline microbrils. The crystal nature (monoclinic sphenodic) of naturally occurring
cellulose is known as cellulose I. Cellulose is resistant to
strong alkali (17.5 wt%) but is easily hydrolyzed by acid
to water-soluble sugars. Cellulose is relatively resistant to
oxidizing agents.
Hemicellulose is not a form of cellulose and the name is
a misnomer. They comprise a group of polysaccharides
composed of a combination of 5- and 6-carbon ring sugars.
Hemicellulose diers from cellulose in three aspects.
Firstly, they contain several dierent sugar units whereas
cellulose contains only 1,4b-D-glucopyranose units.
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Species
Origin
Abaca
Bagasse
Bamboo
Banana
Broom root
Cantala
Caroa
China jute
Coir
Cotton
Curaua
Date palm
Flax
Hemp
Henequen
Isora
Istle
Jute
Kapok
Kenaf
Kudzu
Mauritius hemp
Nettle
Oil palm
Piassava
Pineapple
Phormium
Roselle
Ramie
Sansevieria (Bowstring hemp)
Sisal
Sponge gourd
Straw (Cereal)
Sun hemp
Cadillo/urena
Wood
Musa textilis
(>1250 species)
Musa indica
Muhlenbergia macroura
Agave cantala
Neoglaziovia variegata
Abutilon theophrasti
Cocos nucifera
Gossypium sp.
Ananas erectifolius
Phoenix Dactylifera
Linum usitatissimum
Cannabis sativa
Agave fourcroydes
Helicteres isora
Samuela carnerosana
Corchorus capsularis
Ceiba pentranda
Hibiscus cannabinus
Pueraria thunbergiana
Furcraea gigantea
Urtica dioica
Elaeis guineensis
Attalea funifera
Ananus comosus
Phormium tenas
Hibiscus sabdaria
Boehmeria nivea
Sansevieria
Agave sisilana
Lua cylinderica
Crorolaria juncea
Urena lobata
(>10,000 species)
Leaf
Grass
Grass
Leaf
Root
Leaf
Leaf
Stem
Fruit
Seed
Leaf
Leaf
Stem
Stem
Leaf
Stem
Leaf
Stem
Fruit
Stem
Stem
Leaf
Stem
Fruit
Leaf
Leaf
Leaf
Stem
Stem
Leaf
Leaf
Fruit
Stalk
Stem
Stem
Stem
impairs the eciency of the composite. This is a major disadvantage of natural bre reinforced composites. Another
problem is that the processing temperature of composites is
restricted to 200 C as vegetable bres undergo degradation at higher temperatures; this restricts the choice of
matrix material. Another setback is the high moisture
absorption of natural bres leading to swelling and presence of voids at the interface, which results in poor
mechanical properties and reduces dimensional stability
of composites. Another restriction to the successful exploitation of biobres for durable composite application is low
microbial resistance and susceptibility to rotting. These
properties pose serious problems during shipping, storage
and composite processing. The non-uniformity and variation of dimensions and of their mechanical properties (even
between individual plants in the same cultivation) poses
another serious problem.
It is quite clear that the advantages outweigh the disadvantages and most of the shortcomings have remedial measures in the form of chemical treatments. The
lignocellulosic bres have an advantage over synthetic ones
since they buckle rather than break during processing and
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346
347
Table 2
Natural and biodegradable matrices
Biodegradable polymer matrices
Natural
Synthetic
1. Polysaccharides
Starch
Cellulose
Chitin
2. Proteins
Collagen/gelatin
Casein, albumin, brogen, Silks
3. Polyesters
Polyhydroxyalkanoates
4. Other polymers
Lignin
Lipids
Shellac
Natural rubber
1. Poly(amides)
2. Poly(anhydrides)
3. Poly(amide-enamines)
4. Poly(vinyl alcohol)
5. Poly(vinyl acetate)
6. Polyesters
6.1 Poly(glycolic acid)
6.2 Poly(lactic acid)
6.3 Poly(caprolactone)
6.4 Poly(orthoesters)
7. Poly(ethylene oxides)
8. Poly(phosphazines)
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349
Fig. 4. SEM micrographs of PLA or PBS/BF composites with LDL (NCO content, 0.65%) after dierent enzymatic degradation time. (a) Control of
PLA/BF composite, (b) after 7 days, (c) 9 days, (d) control of PBS/BF composite, (e) after 2 days, (f) 4 days.
Fig. 5. Photographs of PLA (top) artd PLA/lyocell composite (bottom) after the soil burial test: (a) before test, (b) at 60 days, and (c) at 120 days.
350
351
Fig. 6. (a, b) SEM photomicrographs of the fracture tensile surfaces of untreated and treated composites.
