Review 955

Summary: The use of lignocellulosic fibers, pineapple leaf

fiber (PALF) and sisal as reinforcements in thermoplastic and
thermosetting resins for developing low cost and lightweight
composites is an emerging field of research in polymer
science and technology. Although, these biofibers have sev-
eral advantages, such as low densities, low cost, nonabrasive
nature, high filling level possible, low energy consumption,
high specific properties, biodegradability, etc., over synthetic
fibers, the absorption of moisture by untreated biofibers, poor
wettability, and insufficient adhesion between the polymer
matrix and fiber deteriorate the mechanical properties of
composites made up of these biofibers. Therefore, the modi-
fication of these fibers is a key area of research at present to
obtain optimum fiber-matrix properties. This review article is
concerned with the structure, composition and properties of
PALF and sisal, the chemical modifications of these fibers
and PALF/sisal-reinforced thermosets, thermoplastics, rub-
ber, cement, hybrids and biocomposites.
Scanning electron micrograph of tensile fractured surface of
alkali treated sisal fiber (magnification
500).

A Review on Pineapple Leaf Fibers, Sisal Fibers

and Their Biocomposites
Supriya Mishra,1 Amar K. Mohanty,2 Lawrence T. Drzal,3 Manjusri Misra,*3 Georg Hinrichsen4
1
Beech 40, Oak House, 1 Moseley Road, Manchester M14 6HX, UK
2
The School of Packaging, 130 Packaging Building, Michigan State University, East Lansing, MI 48824, USA
3
Composite Materials and Structures Center, Michigan State University, 2100 Engineering Building, East Lansing,
MI 48824-1224, USA
E-mail: misraman@egr.msu.edu
4
Technical University of Berlin, Institute of Materials Science and Technology, Englische Str. 20, D-10587 Berlin, Germany

Received: May 14, 2004; Revised: September 7, 2004; Accepted: September 8, 2004; DOI: 10.1002/mame.200400132
Keywords: biocomposites; biofibers; hybridization; matrix; mechanical properties

1. Introduction years, there has been a dramatic increase in the use of

Present-day research in the field of polymer science and
technology has been focused on developing plastics, papers,
adhesives, textile fibers, composites, blends, and many
other industrial products from renewable resources, mostly
the abundantly available agro-waste and lignocellulosic
materials. Newer materials and composites that have both
economic and environmental benefits are being considered
for application in the automotive, building, furniture, and
packaging industries. Growing environmental awareness,
new rules, and regulations throughout the world for the
creation of bio-based economy are challenging industry,
academia, government, and agriculture. Within the past few
natural fibers for composites. Recent advances in natural
fiber development, genetic engineering, and composite
science offer significant opportunities for improved materi-
als from renewable resources with enhanced support for
global sustainability.[1,2]
The potential of natural fiber-based composites using
cellulose, wood, jute, kenaf, hemp, coir, sisal, pineapple,
etc., as reinforcing fibers in both thermosetting and thermo-
plastic resins has received considerable attention among
scientists all over the world for their excellent specific
properties. Several investigators[3–9] have prepared and
evaluated the properties of composites based on natural
fibers for diverse applications. Polymer composites have

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956
been developed using short and long fibers, chips, flakes,
strands, wood pulp fiber, and wood flour, etc. Mohanty and
Misra[10] have reviewed jute-reinforced thermosets, ther-
moplastics, and rubber-based composites whereas Bledzki
and Gassan have reviewed composites reinforced with
cellulose-based fibers.[11] Recently, sisal fiber and its com-
posites have been reviewed by Li et al.[12]. By embedding
natural reinforcing fibers, e.g., flax, hemp, ramie, jute, etc.,
into biopolymeric matrix made of derivatives from cellu-
lose, starch, lactic acid, etc., new fiber-reinforced materials
called biocomposites have been created and are still being
developed.[13–20] Biocomposites containing natural fibers
and biodegradable matrices have been patented[21] for app-
lications as building materials. The title materials contain
natural fibers, e.g., flax, hemp, ramie, sisal or jute, and a
biodegradable matrix such as cellulose diacetate, or a starch
derivative. The influence of various surface modifications
on the performance of jute-Biopol composites has been
reported by Mohanty et al.[22,23] Lignocellulosic straw
fiber-reinforced Biopol1 generally leads one to expect
good mechanical properties of such composites as reported
by Avella and dell’Erba.[24] Biocomposites from jute and
synthetic biodegradable plastic i.e., polyester amide have
also been reported.[25] A three corner approach – efficient
bio-fiber surface treatment, matrix modification, and selec-
tion of processing technique has been targeted[26–36] in
designing biocomposites of superior physico-mechanical
properties.
Availability of inexpensive lignocellulosic natural fibers,
such as pineapple leaf fiber (PALF) and sisal in tropical
countries, provides an unique opportunity of exploring the
possibility of their utilization for the synthesis of inexpen-
sive biodegradable composites for various applications.
The primary advantages of using these fibers as reinforce-
ments in polymer composites are listed as follows: (1) low
density, (2) low cost, (3) nonabrasive nature, (4) high filling
level possible, (5) low energy consumption, (6) high
specific properties, (7) biodegradability, and (8) generation
of rural/agricultural-based economy. The structure and
properties of these natural fibers depend upon several fac-
tors such as age, source, microfibrils, straightness, diameter,
and chemical constituents. Since these fibers have small
cross-sections and cannot be directly used in engineering
applications, they are embedded in matrix materials to form
fiber composites. The matrix serves as binder to bind the
fibers together and transfers loads to the fibers. In order to
develop and promote these natural fibers and their compo-
sites, it is necessary to understand their physico-mechanical
properties. Several reports have been published on the
structures and properties of these natural fibers but a great
deal of additional research is still needed in this area.
The major constituents of natural fibers (PALF and sisal)
are cellulose, hemicellulose, and lignin. The elementary
unit of a cellulose macromolecule is anhydro-D-glucose,
which contains three alcohol hydroxyls (–OH). These
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S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen
hydroxyls form hydrogen bonds inside the macromolecule
itself (intramolecular) and between other cellulose macro-
molecules (intermolecular) as well as with hydroxyl groups
from the air. Therefore, PALF and sisal, like all vegetable
fibers are hydrophilic in nature and their moisture content
reaches about 11%.[37] These fibers can act as effective
reinforcements for polymer, rubber, gypsum, and cement
matrices. However, PALF/sisal fiber-reinforced composites
generally have poor interface and moisture resistance
properties. The properties of composites depend on those
of the individual components and on their interfacial
compatibility. The adhesion between the fiber and the
matrix is obtained by the mechanical anchoring of the fiber
surface ends into the matrix. The absorption of moisture by
untreated fibers, poor wettability, and insufficient adhesion
between the polymer matrix and fiber leads in time to
debonding.[38–40] Without effective wetting of the fiber,
strong interfacial adhesion cannot exist leading to internal
strains,[41] porosity, and environmental degradation.[42,43]
Therefore, the modification of the fiber is a key area of
research at present to obtain optimum fiber-matrix proper-
ties. Properties of reinforcing fiber can be modified and
tailored to different fashions and degrees by some chemical
and physical methods.
2. Availability, Composition,
Structure and Properties
The source, origin, nature as well as physical and chemical
composition of different natural fibers have been
reviewed.[44,45] Natural fibers are subdivided based on their
origins, coming from plants, animals or minerals. Gener-
ally, plant or vegetable fibers are used to reinforce plastics.
Plant-fibers may include (i) leaf: sisal, pineapple leaf fiber
(PALF), and henequen; (ii) bast: flax, ramie, kenaf/mesta,
hemp, and jute; (iii) seed: cotton; (iv) fruit: coconut husk,
i.e., coir. Climatic conditions, age, and the digestion process
influence not only the structure of fibers but also the
chemical composition. The components of natural fibers are
cellulose, hemicellulose, lignin, pectin, waxes, and water-
soluble substances, with cellulose, hemicellulose, and
lignin as the basic components with regard to the physical
properties of the fibers. The chemical composition and
structural parameters of PALF and sisal are represented in
Table 1 whereas Table 2 comprises the important properties
of these two fibers. A single fiber of all plant-based natural
fibers consists of several cells.[11] These cells are formed out
of crystalline microfibrils based on cellulose, which are
connected to a complete layer, by amorphous lignin and
hemicellulose. Multiple layers of such cellulose-lignin/
hemicellulose in one primary and three secondary cell walls
stick together to form a multiple-layer-composite, the cell.
These cell walls differ in their composition (ratio between
cellulose and lignin/hemicellulose) and in the orientation
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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites 957

