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Composites Science and Technology 61 (2001) 1303–1310

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The influence of fibre treatment on the performance


of coir-polyester composites
J. Rout a, M. Misra b, S.S. Tripathy a, S.K. Nayak c, A.K. Mohanty b,*
a
Polymer and Composite Laboratory, Post Graduate Department of Chemistry, Ravenshaw College (Autonomous), Cuttack 753003, Orissa, India
b
Composite Materials and Structures Center, Michigan State University, 2100 Engineering Building, East Lansing, MI 48824, USA
c
Central Institute of Plastic Engineering and Technology, B-25, CNI Complex, Patia, Bhubaneswar, Orissa, India

Received 19 June 2000; received in revised form 18 January 2001; accepted 13 February 2001

Abstract
Surface modifications of coir fibres involving alkali treatment, bleaching, and vinyl grafting are made in view of their use as
reinforcing agents in general-purpose polyester resin matrix. The mechanical properties of composites like tensile, flexural and
impact strength increase as a result of surface modification. Among all modifications, bleached (65 C) coir-polyester composites
show better flexural strength (61.6 MPa) whereas 2% alkali-treated coir/polyester composites show significant improvement in
tensile strength (26.80 MPa). Hybrid composites comprising glass fibre mat (7 wt.%), coir fibre mat (13 wt.%) and polyester resin
matrix are prepared. Hybrid composites containing surface modified coir fibres show significant improvement in flexural strength.
Water absorption studies of coir/polyester and hybrid composites show significant reduction in water absorption due to surface
modifications of coir fibres. Scanning electron microscopy (SEM) investigations show that surface modifications improve the fibre/
matrix adhesion. # 2001 Elsevier Science Ltd. All rights reserved.
Keywords: Surface modification; Coir-polyester composite; Hybrid composite; Mechanical properties; Water absorption

1. Introduction lignocellulosic based fibres [2]. The efficiency of a fibre-


reinforced composite depends on the fibre/matrix inter-
Growing environmental awareness throughout the face and the ability to transfer stress from the matrix to
world has triggered a paradigm shift towards designing the fibre. This stress transfer efficiency plays a dominant
materials compatible with the environment. The use of role in determining the mechanical properties of the
biofibres, derived from annually renewable resources, as composite.
reinforcing fibres in both thermoplastic and thermoset In natural lignocellulosic fibres, cellulose is the main
matrix composites provide positive environmental ben- component. The elementary unit of a cellulose macro-
efits with respect to ultimate disposability and raw molecule is anhydro-d-glucose, which contains three
material utilization [1]. The advantages of natural lig- hydroxyls (OH). These hydroxyls form hydrogen
nocellulosic fibres over traditional reinforcing materials bonds inside the macromolecule itself (intra-molecular)
such as glass fibres, talc and mica are acceptable specific and also with hydroxyl groups from moist air. There-
strength properties, low cost, low density, non- fore, all natural fibres are hydrophilic in nature and
abrasivity, good thermal properties, enhanced energy their moisture content can reach 3–13% [3]. The inter-
recovery, and biodegradability. The main bottle necks nal adhesion can be improved by modifying the surface
in the broad use of these natural fibres in various poly- topology of fibres by a suitable pre-treatment or by
mer matrixes are poor compatibility between the fibres selecting the proper components of the bonding system.
and the matrix, and the inherent high moisture absorp- Coir is an important lignocellulosic fibre obtained
tion, which brings about dimensional changes in the from coconut trees which grow extensively in tropical
countries. Because of its hard-wearing quality, dur-
ability and other advantages, it is used for making a
* Corresponding author. Tel.: +1-517-353-5466; fax: +1-432-1634. wide variety of floor furnishing materials, yarn, rope etc
E-mail address: mohantya@egr.msu.edu (A.K. Mohanty). [4]. However, these traditional coir products consume
0266-3538/01/$ - see front matter # 2001 Elsevier Science Ltd. All rights reserved.
PII: S0266-3538(01)00021-5
1304 J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310