352
glycerides and oils in beans for producing resins. These resins will be inexpensive compared to those available today
and if suitably modied, could be biodegradable. Research
is also being conducted to develop new pathways to synthesize inexpensive biodegradable resins (Allen, Moore, Lobkovsky, & Coates, 2002) with better mechanical
properties and thermal stability using nanotechnology
(Maiti & Giannelis, 2002).
2.1.2. Hybrid composites
The incorporation of several dierent types of bres into
a single matrix has led to the development of hybrid biocomposites. The behavior of hybrid composites is a
weighed sum of the individual components in which there
is a more favorable balance between the inherent advantages and disadvantages. Also, using a hybrid composite that
contains two or more types of bre, the advantages of one
type of bre could complement with what are lacking in the
other. As a consequence, a balance in cost and performance could be achieved through proper material design
(Thwe & Liao, 2003). The properties of a hybrid composite
mainly depend upon the bre content, length of individual
bres, orientation, extent of intermingling of bres, bre to
matrix bonding and arrangement of both the bres. The
strength of the hybrid composite is also dependent on the
failure strain of individual bres. Maximum hybrid results
are obtained when the bres are highly strain compatible
(Sreekala, George, Kumaran, & Thomas, 2002).
The properties of the hybrid system consisting of two
components can be predicted by the rule of mixtures.
P H P 1V 1 P 2V 2;
1:1:1
where PH is the property to be investigated, P1 the corresponding property of the rst system and P2 the corresponding property of the second system. V1 and V2 are
the relative hybrid volume fractions of the rst and second
system and
V 1 V 2 1:
1:1:2
Untreated
Alkali- treated (5%)
PMMA grafted (5%)
PAN grafted (10%)
Cyanoethylated
Bleached
Hybrid [coir/glass
polyester composite]
8.53
4.994
3.98
4.119
3.6
5.8
5.186
3.147
2.663
2.997
3.138
3.718
353
354
posites that have superior mechanical properties, as continuous orientation of bres is not restricted at any point.
In applications where more than one bre orientation is
required, a fabric combining 0 and 90 bre orientations is
useful. Woven fabrics are produced by the interlacing of
warp (0) bres and weft (90) bres in a regular pattern
or weave style. The fabrics integrity is maintained by the
mechanical interlocking of the bres. Drape (the ability
of a fabric to conform to a complex surface), surface
smoothness and stability of a fabric are controlled primarily by the weave style.
Twill
One or more warp bres alternately weave over and
under two or more weft bres in a regular repeated manner.
This produces the visual eect of a straight or broken diagonal rib to the fabric. Superior wet out and drape is seen in
the twill weave over the plain weave with only a small reduction in stability. With reduced crimp, the fabric also has a
smoother surface and slightly higher mechanical properties.
Satin
Satin weaves are fundamentally twill weaves modied to
produce fewer intersections of warp and weft. The harness
number used in the designation (typically 4, 5, and 8) is the
total number of bres crossed and passed under, before the
bre repeats the pattern. A crowsfoot weave is a form of
satin weave with a dierent stagger in the repeat pattern.
Satin weaves are very at, have good wet out and a high
degree of drape. The low crimp gives good mechanical
properties. Satin weaves allow bres to be woven in the
closest proximity and can produce fabrics with a close
tight weave. However, the styles low stability and asymmetry needs to be considered. The asymmetry causes one
face of the fabric to have bre running predominantly in
the warp direction while the other face has bres running
predominantly in the weft direction.
355
Mock leno
A version of plain weave in which occasional warp
bres, at regular intervals but usually several bres apart,
deviate from the alternate under-over interlacing and
instead interlace every two or more bres. This happens
with similar frequency in the weft direction, and the overall
eect is a fabric with increased thickness, rougher surface,
and additional porosity.
Basket
Basket weave is fundamentally the same as plain weave
except that two or more warp bres alternately interlace
with two or more weft bres. An arrangement of two warps
crossing two wefts is designated 22 basket, but the
arrangement of bre need not be symmetrical. Therefore
it is possible to have 82, 54, etc. Basket weave is atter,
and, though less crimp, stronger than a plain weave, but
less stable. It must be used on heavy weight fabrics made
with thick (high tex) bres to avoid excessive crimping.
Leno
Leno weave improves the stability in open fabrics
which have a low bre count. A form of plain weave in
Researchers have looked into tensile strength of ramiecotton hybrid bre reinforced polyester composites
(Junior, Carvalho, Fonseca, Monteiro, & Almeida, 2004).
They observed that tensile behaviour was dominated by
volume fraction of ramie bres aligned in the test direction.
The fabric and diameter of the thread did not play any role
in tensile characteristics. Cotton fabric was found to have
minor reinforcement eect due to weak cotton/polyester
interface. Similar studies were performed by Mwaikambo
and Bisanda (1999) on kapok-cotton bre reinforced polyester composites.