Table 1. Chemical composition and structural parameters of
PALF and sisal.[2]
PALF
Cellulose/wt.-% 70–82
Lignin/wt.-% 5–12
Hemicellulose/wt.-% – 10–14.2
Pectin/wt.-% – 10
Wax/wt.-% – 2
Microfibrillar-spiral angle/degree 14
Moisture content/wt.-% 11.8
(spiral angle) of the cellulose microfibrils. The character-
istic values for these structural parameters vary from one
natural fiber to another as well as by physico-chemical fiber
treatments.
The spiral angle of the fibrils and the content of cellulose
generally determine the mechanical properties of the
cellulose-based natural fibers. For instance, models devel-
oped by Hearle et al.[46] considers these two structure
parameters to calculate the Young’s modulus of the fibers.
The basic idea of the model has been described by Hearle
and Sparrow[46] and the model has been applied by
Mukherjee and Satyanarayana[47] on various natural fibers.
2.1. Pineapple Leaf Fiber (PALF)
Pineapple leaf fiber (PALF) is obtained from the leaves of
the plant, Anannus comosus, belonging to the Bromeliaceae
family. These pineapple leaves are going to waste because
of lack of knowledge about their economic uses. One of
the SITRA’s (South India Textile Research Association)
findings[48] under the UNDP/UNIDO assisted project
revealed that PALF could be successfully spun in the cotton
spinning system with slight modifications to produce 100%
PALF yarn and their blends with other natural and synthetic
fibers, especially with cotton. The yarns thus produced were
used to make fabrics, fancy carpets, mops, curtains, etc.
2.1.1. Production
PALF is largely cultivated in tropical countries, mainly for
its fruits. Its cultivation in India is substantial (about
2 250 000 acres of land is cultivated[49] and is increasing; in
the future a considerable increase in the production of the
fiber is envisaged). The pineapple plant has a very short
stem which first produces a rosette of leaves but which latter
elongated and bear numerous spirally arranged fibrous
leaves.[50] The leaves are 3ft. long, 2 to 3 inch wide sword
Sisal shaped, dark green in color and bear spines of claws on their
margins. The leaves of the pineapple plant yield strong,
67–78 white fine silky fibers. Since the pineapple plant is a special
8–12
crop, only limited quantity of fiber is available. Therefore,
no attempt has been made to grade these fibers.
20 2.1.2. Processing
11
Fibers are obtained by either mechanical means or retting
the leaves in water. Fresh leaves yield about 2 to 3% of
fiber.[51] The fiber is multicellular with very small lumen
size almost like a line. The filaments of PALF being strong-
er and finer than jute, have been successfully spun to a fine
yarn on jute machinery.[50] Some techniques are also being
developed for processing PALF on jute machinery. Jute
finisher, a card and a flax finisher with progressively, higher
density are used as the first and the second cards, respec-
tively, for PALF instead of conventional breaker and
finisher card. The optimum twist factor in the case of PALF
yarn is found to be of the order of 24 to 27 tex to cm units in
yarn of 70 tex.
2.1.3. Composition and Structure
Chemically, PALF is multicellular lignocellulosic in nature,
comprising mainly polysaccharides and lignin and other
compounds such as fat, wax, pectin, uronic anhydride,
pentosan, coloring matter, inorganic substances,[52] etc. It
has a ribbon-like structure and is cemented together by
gummy matters like lignin and pentosan, which contribute
to the strength of the fiber. It consists of a vascular bundle
system present in the form of bunches of fibrous cell which
is obtained after mechanical removal of all the epidermal
tissues from the harvest.
Since PALF contains about 70–82% of cellulose,[47] the
arrangement of molecules in the fibers is similar to cotton
cellulosic fibers. The molecular chains of cellulose lie para-
llel and in three-dimensional arrangements in the crystal-
line region of fibers. The other portions of the molecular
chains are believed to lie in a less ordered state in the
amorphous regions. PALF is of fine quality, and unlike jute,
its structure is without mesh. Filaments are well separated
and it is two and half times more extensible, with superior
fiber bundle strength.

Table 2. Physical and mechanical properties of PALF and 2.1.4. Properties

sisal.[2]
The superior mechanical properties of pineapple leaf fiber
Properties PALF Sisal are associated with its high cellulose content and compara-
tively low microfibrillar angle. Both the flexural and
Density/(g  cm3) 1.44 1.45 torsional rigidity of PALF are comparable with jute fibers.
Diameter/mm 20–80 50–200
Tensile strength/MPa 413–1 627 468–640 An interesting characteristic of PALF is that the bundle
Young’s modulus/GPa 34.5–82.51 9.4–22.0 strength of PALF decreases by 50% when in a wet condition
Elongation at break/% 1.6 3–7 but the yarn strength increases by about 13%. Studies of