only a small percentage of the potential total world Bleaching of deffated fibres was done by the following
production of coconut husk. Hence, research and process: the fibres were carefully kept in 0.7% textone
development efforts have been underway to find new use (sodium chlorite) solution in the liquor ratio 50:1 buffered
areas for coir, including utilization of coir as reinforce- by 1% acetic acid and sodium acetate solution at pH 4
ment in polymer composites [5–11]. Unfortunately, the and temperature range 65–85 C for 2 h. The bleached
performance of coir as a reinforcement in polymer fibres were then carefully and thoroughly washed with
composites is unsatisfactory and not comparable even 2% sodium bisulfite (antichlor) for 15 min at room tem-
with other natural fibres due to its low cellulose content perature followed by washing with distilled water and
(36–43%), high lignin content (41–45%) and high finally air dried. The colour change of fibre from dark
microfibrillar angle. Morphological studies of coir fibres brown to silvery white was observed due to removal of
show the outer sheath of lignin that develop the cellu- lignin.
lose ultimates. The removal of this surface layer of lig-
nin usually results in a better and more stable bond. 2.3. Composite fabrication and testing
Keeping in view the above facts in our present investi-
gation, we have chosen alkali treatment, bleaching and Non-woven aligned mats (8.500 8.500 ) were used for
graft copolymerization as surface treatments for coir composite fabrication with polyester resin in a close
fibres in order to obtain better adhesion of these fibres mold. First, the mold was polished and then mold
with the polyester resin. The mechanical properties like releasing agent was applied on the surface. General pur-
tensile, flexural and impact strength of coir-polyester pose polyester resin was mixed with 1 wt.% cobalt
and hybrid composites are determined. The improved naphtenate (accelerator) and 1 wt.% methyl ethyl ketone
fibre-matrix adhesion has been examined by scanning peroxide (catalyst). The resin mixture was degassed in a
electron microscopy (SEM). vacuum desicator and then poured on to the mat placed
in the mold. When the mat was completely wet by the
resin, the mold was closed, pressed and cured at room
2. Experimental temperature for 24 h. For hybrid composites a glass mat
(8.500 8.500 ) was uniformly coated with polyester resin
2.1. Materials mixture (containing accelerator and catalyst) and placed
on the mold. A nonwoven coir mat was placed on this
Bristol coir fibres were collected from Aerocom Indus- and was coated with the resin. A second glass mat
try Pvt. Ltd., Orissa, India. General purpose polyester coated with resin solution was then placed on top of the
resin (FB-333), methyl ethyl ketone peroxide (MEKP) coir mat and a slight pressure was applied with a steel
and cobalt napthenate were obtained from Ruia Chemi- roller to remove the entrapped air. The mold, then
cals Pvt. Ltd., Calcutta, India. Acrylonitrile (AN) has closed, received slight pressure and was cured at room
been purified according to the usual procedure [12]. Che- temperature for 24 h.
micals and solvents like sodium hydroxide, ethanol, Tensile and flexural tests of the composite specimens
benzene, copper sulphate, sodium periodate, sodium were carried out at 23 C and 55% RH using UTM
chlorite and sodium bisulfite were of AnalaR grade and (Universal Testing machine) LR-100K, Lloyds Instru-
were used without further purification. ment Ltd., UK as per ASTM-D638, at a cross head speed
of 100 mm/min, gauge length 50 mm and ASTM-D 790,
2.2. Methods of surface modification at a cross head speed of 2.8 mm/min, gauge length of 100
mm, respectively. The notched izod impact energy was
The coir fibres were first scoured with hot detergent determined by impactometer (CEAST Italy) as per
solution (2%) at 70 C for 1 h and washed with distilled ASTM-256. All the results were taken as the average
water and finally dried in vacuum oven at 70 C. The value of five samples.
fibres were then extracted in a 1:2 mixture of ethanol and
benzene for 72 h to dewax the sample, followed by wash- 2.4. Water absorption
ing with distilled water and air drying. The fibres thus
obtained were known as dewaxed or deffated fibres. The water absorption test of the coir-polyester and
The defatted fibres were treated with NaOH solution hybrid composites was carried out as per ASTM D-570
of varying concentrations (2–10%) for 1 h at 300 C with method.
occasional shaking followed by washing with distilled
water for several times to leach out the absorbed alkali. 2.5. Scanning electron microscopy (SEM)
The fibres were dried and treated as alkali treated fibres.
Alkali treated coir fibres (5%) were subjected to graft The surfaces of the fractured specimens under tensile
copolimerization with AN using Cu2+–IO 4 combina- and impact tests were examined using a scanning elec-
tion as initiator in an aqueous medium [13]. tron microscope (SEM) Jeol JSM-T 330 A. All specimens
J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310 1305