Pothen, Thomas, Li, and Mai (2002) conducted tensile
and impact studies of woven sisal fabric reinforced polyester composites prepared by RTM technique. It was found
that the weave architecture was a crucial factor in deter-
356
357
358
Fig. 9. (a) Under oor protection trim of Mercedes A class made from banana bre reinforced composites. (b) Newest Mercedes S class automotive
components made from dierent bio bre reinforced composites.
3. Electrospinning (ELSP)
high performance
359
Fig. 11. Proposed electrospinning techniques (a) electrospinning (b) multilayer spinning.
degradable nanobrous non-woven mats via multi jet electro spinning (Ding, Kimura, Sato, Fujita, & Shiratori,
2004).
Another interesting study was the electrospinning of
chitosan nanobres from aqueous chitosan solution using
concentrated acetic acid solution as a solvent. A uniform
nanobrous mat of average bre diameter of 130 nm was
obtained from 7% chitosan solution in aqueous 90% acetic
acid solution in an electric eld of 4 kV/cm. An aqueous
acetic acid concentration higher than 30% was prerequisite
for chitosan nanobre formation, because more concentrated acetic acid in water progressively decreased surface
tension of the chitosan solution and concomitantly
increased charge density of jet without signicant eect
on solution viscosity (Geng, Kwon, & Jang, 2005).
The fabrication and characterization of poly(vinyl alcohol)/chitosan blend nanobers by electrospinning method
was investigated by Yong-Tang et al. (2007). The results
showed that showed that the morphology and diameter
of the nanobers were mainly aected by concentration
of the blend solution, weight ratio of the blend, respectively. It was also observed that that there were strong
intermolecular hydrogen bonds between the molecules of
chitosan and poly(vinyl alcohol).
Recently researchers reported on the electrospinning
and crosslinking of zein nanobre mats (Yao, Li, & Song,
2007). Zein is a protein found in corn. The authors
observed that crosslinked zein exhibited higher tensile
properties than uncrosslinked zein.
4. Cellulose based nanocomposites
The concept of nanostructured materials design is gaining widespread importance among the scientic community (Berglund, 2005). The strong reinforcement eects
at low volume fraction resulted in a tremendous interest
from the industry and research circles. With this as an
inspiration, the potential of nanoscale cellulose structures
as reinforcement in novel composite materials was extre-
360
The basic idea was to increase the volume fraction of cellulose microbrils by partially removing the lignin and hemicellulose wood polymers and by compressing the veneer.
Phenol formaldehyde resin (PF) was used to preserve the
compressed microstructure of the material and to bond
microbrils.
The orientation of cellulose nanowhiskers in polyvinyl
alcohol was investigated by Kvien and Oksman (2007).
Cellulose whiskers were incorporated in a polyvinyl alcohol
matrix using solution casting with water as the solvent. The
suspension was cast and the water was evaporated while a
homogeneous magnetic eld of 7 T was applied. Dierent
microscopy investigations of prepared nanocomposites
indicated that the cellulose whiskers were oriented perpendicular to the direction of the magnetic eld. Dynamic
mechanical thermal analysis further strengthened the idea
of alignment because the results showed that the dynamic
modulus of the nanocomposite was around 2 GPa higher
at room temperature in the aligned direction compared to
the transverse direction.
In an interesting study, nanocomposite materials reinforced with ax cellulose nanocrystals in waterborne polyurethane was reported by Xiaodong, Hua, and Chang
(2007). The results indicated that the cellulose nanocrystals
could disperse in the polyurethane uniformly and resulted
in an improvement of microphase separation between the
soft and hard segments of the WPU matrix. The lms
showed a signicant increase in Youngs modulus and tensile strength from 0.51 to 344 MPa and 4.27 to 14.96 MPa,
respectively, with increasing ller content from 0 to
30 wt%.
5. Conclusions
The term biocomposite is now being applied to a staggering range of materials derived wholly or in part from
renewable biomass resources. Keeping up with the developments in technology, it is compulsory that we stop
developing materials, which are environmentally hazardous. This concept of bio-based materials has now become
of key importance due to the need to preserve our environment. Biobres like sisal, coir, hemp, oil palm are
now nding applications in a wide range of industries.
The eld of bio-bre research has experienced an explosion of interest, particularly with regard to its comparable
properties to glass bres within composites materials. The
main area of increasing usage of these composites materials is the automotive industry, predominantly in interior
applications.
Material revolution of this century may be provided by
green composite materials. Sustainability, cradle-to-grave
design, industrial ecology, eco-eciency, and green chemistry are not just newly coined buzz words, but form the
principles that are guiding the development of a new generation of green materials. Another promising area is that
of nanocomposites and electrospinning of nanobers.
361
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