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958
stress-strain relationship have indicated the fiber to be
sufficiently strong. The fiber has an initial modulus of 34.5–
82.51 GN  m2, a tensile strength of 413–1 627 MN  m2,
and an elongation at break of 0.8–1.6%. It is highly resistant
to abrasive wear.[53] The physical, mechanical and di-
electric properties, tensile behavior, surface and fracture
morphology of PALF have been reported by many work-
ers.[54–57] Datta et al.[54] have studied the mechanical and
dielectric properties of pineapple fibers. Pineapple fibers
with cellulose type I structure have good elastic properties,
can withstand high strains comparable with other similar
fibers, but have lower breaking stresses because of the high
concentration of disorder. The electrical properties show
high anisotropy. Mukherjee and Satyanarayana[55] reported
on the mechanical properties of PALF. X-ray analysis
indicated[58] that there is a high degree of crystallinity along
with the orientation of the spiral angle of 148 with the fiber
axis. The fiber is highly hygroscopic. The range of its
crystallinity[54] is from 0.63 to 0.68 and its dielectric
behavior is comparable to jute.[59]
i. Effect of Acid and Alkali
Generally, plant lignin resists the action of acids to a greater
extent, while cellulose and hemicellulose undergo slow
hydrolysis with mineral acids. Aqueous solutions of organic
acids at low temperature have little or no effect on car-
bohydrates, but at high temperature, however, a gradual
conversion of cellulose to hydrocellulose and of xylose to
furfural occurs.[59] Pure cellulose (as in cotton) gives
colloidal solutions of low molecular weight compounds
when treated with aqueous sulfuric acid of concentration
about 1 000 g  l1 but lignified fibers like PALF, do not give
colloidal solutions at such concentration when washed
unless they are subjected to severe mechanical action.
Alkalis, particularly sodium hydroxide, readily react with
hemicellulose but have little effect on lignin at low
concentrations.[59]
ii. Effect of Bleaching
Bleaching of PALF with H2O2 improved the fineness by
5–6% but reduced the tensile strength by 40–45%.[60]
Bleached fibers when spun into yarns produced a more
uniform and extensible but lower strength yarns than unble-
ached raw fibers. Raw yarns upon bleaching showed higher
extension, lower strength, and more irregularity than
unbleached yarns.
iii. Effect of Dyeing
PALF is a lignified fiber and the presence of high amounts of
lignin and other waxy substances causes dyes to fade more
rapidly than when applied to cotton. PALF has an additional
problem of difficult dye penetration due to its relatively high
coarseness.
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S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen
2.2. Sisal Fiber
Sisal fiber is a hard fiber extracted from the leaves of the
sisal plant (Agava sisalana). It is one of the four most
widely used natural fibers and almost accounts for half the
total production of textile fibers. The reason for this is due to
the ease of cultivation of sisal plants and which have short
renewal times.[61]
2.2.1. Production
Though native to tropical and sub-tropical North and South
America, sisal plant is now widely grown in tropical
countries of Africa, the West Indies and the Far East.[40]
Nearly 4.5 million tons of sisal fiber are produced every year
throughout the world. Tanzania and Brazil are the two main
producing countries.[53]
A sisal plant produces about 200–250 leaves and each
leaf contains 1 000–1 200 fiber bundles, which is composed
of 4% fiber, 0.75% cuticle, 8% dry matter, and 87.25%
water.[61] The sisal leaf contains three types of fibers:[40]
mechanical, ribbon, and xylem. The mechanical fibers are
mostly extracted from the periphery of the leaf. They have a
more or less thickened horseshoe shape and seldom divide
during extraction processes. They are the most predominant
fibers and their fineness dictates the grading and general
commercial usefulness of sisal fiber. Ribbon fibers occur in
association with the conducting tissues in the median line
of the leaf, which gives them considerable mechanical
strength. Xylem fibers have an irregular shape and occur
opposite to the ribbon fibers through the connection of vas-
cular bundles. They are composed of thin-walled cells and
are therefore easily broken up and lost during the extraction
process.
2.2.2. Processing
The processing methods used to extract sisal fibers have
been reported by Chand et al.[53] and Mukherjee and
Satynarayana.[61]
The methods include:
a) Retting followed by scrapping
b) Mechanical means using decorticators
It is shown that the mechanical process yields about 2–4%
fiber with good quality having lustrous color while the
retting process yields a large quantity of poor quality fibers.
After extraction, the fibers are washed thoroughly in plenty
of clean water to remove the surplus wastes such as
chlorophyll, leaf juices, and adhesive solids.
2.2.3. Composition and Structure
Sisal fiber is composed of 78% cellulose, 8% lignin, 10%
hemicelluloses, 2% waxes, and about 1% ash by weight.[62]
Cellulose (a-cellulose): These components consist of
mainly cellulose chains with glucose as the ultimate build-
ing units. They are resistant to strong alkali (17.5 wt.-%),
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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites
easily hydrolyzed by acids to water-soluble sugars and
relatively resistant to oxidizing agents.
Hemicellulose: They are composed of cellulose chains,
but are much shorter in length and are built up of a mixture of
polysaccharides of relatively low molecular weight. They are
soluble in alkali and are easily hydrolyzed by acids.
Lignin: Its chemistry has not yet been precisely estab-
lished, but the functional groups and building units of the
molecule have been mostly identified. It is characterized by
high carbon content and low hydrogen content, which
indicate that it is either highly unsaturated or aromatic in
character along with the presence of hydroxyl, methoxyl
and possibly carbonyl groups. It has been found to contain
five hydroxyl and five methoxyl groups per building units,
with a minimum molecular weight of 830. Most researchers
believe that the structural units of a lignin molecule are
derivatives of 4-hydroxy-3-methoxy phenyl propane. It is
highly complex and amorphous in nature. It is not hydro-
lyzed by acids, but soluble in hot alkali, readily oxidizable,
easily condensable with phenol and giving a number of
color reactions.
Chemically, sisal fiber may therefore be considered to be
composed of cellulose chains and hemicellulose intimately
associated with lignin. The length of sisal fiber is in between 1
to1.5 m and the diameterisabout 100–300 mm.[63] The fiber is
actually a bundle of hollow sub-fibers. Their cell walls are
reinforced with spirally oriented cellulose in a hemicellulose
and lignin matrix. Thus, the cell wall is a composite structure
of lignocellulosic materials reinforced by helical microfi-
brillar bands of cellulose. The composition of the external
surface of the cell wall is a layer of lignaceous material and
waxy substances that bond the cell to its adjacent neighbors.
Hence, this surface does not form a strong bond with a
polymer matrix. Also, cellulose is a hydrophilic glucan
polymer consisting of linear chains of 1,4-b-bonded anhy-
droglucose units[64] and these large amounts of hydroxyl
groups give sisal fiber hydrophilic properties. This leads to a
very poor interface between sisal fiber and the hydrophobic
matrix and very poor moisture absorption resistance.
2.2.4. Properties
Sisal fibers having both crystalline and non-crystalline
components when subjected to tension are expected to
undergo deformation as in the case of banana fibers.[65] The
applied stress initially is shared between the crystalline and
non-crystalline components in fibrous composites and the
extent to which the fiber resists deformation in this low
strain region is called initial modulus of the fiber. The
effective modulus (Ef) may also be calculated in terms of
major chemical components present in the fiber and is given
by the equation according to McLaughlin and Tait:[61,66]
Ef ¼ Wc Ec cos2 y þ Wnc Enc ð1Þ
where Ec and Enc are modulus values of the crystalline and
non-crystalline regions, respectively, and are assumed to be
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959
45 GN  m2 and 3 GN  m2, respectively, for the vegetable
fibers.[61] Wc and Wnc are the weight fractions of the cryst-
alline and non-crystalline components, which have the
values of 0.67 and 0.12, respectively, for sisal fiber. The
microfibrillar angle (y) for sisal is found to be 23.148.[61]
The modulus value (Ef) calculated using the above values in
Equation (1) is 26 GN  m2.
The structure and properties of natural fibers depend on
their source, age, etc.[67] It was reported that the tensile
properties of sisal fiber are not uniform along its length.[40]
The root or lower part has low tensile strength and modulus
but high fracture strain. The fiber becomes stronger and
stiffer at mid-span and the tip has moderate properties. The
fiber has tensile strength of 445–600 MN  m2 and tensile
modulus of 9–15.8 GN  m2. Mukherjee and Satyanar-
ayana[61] have studied the effects of fiber diameter, test
length, and test speed on the tensile strength, initial modu-
lus, and percent elongation at break of sisal fibers. They
concluded that no significant variation of mechanical pro-
perties with change in diameter is observed. However, the
tensile strength and percent elongation at break decrease
while Young’s modulus increases with fiber length. With
increasing test speed, Young’s modulus and tensile strength
both increase but elongation does not show any significant
variation. The mechanical properties of sisal fibers of dif-
ferent age at 3 different temperatures have been investigated
by Chand and Hashmi.[68] The tensile strength, modulus,
and toughness of sisal fiber decrease with increase of
temperature. The effect of plant age on these mechanical
properties is less at 100 8C when compared to 30 8C. This is
attributed to the more intense removal of water and/or other
volatiles (at 100 8C) originally present in the fibers, which
otherwise act as plasticizing agents in the chains of the
cellulose molecules. It is however noted that at 80 8C both
tensile strength and modulus decreasewith age of the
plant.[68]
In the case of the dielectric properties of sisal fiber,[69] an
increase of frequency decreases the dielectric constant e
value, while an increase of temperature increases e at all
frequencies. Increasing the plant age shifts the dissipation
factor (tan d) peak to higher temperatures. These phenom-
ena are explained on the basis of structural changes. The
thermal treatment of sisal fiber[70] shows that the chemical
structure of fibers will not be changed under 200 8C while
the degree of crystallinity can be increased and hence the
density. The thermal behavior is essentially identical for
heat treatment between 150 to 200 8C. Hence, thermal
treatment of sisal fibers can be carried out below 200 8C.
The water uptake behavior of sisal fiber has been studied by
Mohanty et al.[71]
3. Surface Modifications
The quality of the fiber-matrix interface is significant for
the application of natural fibers (PALF and sisal) as
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960
reinforcement fibers for plastics. Physical and chemical
methods can be used to optimize this interface. The
hydroxyl groups, which occur throughout the structure of
natural fibers (PALF and sisal), make them hydrophilic. But
many polymer matrices are hydrophobic so that PALF/
sisal-polymer composites have poor interfaces. Also, the
hydrophilic PALF/sisal fibers absorb large amount of water
in the composites leading to failure by delamination.
Adequate adhesion across the interface has been tried to
achieve at desirable levels by better wetting and chemical
bonding between fiber and matrix. The chemical methods
of modifications include:
. chemical treatments of fibers, and
. chemical coupling
3.1. Chemical Treatments
A schematic representation of various chemical treatments,
such as alkali treatment, cyanoethylation, and acetylation of
PALF/sisal fibers is given in Scheme 1.
The structural features and fracture morphology of raw
and chemically treated PALFs have been studied by Saha
et al.[57] using scanning electron microscopy (SEM). Sur-
face morphology progressively changes with gradual
removal of non-cellulosic constituents like lignin and
hemicellulose by alkali treatment. Fracture morphology
shows that there is a uniform sharing of the load in the
ultimate fibers of raw pineapple leaf, whereas treated leaf
shows irregular fractures characterized by the slippage of
individual ultimate fibers. Saha et al.[72] also studied the
infrared spectra of raw and chemically treated PALF using
the KBr disk technique. Bands due to lignin and hemi-
cellulose in the spectra of the fibers and their changes due to
Scheme 1.
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S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen
chemical (NaOH and NaClO2) treatment were discussed.
The quality enhancement of PALF has been tried by various
workers[60,73–75] through different chemical modifications.
Samal et al.[73] studied the functionality changes in PALF
through mercerization, cyanoethylation, and oxidation. The
modified fibers have been characterized by FTIR spectro-
scopy and viscosity measurements. It has been shown that
cyanoethylation and cyanoethylation followed by grafting
with acrylonitrile (AN) and methyl methacrylate (MMA)
bring about a significant reduction in the moisture regain
(enhanced hydrophobicity) of PALF. The dye uptake ability
of PALF is progressive with the time of cyanoethylation.
Chemical modifications like alkali treatment, nitration,
dinitrophenylation, benzoylation, and benzoylation-acety-
lation have been carried out on PALF.[60] It has been shown
that the reduction in percent moisture regain is significant
upon dinitrophenylation and benzoylation-acetylation but
low upon nitration. All the above chemically modified
fibers except benzoylated PALF have higher mechanical
strength than that of PALF. Bleaching of PALF with
H2O2[76] improves the fineness by 5–6% but reduces the
tensile strength by 40–45%. Raw yarns upon bleaching
show higher extension, lower strength, and more irregular-
ity than unbleached yarns.
Most previous studies are focused on sisal fiber surface
treatment methods and the resultant effects on the physical
and mechanical properties of sisal fiber-reinforced polymer
composite systems. Yang et al.[77] studied the relationship
of surface modification and tensile properties of sisal fibers.
Their modification methods include: alkali treatment,
H2SO4 treatment, combined H2SO4, and alkali-thermal
treatment. Thermal treatment (at 150 8C for 4 h) seems to be
the most desirable method in terms of strength and modulus
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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites 961