were sputtered with a 10 nm thick layer of gold prior to composites. The 5% NaOH treated fibre composite
SEM observations. improves the FS by 17% in comparison to untreated
fibre composite. For 10% NaOH treated fibre compo-
sites, both the TS and FS decrease. The enhancement in
3. Results and discussion mechanical properties in alkali treated (2 and 5%) fibre
composites is attributed to the improved wetting of
Coir/polyester composites with 17 wt.% of fibre alkali treated coir with polyester [8]. Morphological
loading was prepared to investigate the effect of surface studies of untreated coir fibre surfaces shows that the
modifications on mechanical properties like tensile surface contains globular protrusions at regular inter-
strength (TS), flexural strength (FS) and impact strength vals [15]. Voids are produced on the surface of coir by
(IS) of composites. We have reported earlier that coir- NaOH treatment as a result of the removal of these
polyester composites with 17–25 wt.% of coir fibres show globular protrusions which would increase the mechan-
optimum mechanical properties [14]. While studying the ical interlocking between the fibre and the polyester resin.
effects of various surface modifications of coir fibres on The decrease in mechanical properties in the case of 10%
mechanical properties of coir/polyester composites, alkali treated fibre composites may be due to cell wall
untreated coir-polyester composite was taken as stan- thickening which leads to poor adhesion with polyester
dard material for comparison. resin.
The impact strength of untreated and NaOH treated
3.1. Effect of alkali treatment (2–10%) coir-polyester composites (17 wt.% fibre load-
ing) is shown in Table 1. With incorporation of 2%
The effect of alkali treatment (2–10%) of coir fibres on NaOH treated fibre, the IS increases from 433.5 J/m
TS and FS of composites (containing 17% fibre by weight) (untreated) to 521.9 J/m and with further increase in
can be readily assessed from Fig. 1. NaOH (2%) treated NaOH concentration (5%) increases the IS to 634.6 J/
fibre polyester composites improve the TS and FS by 26 m. This large increase in IS is due to toughness of the
and 15%, respectively, in comparison to untreated fibre coir fibres [14]. At still higher NaOH concentration
polyester composites. With further increase in NaOH (10%), the IS decreases in comparison to 2 and 5%
concentration from 2 to 5%, the TS decreases whereas FS NaOH treated fibre composites but the value is higher
increases in comparison to 2% NaOH treated fibre than the IS value of untreated fibre composite.

Fig. 1. Effect of alkali treatment on TS and FS of coir-polyester composite.