properties. To improve the moisture-resistance of sisal fiber,

Chand et al.[78] have taken acetylated sisal fiber and studied
its tensile strength. It was shown that acetylation can reduce
the moisture content from 11 to 5.45%. However, the tensile
strength of acetylated sisal fiber is reduced from 445 to
320 MPa due to the loss of the hemicelluloses in the fiber
during acetylation. The sisal fibers have been modified by
various chemical treatments, e.g., alkali treatment, cyano-
ethylation, and acetylation with the objective of improving
the fiber-matrix adhesion in the resulting composites.[79]
The presence of different functional groups such as –OH,
–COOH, >C O, –C N (in cyanoethylated fiber), and
aromatic moieties, etc. are indicated by the FTIR spectra of
the chemically modified fibers. The alkali treatment pro- Figure 2. Scanning electron micrograph of tensile fractured
duces fibers with optimum thermal stability, as revealed by surface of alkali treated sisal fiber (magnification
500).
the thermo-gravimetric analysis (TGA). The cyanoethyl-
ated fibers have lower decomposition temperatures (in the 3.2.1. Graft Copolymerization
second zone) as compared to the control i.e., untreated sisal
Graft copolymerization of monomers is one of the univer-
fiber. Furthermore, the alkali treatment removes the surface
sal, effective, and accessible methods of chemical mod-
debris and irregularities by removing the lignin and hemi-
ification of high molecular weight compounds, particularly
cellulose, as shown by the SEM photographs. Figure 1
natural polymers.[80–83] The studies on the effect of grafting
and 2 present SEM photographs of untreated and alkali
on the performance of composites are a challenging field of
treated sisal fibers. In the case of cyanoethylated sisal fiber
research, which is yet to be established by research workers.
(Figure 3), the intercellular gaps are reduced due to
Graft copolymerization of acrylonitrile (AN) onto chemi-
deposition of the cyanoethyl moieties on the fiber surface.
cally modified PALF has been studied by Mohanty et al.[74]
From the results of Table 3, it has been shown that the
using Ce(IV) and N-acetylglycine (NAG) combination as
cyanoethylated sisal fiber shows the highest tensile proper-
initiator in the temperature range 40–60 8C. Tripathy
ties (tensile strength ¼ 680 N  mm2, Young’s modulus ¼
et al.[75] studied the Cu(II)-IO4 initiated graft copolymer-
22.5 GN  mm2 and elongation at break ¼ 7.1%).
ization of MMA from defatted PALF. Effects of variation of
time and temperature, concentration of Cu(II), KIO4, and
MMA, the amount of PALF, and also the effects of some
3.2. Chemical Coupling
inorganic salts and organic solvents on the percentage of
An important chemical modification method is the chemi- graft yield have been investigated. On the basis of these
cal coupling method, which improves the interfacial experimental findings, a reaction mechanism (Scheme 2)
adhesion. The fiber surface is treated with a compound has been proposed. It has been shown that grafting improv-
that forms a bridge of chemical bonds between fiber and ed the thermal stability of PALF. Samal and Bhuyan[73]
matrix. studied the graft copolymerization of AN and MMA onto
PALF, using cerric ion as an initiator at varying concentra-
tions of monomer, initiator, and mineral acid at a number of

Figure 1. Scanning electron micrograph of tensile fractured Figure 3. Scanning electron micrograph of tensile fractured
surface of untreated sisal fiber (magnification
500). surface of cyanoethylated sisal fiber (magnification
1 500).

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962 S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen

Table 3. Tensile properties of control (untreated) and chemically including thermoplastics and thermosets, for the prepara-
modified sisal fibers.[79] tion of high performance composites. Joseph et al.[85]
Fiber samples Tensile Young’s Elongation treated sisal fibers with maleic anhydride grafted poly-
strength modulus at break (propylene) (MAH-PP) in order to improve the interfacial
adhesion between the fiber and the PP matrix in sisal/PP
N  mm2 GN  mm2 %
composite. The beneficial effect of maleated PP on the
Control 575 14.9 3.9 strength properties of sisal/PP composites have been attri-
Alkali treated 460 10.6 4.1 buted to the esterification reaction between cellulosic fiber
Cyanoethylated 680 22.5 7.1
hydroxyl groups and anhydride functionality of maleated
Acetylated 637 19.7 6.5
PP. The mechanism of reaction can be divided into two
steps:
. activation of the copolymer by heating (Scheme 3)
temperatures for various time intervals. The tensile data . esterification of cellulose (Scheme 4)
reveal a moderate increase in the tensile modulus of PALF
when grafted with AN; on the other hand, for cyanoethyl-
3.2.2. Treatment with Isocyanates
ated PALF-graft-PAN the samples have higher percentage
grafting, but the increase in tensile modulus is not high. Sisal fibers were treated with urethane derivative of toluene
Graft copolymerization of AN onto chemically modified diisocyanate/poly(propylene glycol) (TDI/PPG) and poly-
sisal fiber has been carried out by Mishra et al.[84] with a methylene-poly(phenyl isocyanate) (PMPPIC) by Joseph
view to improving the surface, as well as the bulk mech- et al.[85] with the objective of improving the dynamic
anical properties for its potential use as a reinforcing mechanical properties of sisal/PP composites. The better
fiber for polymer composites. It has been found that performance is due to the formation of urethane linkage
[IO4 ] ¼ 0.008 mol  L
1
and [Cu2þ] ¼ 0.002 mol  L1 between –OH group of the fiber and –N C O group of
produced optimum grafting for 0.1 g chemically modified PMPPIC or TDI/PPG, as shown in Scheme 5.
sisal fiber and 1 mL AN at 60 8C. Further, the best water
absorption and tensile properties are obtained with a low
3.2.3. Other Coupling Agents
percentage of grafting (5% grafting) of fiber. The AN-
grafted sisal fibers are expected to act as compatible rein- Surface modification of sisal fiber using coupling agents has
forcing fibers with several hydrophobic resin systems, been studied by Singh et al.[86]. The four coupling agents

Scheme 2.

Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de ß 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites
Scheme 3.
used are: N-substituted methacrylamide; g-methacryloxy-
propyltrimethoxysilane; neopentyl(diallyl)oxytri(dioctyl)-
pyrophosphato titanate; and neopentyl(diallyl)oxytriacryl
zirconate. The moisture absorption of surface-treated fibers
has been reduced significantly by providing hydrophobicity
to the surface via long chain hydrocarbon attachment. In
addition, these coupling agents penetrate the cell wall
through surface pores and deposit in the interfibrillar re-
gions and on the surface, restricting further ingress of
moisture.
4. PALF/Sisal Fiber-Reinforced Composites
4.1. Thermoset Composites
4.1.1. Polyester Composites
Useful composites with good strength can be successfully
developed using PALF as reinforcing agent for the polymer
matrix. Pavithran et al.[87] studied unidirectionally aligned
PALF-polyester composites and the toughness of these
composites is found to increase with the microfibrillar angle
of the fibers. Mechanical properties of PALF-reinforced
polyester composites have also been studied by Uma Devi
et al.[88] The influence of fiber length, fiber loading, and
coupling agents on the tensile, flexural, and impact proper-
Scheme 4.
Scheme 5.
Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de
963
ties of the composites were analyzed. The optimum length
of the fiber required to obtain composites of maximum
properties is found to be 30 mm. The tensile strength and
Young’s modulus of these composites increased linearly
with the fiber weight fraction. But in the case of flexural
strength, there is a leveling off beyond 30%. The impact
strength also increased linearly with the weight fraction of
the fiber. A significant increase in the strength of the
composites is observed after treatment of the fibers. Table 4
shows the mechanical properties of composites obtained
with chemically treated PALF and polyester matrix. The
best improvement is observed in the case of silane A-172-
treated fiber composites. Recently, Mishra et al.[89] reported
on the potential of PALF as a reinforcement in PALF-
polyester composites. The tensile strength and flexural
strength of these PALF-polyester composites increased
linearly with the fiber weight fraction up to 30 wt.-% and
then decreased (Figure 4). The impact (izod) strength also
increased linearly with the weight fraction of the fiber
(Table 5). The composite with 30 wt.-% fiber content
exhibits impact (izod) strength of 80.3 J  m1. The high
toughness of this natural fiber polymer composite places it
in the category of tough engineering materials. The quality
enhancement of PALF has been tried through different
surface modifications, such as dewaxing, alkali treatment,
cyanoethylation, and grafting of AN onto dewaxed PALF.
Amongst all the modifications, 10% AN-grafted PALF
composite exhibited maximum tensile strength whereas
cyanoethylated PALF composite exhibited better flexural
and impact (izod) strengths. Figure 5 and Table 6 present the
effect of surface modifications on the mechanical properties
of PALF-polyester composites.
The most widely used thermosetting matrix reinforced
by natural fibers is polyester.[90,91] Compression molding is
ß 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
964 S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen

Table 4. Effect of chemical treatment on mechanical properties of PALF-polyester composite (Fiber length ¼ 30 mm, Fiber content ¼
30 wt.-%).[88]

Type/nature of treatment Tensile strength Elongation at break Young’s modulus Flexural strength Flexural modulus
MPa % MPa MPa GPa
Untreated 52.9 3.6 2 290 80.2 2.76
2% NaOH (treated for 1 h) 55.4 4.7 1 460 77.4 2.93
Silane A172 73.5 4.3 – 85.6 –
Silane A1100 52.7 3.5 2 690 79.6 2.84
Glacial acetic acid and 42.7 3.6 2 260 71.5 2.55
acetic anhydride

the most widely used and convenient method to make these
composites, whether the fiber is long or short. The tensile
and impact (izod) properties of these composites have been
studied by Sanadi et al.[90] Comparison of the impact
properties of different natural fiber-reinforced composites,
including sisal, pineapple, banana, and coir shows that sisal
fiber composites possess the highest impact (izod) tough-
ness owing to the optimal microfibrillar angle of the fiber.
The properties of sisal fiber-reinforced polyester compo-
sites can be improved when sisal fibers are suitably modified
with surface treatments. In the work by Singh et al.[86], it
was explained that the modified ‘‘interphase’’ is much less
stiff than the resin matrix and provides a deformation
mechanism to reduce interfacial stress concentration.[91]
Further, it may also prevent fiber-fiber contacts, hence
removing the sources of high stress concentrations in the
final composites. The effect of fiber surface treatment on
the mechanical properties under wet conditions has also
been studied.[77] The results show that improving interfacial
adhesion can reduce moisture-induced degradation of
composites. Treated fiber composites absorb moisture at a
slower rate than the untreated counterparts, probably be-
cause of the formation of a relatively more hydrophobic
matrix interface region by co-reacting organo-functionality
of the coupling agents with the resin matrix. N-substituted
methacrylamide treated sisal fiber-reinforced polyester
composites exhibit better mechanical properties under dry
as well as wet conditions. Aligned sisal-polyester compo-
sites[92] developed from untreated sisal fiber do not have
good bonding with polyester matrix. But there is little
increase in the tensile strength of the composite with an
increase of the volume fraction of fiber. Mishra et al.[93]
have also reported on surface modified sisal-polyester bio-
composites. This article is concerned with the effectiveness
of various types and degrees of surface modifications of
sisal fibers involving dewaxing, alkali treatment, bleaching,
cyanoethylation, and vinyl grafting in enhancing the mech-
anical properties like tensile, flexural, and impact strengths
of sisal-polyester biocomposites. The mechanical proper-
ties are at an optimum at a fiber loading of 30 wt.-%. The
results in Figure 5 to 7 and Table 7 clearly show that among
all the modifications, cyanoethylation and alkali treatment
result in improved properties of the biocomposites. Cyano-
ethylated sisal-polyester composite exhibit the maximum
tensile strength (84.3 MPa), whereas 5% alkali treated sisal-
polyester composite exhibit the best flexural (153.9 MPa)
and impact strengths (197.9 J  m1), which are 21.8% and
20.9%, respectively, more than the control (i.e. untreated
sisal-polyester composite). Cyanoethylation of sisal, which
improves the mechanical properties of the ultimate com-
posite, is possibly due to the bonding of b-cyanoethyl group

Table 5. Impact (izod) strength of PALF-polyester composite

with different wt.-% of loading of control PALF.[89]

Fiber content Impact (izod) strength

wt.-% J  m1
0 14.8
10 64.6
Figure 4. Effect of fiber content (wt.-%) on mechanical 20 69.9
strengths (tensile and flexural) of PALF-polyester composite, 30 80.3
after ref.[89] 40 76.9

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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites 965

Figure 5. Effect of surface modification on mechanical strengths

(tensile and flexural) of PALF-polyester composite, after ref.[89] Figure 6. Effect of surface modification on tensile strength of
A) Untreated; B) Defatted; C) Alkali treated; D) Cyanoethylated; sisal-polyester composite, after ref.[93] A) Untreated; B) Defatted;
E) AN-grafted (5%); F) AN-grafted (10%); G) AN-grafted C) Alkali treated (5%); D) Alkali treated (10%); E) Bleached; F)
(20%). Cyanoethylated (50 8C); G) Cyanoethylated (60 8C); H)
Cyanoethylated (70 8C); I) AN-grafted (5%); J) AN-grafted
(10%); K) AN-grafted (20%); L) MMA-grafted (5%); M)
MMA-grafted (10%); N) MMA-grafted (20%).
of the fiber with the polyester matrix thereby improving the
fiber-matrix interaction. The superior mechanical proper-
ties of alkali treated sisal-polyester composite may be 4.1.2. Epoxy Composites
attributed to the fact that alkali treatment leads to fiber
From the interface improvement point of view, Bisanda and
fibrillation, i.e., breaking down of fiber bundle into smaller
Ansell studied the mechanical and physical properties of
fibers thereby increasing the effective surface area available
for contact with the matrix. Alkali treatment also improves
the fiber surface adhesive characteristics by removing
natural and artificial impurities which leads to a consider-
able increase in mechanical properties. In the case of vinyl
grafting, AN-grafted sisal-polyester composites show better
mechanical properties in comparison to MMA-grafted sisal
composites. The enhanced mechanical strengths of the
composites with optimum percentage of vinyl grafted
(10%) sisal may be due to increase in individual fiber
strength and due to increased adhesion between fiber and
matrix as the hydrophobicity of the fiber increases through
grafting.

Table 6. Impact (izod) strength of PALF-Polyester composite

with different surface treated PALF (PALF ¼ 30 wt.-%).[89]

Surface Treated PALF Impact (izod) strength

J  m1
Control 80.3 Figure 7. Effect of surface modification on flexural strength of
Defatted 81.4 sisal-polyester composite, after ref.[93] A) Untreated; B. Defatted;
Alkali treated 91.5 C. Alkali treated (5%); D. Alkali treated (10%); E. Bleached;
Cyanoethylated 102.0 F. Cyanoethylated (50 8C); G. Cyanoethylated (60 8C); H.
AN-grafted (5%) 76.9 Cyanoethylated (70 8C); I. AN-grafted (5%); J. AN-grafted
AN-grafted (10%) 83.3 (10%); K. AN-grafted (20%); L. MMA-grafted (5%); M.
AN-grafted (20%) 57.9 MMA-grafted (10%); N. MMA-grafted (20%).

Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de ß 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
966 S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen

Table 7. Impact (izod) strength of sisal-polyester composite with level off beyond 20% due to fiber-to-fiber interactions.
different surface treated sisal fiber (sisal ¼ 30 wt.-%).[94] From the dynamic viscoelastic properties, it has been found
Surface treated sisal Impact (izod) strength that 2 mm is the optimum fiber length for reinforcement.
The melt rheological behavior of short PALF/LDPE
J  m1 composites has been studied[98] using a capillary rheometer.
Control 163.6 The melt viscosity was found to increase with loading.
Defatted 172.8 Various chemical treatments have been made to improve
Alkali treated (5%) 197.9 fiber-matrix interfacial adhesion. Treatments based on poly-
Alkali treated (10%) 167.2
methylene-poly(phenyl isocyanate) (PMPPIC), silane, and
Bleached (75 8C) 171.2
Cyanoethylated (50 8C) 171.3 peroxide increase the viscosity of the system due to high
Cyanoethylated (60 8C) 192.5 fiber-matrix interfacial interaction. Viscosity of the system
Cyanoethylated (70 8C) 175.4 decrease with an increase of temperature. However, in
AN-grafted (5%) 160.3 peroxide-treated composites, viscosity is increased due to
AN-grafted (10%) 171.2
the crosslinking of composite at high temperature. The
AN-grafted (20%) 102.4
MMA-grafted (5%) 158.3 water absorption behavior of PALF/LDPE composites has
MMA-grafted (10%) 169.7 been investigated[99] with special reference to fiber loading,
MMA-grafted (20%) 99.4 the nature of the fiber/matrix interface, and temperature. It
is found that the uptake of water increases with fiber loading
owing to the increased cellulose content. The chemically
sisal fiber-reinforced epoxy composites.[94] Paramsivan and modified fiber composite exhibit a reduction in water
Kalam[95] suggested extensive application of sisal/epoxy uptake because of better interfacial bonding. The maximum
composites in consumer goods, low cost housing, and other improvement is observed in the case of isocyanate-treated
structures. These workers conducted experiments[95] to composites. Kinetic parameters such as diffusion, sorption,
incorporate sisal fibers in epoxy resins. The fabrication and permeability coefficients have been determined. By
process attempted by them included winding and lamina- using the Van’t Hoff relationship, the entropy and enthalpy
tion. It is found that the fabrication of these composites is of sorption have been estimated. The first-order rate
easy and cost of production is quite low. The tensile strength equation has been fitted to the system. The tensile properties
of the sisal-epoxy composites is found to be 250 MN  m2 of the composites were determined after immersion in
to 300 MN  m2; this value is nearly half the strength of water for different time intervals. The reduction in tensile
glass fiber-epoxy composites of same composition. But due properties is associated with the plasticization effect of
to low density (specific gravity) of sisal fiber, the specific water. Flexural strength and modulus of composite samples
strength (strength/specific gravity) of sisal composites is after exposure to UV light were studied. In the case of the
found to be about 8.5 GN  m2. Rong et al.[96] studied the unreinforced LDPE, the decrease in strength and modulus is
effect of fiber treatment on the mechanical properties of marginal. Addition of PALF does not have any significant
unidirectional sisal-reinforced epoxy composites. Treat- effect on the UV resistance.
ments including alkalization, acetylation, cyanoethylation, Due to the increasing use of thermoplastics, sisal fiber-
the use of silane coupling agent, and heating were carried reinforced thermoplastics have become increasingly impor-
out to modify the fiber surface and its internal structure. As tant. In 1993, Joseph et al.[100] used sisal fibers-reinforced
indicated by infrared spectroscopy, X-ray diffraction, and LDPE composites to investigate the effect of fiber length,
tensile tests, variations in composition, structure, dimen- fiber orientation, and processing conditions on the tensile
sions, morphology, and mechanical properties of the sisal properties. They observed that the tensile properties of sisal
fibers can be induced by means of different modification fiber-LDPE composites were sensitive to fiber length, fiber
methods. content, and fiber orientation. The composites prepared
from blends processed by a solution-mixing process exhi-
4.2. Thermoplastic Composites bited a uniform increase in their tensile strength and
modulus with fiber content. The composites also exhibited
4.2.1. Polyethylene Composites
maximum properties at a fiber length of about 6 mm.
George et al.[97,98] reported on the processing character- Unidirectional alignment of the fiber enhanced the strength
istics, viscoelastic properties, and mechanical behavior of and modulus of the composites along the axis of fiber
PALF/low density polyethylene (LDPE) composites. The alignment by more than twice compared to randomly orien-
effects of fiber orientation, fiber loading, and fiber length on ted fiber composites. The experimental tensile properties of
the viscoelastic properties of PALF/LDPE composites have short sisal fiber-reinforced LDPE with different fiber
been studied.[97] Longitudinally oriented composites show volume fractions have been compared with existing theo-
the maximum value of the storage modulus. Dynamic ries of reinforcement.[101] The models selected were
storage and loss modulus increase with fiber loading and the series and parallel,[102] Hirsch,[103] Halpin-Tsai,[104]

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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites 967

modified Halpin-Tsai,[105] Cox,[106] and modified Bowyer 4.2.2. Poly(propylene) (PP) Composites
and Bader[107] models. Bowyer and Bader’s model indicated
Joseph et al.[112] have studied the effect of processing vari-
that the tensile strength of the short fiber-reinforced thermo-
ables on the mechanical properties of sisal fiber-reinforced
plastic composites is the sum of contributions from sub-
PP composites. Composites were prepared by melt-mixing
critical and super-critical fibers and that from the matrix.
and solution-mixing methods. In the melt-mixing techni-
Electrical properties of sisal fiber-reinforced LDPE have
que, mixing parameters were optimized by varying the
been studied with respect to the effects of frequency, fiber
mixing time, rotor speed, and chamber temperature. A
content, and fiber length on the dielectric constant, volume
mixing time of 10 min, a rotor speed of 50 rpm, and a mixing
resistivity, and dielectric loss factor.[108] Sisal-LDPE com-
temperature of 170 8C were found to be the optimum
posites of 1 mm fiber length and 30 wt.-% fiber content were
mixing conditions. Under these conditions, melt-mixed
found to have the highest values of dielectric constants at all
composites showed better tensile properties than those of
frequencies. The dielectric constant, dielectric loss factor,
solution-mixed composites. The influence of fiber length,
and electrical conductivity of 25 wt.-% sisal-LDPE can
fiber loading, and fiber orientation on the mechanical pro-
be increased considerably by adding 5% carbon black. The
perties of sisal/PP composites has been evaluated. Treat-
electrical conductivity of hydrophobic LDPE can also be
ments with chemicals such as sodium hydroxide, maleic
improved by mixing it with hydrophilic lignocellulosic
anhydride, urethane derivative of PPG, and permanganate
fibers. A 25% sisal-LDPE composite containing 5% carbon
were carried out to improve the bonding at the fiber/
black can be used in anti-static applications to dissipate
polymer interface. It has been observed that all the treat-
static charges. The dielectric constant, volume resistivity,
ments enhanced the tensile properties of the composites
and dielectric loss factor of LDPE composites reinforced
considerably, but to varying degrees. Albano et al.[113] stud-
with raw and treated (alkali, stearic acid, benzoyl peroxide,
ied the effect of acetylated and non-acetylated sisal fiber on
dicumyl peroxide, permanganate, isocyanate, and acetyla-
the thermal degradation of blends of PP and polyolefins,
tion) sisal fibers have also been studied as a function of
specifically: PP/HDPE, PP/HDPE/functionalized (EPR),
frequency and fiber loading.[109] It is noted that in the case
and PP/HDPE/non-functionalized EPR. The studies have
of treated- and untreated-sisal fiber/LDPE composites, the
shown that the starting temperature of the decomposition of
dielectric constant decreases with an increase in frequency.
the fiber, whether treated or not, is maintained at almost at
The dielectric constant values were found to decrease
the same level. Acetylated fiber stability was also found to
following chemical treatments as a consequence of the low
be increased, because activation energy ranged between
sorption of water by the treated fiber. It was also observed
119 and 117 kJ  mol1; for non-acetylated fiber it was
that the dielectric constants of isocyanate- and stearic acid-
between 98 and 148 kJ  mol1. The activation energy of PP
treated-sisal fiber composites increased with fiber loading.
and PP/HDPE and PP/HDPE/functionalized and non-
The volume resistivity values for treated-sisal fiber/LDPE
functionalized EPR blends ranged between 250 and
composites are higher than those for raw sisal fiber/LDPE
180 kJ  mol1. When they were mixed with treated and
composites, i.e., the conductivity decreases as a result of the
non-treated sisal fiber, a sudden decrease in activation
surface treatments. The volume resistivity values for per-
energy was observed. This can be explained because mixing
manganate-treated-sisal fiber/LDPE composites depend
acetylated fiber with polymer results in high polymer-filler
upon the concentration of permanganate solution used.
interaction, which favors the thermal stability of the com-
The dielectric loss factor values were found to decrease as a
pounds. The dynamic mechanical properties of short sisal
result of chemical treatments. A strong relaxation is ob-
fiber-reinforced PP composites containing both untreated
served with a peak at frequency of 105.5 Hz for all the
and treated fibers have been studied by Joseph et al.[85] with
composites. Joseph and Thomas[110] reported the effect of
reference to fiber loading, fiber length, chemical treatments,
chemical treatment on the tensile properties of short sisal
frequency, and temperature. By the incorporation of short
fiber-reinforced polyethylene composites (both randomly
sisal fiber into PP, the storage moduli (E0 ) and loss moduli
and unidirectionally oriented) and analyzed the mechan-
(E00 ) have been found to be increased whereas the mech-
isms of different treatment methods like alkali treatment,
anical loss factor (tan d) decreased. The treated fiber
isocyanate treatment, i.e., treating fiber surface with ur-
composites show better properties compared to an untreated
ethane derivative of cardanol (CTDIC), peroxide treatment,
system. The use and limitations of various theoretical
i.e., benzoyl peroxide (BP) and permanganate treatment
equations to predict the tan d and the storage modulus of the
(KMnO4). It appears that the increase in the tensile property
fiber-reinforced plastic composites have been discussed.
values due to these treatments are in the order: CTDIC >
BP > KMnO4 > alkali. Environmental properties of sisal
4.2.3. Polystyrene (PS) Composites
fiber composites are very important because, as a natural
fiber, sisal aging causes degradation. The effect of ageing on The thermal behavior of PS composites reinforced with
the physical and mechanical properties of sisal fiber- short sisal fibers was studied by Nair et al.[114] by means
reinforced polyethylene composites has been studied.[111] of thermogravimetric and dynamic mechanical thermal

Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de ß 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
968
analyses. The thermal stability of the composites was found
to be higher than that of sisal fiber and the PS matrix. The
effects of fiber loading, fiber length, fiber orientation, and
fiber modification on the dynamic mechanical properties of
the composites were evaluated. Fiber modifications were
carried out by benzoylation, PS maleic anhydride coating
and acetylation of the fiber and the treatments improved the
fiber-matrix adhesion. PS/sisal composites are thermally
more stable than unreinforced PS and sisal fiber. The Tg
values of the composites are lower than that of unreinforced
PS and may be attributed to the presence of some residual
solvents in the composites entrapped during the composite
preparation.
4.2.4. Poly(vinyl chloride) (PVC) Composites
Yang et al.[115] studied sisal-PVC composites with respect
to the effects of fiber and matrix modification, processing
parameters on the mechanical and water resistance proper-
ties. Their main objective was to obtain the best processing
parameters and interface modification to make novel sisal-
PVC composites. But, their results showed that thermal
treatment, acetylation, and coupling agent improve neither
the interface nor the mechanical properties. These results
have been explained by the small fiber-volume fraction
(18.5%) of their composites and the melting processing
method that leads to the poor immersion of fibers in the PVC
matrix.
4.3. Rubber Composites
Bhattacharya et al.[116] reported on the mechanical proper-
ties of PALF-reinforced elastomer composites. Addition of
PALF to natural rubber increases hardness, compression
set, tear resistance, and Mooney viscosity but decreases
elongation at break, mill shrinkage, and Mooney scorch
time. The addition of resorcinol, hexamethylenetetramine,
and silica are essential for fiber-rubber adhesion. PALF-
reinforced natural rubbers filled with carbon black have
high hardness; low elongation, moderate tensile strength,
and moderate flex resistance properties.
Rubber is the second most widely used matrix for sisal
fiber composites behind polyethylene.[117–122] Rubber
matrices include natural rubber and styrene-butadiene
rubber (SBR). The main research areas are concerned with
the effect of fiber length, orientation, loading, type of bond-
ing agent, and fiber-matrix interaction on the properties of
composites, which include mechanical properties, rheol-
ogical behavior, thermal ageing, g-irradiation and ozone
resistance. Experimental results show that for best balance
of properties, the fiber length is about 6 mm. This is
the same as the sisal/PP composites. Orientation effects are
as expected. The efficiency of sisal as reinforcement in
rubber matrices is achieved by modifying the surface
topology of sisal fiber by suitable chemical treatment or by
Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de
S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen
selecting a bonding system. It has been observed that 18%
mercerization (caustic soda) treatment of sisal fiber
enhanced the bonding of fiber with the rubber matrix.[62]
When short fibers are not properly bonded with the rubber
matrix, they slide past each other under tension resulting in
low strength properties. Hence, interface adhesion between
short fiber composites is extremely important in designing
the properties of the composites. Interfacial adhesion be-
tween sisal and SBR has been improved by hydration,
mercerization, acetylation, benzoylation, SBR solution,
PS-MA treatment of sisal fibers, and by incorporation of an
RH bonding system.[123] The mechanical properties
increase upon various chemical treatments that is in the
order: SBR solution < PS-MA coating < mercerization <
acetylation < benzoylation. Varghese et al.[120] studied the
effect of acetylation and bonding agent on the ageing
properties of sisal fiber-reinforced natural rubber compo-
sites which included thermal ageing, g- radiation, and ozone
resistance. High fiber-volume fraction showed better resis-
tance to ageing, especially with fiber-surface treatment.
Increasing the dosage of gamma radiation was found to
increase the extent of the ageing process.
The rheological behavior of short sisal fiber reinforced
SBR composite has been studied by Kumar et al.[123] The
effects of shear rate, fiber loading, temperature, and the
extent of interface bonding on the viscosity of the system
have been examined. All the system showed pseudoplastic
behavior leading to the decrease of viscosity with increas-
ing shear rate. The incorporation of treated fibers increased
the melt viscosity and of the various chemical treatments,
the benzoylated fiber-reinforced composite showed max-
imum viscosity among all the mixes. The relative viscosity
of the composites was also found to increase with an
increase of the fiber loading.
4.4. Cement Composites
Due to the increased cost of conventional reinforcements
like steel, it is not possible to use them in low cost housing in
developing countries. Sisal has been explored as an additive
to concrete as a low cost substitute. Rohatgi et al.[124]
developed the chopped sisal-cement sheet by thoroughly
mixing chopped sisal fibers with cement. For further
improvement in strength of sisal-reinforced composites, a
steel fabric was also added to the sisal-cement mixture. The
load bearing capacity of this fiber-reinforced cement sheet
is found to be 2.5 kg  cm1 width. In order to improve the
bonding between fiber and cement, the surfaces of the fibers
were suitably treated prior to their addition to cement.
Sisal fiber-reinforced concrete beams have also been
developed by Khan and Shariff[125] and treated under pure
bending and torsion. The concrete was composed of 1.0 part
of ordinary Portland cement, 2.4 parts of sand, and 4.0 parts
of crushed granite rock. Sisal fibers of 0.35 mm diameter
having lengths of 2, 3, 4, 5, and 6 cm were used for the
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 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites
reinforcement. The mixing of concrete was done in a rotary
type of mixer. It was found that the ultimate flexural and
torsional strengths were linear functions of the percentage
of fiber content. The aspect ratio of fibers also affected the
strength and toughness of the composite in the case of pure
bending and torsion. From mechanical and economical
considerations sisal-cement composites appear to be suit-
able for some applications, but there is little information on
how well the sisal fibers bond to cement. Interfacial bond
strength of sisal bonded to cement matrix has been assessed
by several investigators.[124–126] Different techniques have
been used to determine the fiber-matrix bond strength in
composites.[127] These include pull-out measurements,
single filament tests, and the measurement of crack spacing
resulting from tensile tests.[128] The latter method requires
fairly large specimens. Aveston et al.[128] gave a method of
assessing interfacial bond strength, which depends on the
fact that in a brittle matrix reinforced with ductile fibers,
the tensile fracture will take place by multiple cracking in
the directions normal to the applied load.
Filho et al.[129] studied the durability of alkali-sensitive
sisal fibers in cement mortar composites. The composites
manufactured with short sisal and ordinary Portland cement
‘‘OPC’’ matrix presented a significant reduction in tough-
ness after six months of exposure to the open-air weathering
or after being submitted to cycles of wetting and drying. The
embrittlement of the composites can be mainly associated
with the mineralization of the fibers due to the migration of
hydration products, especially calcium hydroxide, to the
fiber lumen, walls and voids.
4.5. Other Matrix Composites
In 1992 Bisanda and Ansell[40] produced plain and corru-
gated laminated composites, from plain-woven mats of
mercerized sisal fiber impregnated with a cashew nut shell
liquid-formaldehyde resin having mean tensile strength of
24.5 MPa and Young’s modulus of 8.8 GPa. They observed
from bending tests that the corrugated composites had
adequate strength for roofing applications. To assess the
effect of simulated sunlight on composites as a function of
time, they also used dynamic mechanical thermal analysis.
After long irradiation times, they observed that the resin
component of the composite suffered further cross-linking
whilst the reinforcing cellulosic sisal fibers suffered some
degradation.
4.6. Hybrid Composites
Reinforcement by two or more fibers into a single matrix
leads to the development of hybrid composites with a great
diversity of material properties. It appears that the behavior
of hybrid composites is simply a weighted sum of the
individual components so that there is a more favorable
balance of properties in the resultant composite material.
Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de
969
Sisal and glass fibers are good examples of hybrid
composites[127,128,130 –132] possessing very good combined
properties. For sisal/glass fiber-reinforced LDPE compo-
sites, the effects of fiber orientation, composition, and fiber
surface treatment on the mechanical properties have been
studied. Due to superior properties of glass fibers, the
mechanical properties of the hybrid composites increased
with increasing volume fraction of glass fibers. ‘Positive’ or
‘negative’ hybrid effect is defined as ‘larger’ or ‘smaller’
than the properties calculated from the rule of mixtures of the
two constituent fiber-reinforced composites. A positive
hybrid effect has been observed for all mechanical properties
except the elongation at break. It is suggested that this effect
may be due to the increased fiber dispersion and orientation
with the increase in volume fraction of the glass fibers.
Yang et al.[132] studied the mechanical and interface
properties of sisal/glass fiber reinforced PVC hybrid com-
posites before and after immersion in water. It was found
that there exists a ‘positive’ hybrid effect for the flexural
modulus and unnotched impact strength but a ‘negative’
hybrid effect is caused by the poor interface between sisal,
glass and PVC matrix. They also suggested that water might
have a detrimental effect on the fiber-matrix interface
leading to a reduction in properties.
Recently, Mishra et al.[133] reported on the mechanical
properties of PALF/glass and sisal/glass fiber-reinforced
polyester composites. The tensile, flexural, and impact
strengths of PALF and sisal-reinforced polyester compo-
sites were observed to be improved by the incorporation of a
small amount of glass fibers in these composites, showing
positive hybrid effect. Optimum glass fiber loadings for
PALF/glass hybrid polyester and sisal/glass hybrid poly-
ester composites are 8.6 and 5.7 wt.-%, respectively, under
the present experimental conditions adopted. Sisal/glass
hybrid polyester composites of different chemically modi-
fied sisal fibers are fabricated and tested. Among the dif-
ferent chemical modifications of the sisal fibers, 5% alkali
treatment produced optimum tensile and impact strengths
(about 28% and 16% more than that of the control), while
cyanoethylation resulted in the maximum increase in
flexural strength (about 10%) in the hybrid composites.
Figure 8 and Table 8 summarize the results of mechanical
properties of untreated and treated biofiber hybrid compo-
sites. It is also observed that water absorption tendency of
the hybrid composite (Table 9) decreases by the process of
hybridization and surface treatment of biofibers. In the case
of alkali treated, cyanoethylated, and acetylated sisal fibers
used in making composites with unsaturated polyester
resin, the extent of interaction is greater between the fiber
and the matrix than that of raw fiber in the composites due to
existence of more polar reactive functional groups on the
surface of the fiber. As a result of this, the whole composite
absorbs less water.
The mechanical properties of sisal-saw dust hybrid fiber
composites with phenol-formaldehyde resin as a reinforce-
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970
Figure 8. Effect of surface modification on mechanical strengths
(tensile and flexural) of sisal/glass hybrid polyester composite,
after ref.[133] A) Untreated; B) Alkali treated (5%); C) Alkali
treated (10%); D) Cyanoethylated; E) Acetylated.
ment have been studied by Thomas et al.[134] as a function of
sisal fiber loading. The fiber length used was 6 mm. It was
observed that mechanical properties (tensile and flexural)
increased with sisal fiber content. This is due to the fact that
the sisal fiber possessed moderately higher strength and
modulus compared to saw dust. The thermal conductivity
and thermal diffusivity of sisal/glass hybrid fiber-reinforced
polyethylene composites were analyzed by Kalaprasad
et al.[135] Hybridization of sisal with glass fibers increased
the thermal conductivity of sisal-reinforced polyethylene.
4.7. Biocomposites
Luo and Netravali[136] have reported the mechanical and
thermal properties of bio/green composites obtained from
PALF (with fiber content up to 28%) and Biopol1. The ten-
sile strength and modulus of the biocomposites increased
significantly as compared to pure Biopol1, in the long-
itudinal direction but decreased in the transverse direction
with an increase of fiber content. The interfacial and
Table 8. Impact (izod) strength of sisal/glass hybrid polyester
composites with different surface treated sisal fiber (sisal ¼
24.3 wt.-%, glass ¼ 5.7 wt.-%).[133]
Surface treated sisal Impact (izod) strength
J  m1
Control 143.8
Alkali treated (5%) 167.4
Alkali treated (10%) 147.2
Cyanoethylated 155.9
Acetylated 164.7
Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de
S. Mishra, A. K. Mohanty, L. T. Drzal, M. Misra, G. Hinrichsen
Table 9. Water absorption of hybrid composites.[133]
Composite samples Water absorption
(24h)
%
PALF-polyester 12.49
PALF/glass hybrid polyester 7.6
Sisal-polyester 10.59
Sisal/glass hybrid polyester 7.24
Sisal/glass hybrid polyester 5.55
(alkali treated sisal)
Sisal/glass hybrid polyester 5.82
(cyanoethylated sisal)
Sisal/glass hybrid polyester (acetylated sisal) 5.24
mechanical properties of PALF- Biopol1 green composites
with 20 to 30 wt.-% content of fibers placed in a 08/908/08
fiber arrangement have also been reported.[137] Recently,
Mishra et al.[138] studied the mechanical performance of
biofiber-reinforced polyester amide composites and eval-
uated their biodegradability. Various surface treatments of
sisal fiber-like mercerization, cyanoethylation, acetylation,
bleaching, and vinyl monomer (acrylonitrile) grafting were
carried out which results in improved mechanical perfor-
mance of the sisal-BAK 1095 composites. Mechanical
properties like tensile and flexural strength were optimized
at a fiber loading of 50 wt.-%. Amongst all the modifica-
tions, alkali treatment and acetylation resulted in improved
properties of the composites. Alkali treated sisal composite
showed about 20% increase in tensile strength whereas
acetylated sisal composite showed about 14% increase in
flexural strength (Figure 9) than the control (untreated sisal
Figure 9. Effect of surface modification on mechanical strengths
(tensile and flexural) of sisal-BAK 1095 composite, after ref.[138]
A) Untreated; B) Alkali treated; C) Cyanoethylated; D) Acetyl-
ated; E) Bleached; F) AN-grafted.
ß 2004 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
 A Review on Pineapple Leaf Fibers, Sisal Fibers and Their Biocomposites
Figure 10. Effect of surface modification on biodegradation (%
weight loss) of sisal-BAK 1095 composite, after ref.[138] A)
BAK 1095; B) Untreated; C) Alkali treated; D) Cyanoethy-
lated; E) Acetylated; F) Bleached; G) AN-grafted.
composite). Surface treatments of fibers allowed better
wetting of fibers in matrix resin and thereby improving
the mechanical properties of the composite. However, the
bleached sisal-BAK composite showed a lower tensile
strength (45 MPa) than the control. This was attributed to
the lowering of fiber tensile strength due to delignification
(bleaching). Due to the loss of cementing material (lignin),
the tensile strength of the fiber decreased, which resulted in
a decrease in the tensile strength of bleached sisal com-
posite. From the biodegradation study (Figure 10), it has
been found that after 60 d of soil burial about 12% weight
loss is observed for BAK 1095 whereas acetylated sisal-
BAK 1095 composite shows maximum weight loss (22%).
It also shows maximum decrease in flexural strength (47%)
after 15 d of soil burial. A comparative account of properties
of PALF-BAK 1095 and sisal-BAK 1095 is given in
Table 10.
5. Conclusion
The composites made up of two biofibers, PALF and sisal
aim to partially replace the conventional and pollution
Table 10. Comparative account of properties of untreated
biofiber-polyester amide (BAK 1095) composites (fiber content
50 wt.-%).[138]
Property Sisal-BAK PALF-BAK
Tensile strength/MPa 59.9 29.6
Flexural strength/MPa 78.1 40.0
Weight loss/% 8.2 9.2
Decrease in flexural strength/% 23.0 11.0
Macromol. Mater. Eng. 2004, 289, 955–974 www.mme-journal.de
971
causing fibers, such as glass, carbon, borosilicate, aramid,
etc., in the composite industry, so that economical engi-
neering can be provided to the plastic industry for multiple
applications. The mechanical and physical properties of
these natural fibers vary considerably and are determined by
the chemical and structural composition of the fibers.
Natural fibers are themselves cellulose-reinforced materials
and the cellulose content and microfibrillar angle determine
the mechanical properties of the fiber.
PALF and sisal fibers can be used as reinforcements in
various thermoset, thermoplastic, rubber, and cement resin
matrices. These fibers can also be used in the preparation of
hybrid composites with synthetic fibers such as glass fiber.
Technologies are being developed to prepare biocomposites
from these biofibers and existing biodegradable polymers.
However, natural fiber (PALF/sisal) reinforced composites
generally have poor interface and moisture resistance
properties. The mechanical properties of composites are
influenced mainly by the adhesion between fibers and
matrix. So, various surface (chemical/physical) modifica-
tion methods of fibers have been developed in order to alter
the adhesion properties. Mechanical properties, moisture
resistance and biodegradation are improved by these
pretreatments of fibers.
Acknowledgements: M. Misra and A. K. Mohanty are thankful
to DST, New Delhi, India and Aerocom Pvt. Ltd., Orissa, India for
financial support in form of sanctioning a Research Project to carry
out the present investigation. S. Mishra is thankful for Junior
Research Fellowship in the said Research Project. Help rendered
by CIPET, Bhubaneswar, India and Dept. of Geology, Lucknow
University, Lucknow, India is gratefully acknowledged. A. K. M.
and G. H. are thankful to the Alexander von Humboldt Foundation,
Germany for an AvH fellowship.
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