1306 J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310

3.2. Effect of bleaching composites. This is attributed to lowering of the fibre


tensile strength due to loss of the cementing material
The effect of bleaching of coir fibres on TS and FS of (lignin) which results in a decrease in TS of coir-polye-
coir-polyester composites (17 wt.% fibre) is shown in ster composites. But the bleached fibre polyester compo-
Fig. 2. The bleached coir-polyester composites show a sites show better FS than the untreated fibre composite.
slight reduction in TS in comparison to untreated fibre Coir fibres bleached at 65 C show an increase in FS by
 20% in respect of composite. Bleached fibres (at 75
Table 1 and 85 C) also show an improvement in FS in compar-
Effect of surface modification on IS of coir-polyester and glass/coir- ison to untreated fibre polyester composite but these
polyester hybrid composites
values are lower than the FS of bleached fibre (65 C)
Surface Impact strength (J/m) polyester composite. Similar results have also been
modification reported in the literature for bleached jute polyester
Coir-polyester Glass/coir-polyester
composite [16]. The improved FS may be due to less
hybrid
stiffness and more flexible character of the fibres after
Untreated 433.5 576.0 delignification. The bending forces (flexural) are better
propagated along the longitudinal direction of the fibres
Alkali treatment
Alkali treated (2%) 521.9 –
in case of bleached coir-polyester composites. This may
Alkali treated (5%) 634.6 687.8 again due to high fibre-matrix bonding strength in
Alkali treated (10%) 494.7 – bleached fibre composites.
The effect of bleaching of coir fibres on IS of resulting
Bleaching composites (17 wt.% fibre content) is shown in Table 1.
Bleached (65 C) 458.3 593.0
Bleached (75 C) 425.2 –
The improvement in IS may be due to better wetting of
Bleached (85 C) 389.8 – bleached fibres with polyester resin.

AN-grafting 3.3. Effect of grafting


AN-grafted (5%) 477.0 –
AN-grafted (10%) 596.3 629.8
AN-grafted (15%) 189.7 –
Fig. 3 represents the effect of AN-grafting (varying
from 5 to 15%) onto coir fibres on TS and FS of the

Fig. 2. Effect of bleaching temperature ( C) on TS and FS of coir-polyester composite.


J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310 1307

Fig. 3. Effect of AN-grafting on TS and FS of coir-polyester composite.

Fig. 4. Effect of surface modification on TS and FS of glass/coir-hybrid composite: A, untreated; B, alkali treated (5%); C, AN-grafted (10%); D,
bleached (65 C).
1308 J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310

resulting composites (17 wt.% fibre). While studying 3.4. Hybrid composites
grafting effect untreated coir composite is taken as stan-
dard material for comparison. In case of 5% AN-grafted Hybrid composites are prepared with untreated, 5%
coir composites, both the TS and FS increases margin- alkali treated, 10% AN-grafted and bleached (65 C)
ally but with increase in grafting (10%), both TS and FS coir fibres (13 wt.%) in combination with glass fibre (7
increases by 14 and 15%, respectively. With further wt.%) in polyester resin.
increase in AN grafting (i.e. at 15%) the TS and FS The effect of different types of surface modifications,
decrease drastically. The improved TS and FS of AN- i.e. alkali treatment (5%), AN-grafting (10%) and
grafted (5 and 10%) fibre composites may be due to bet- bleaching (65 C) of coir fibres on TS and FS of hybrid
ter wettability and adhesion between the grafted fibres composites is shown in Fig. 4. The untreated coir hybrid
and the matrix polymer [14]. The decrease in TS and FS composite is taken as standard material for comparison.
at higher percentage of AN grafting (15%) is due to the In comparison to alkali treated (5%) and bleached
fact that at higher percentage of grafting the fibre (65 C) coir hybrid composites, 10% AN-grafted coir
strength reduced drastically and fibre becomes porous hybrid composite shows better TS (45.80 MPa) as well as
for which composite prepared from it become weak. better FS (110.9 MPa). Alkali treated coir hybrid com-
The effect of different extent of AN-grafting onto coir posites (5%) improve the TS by 8.25% and FS by 19%
fibres on izod impact strength of the resulting composite in comparison to untreated coir hybrid composites. For
is represented in Table 1. As observed in TS and FS, the bleached (65 C) coir hybrid composite an improved
IS of AN grafted fibre composites increases upto graft- flexural strength (109.7 MPa) is found although the
ing percentage of 10%. At higher AN-grafting (15%), sample does not show any improvement in TS.
the IS of resulting composites decrease drastically. The The IS values of untreated and different surface
impact performance of the AN-grafted coir composites modified coir hybrid composites are shown in Table 1.
may be attributed to several factors such as fibre rigid- Alkali treated coir hybrid composites (5%) show better
ity, interfacial stress resistance, fibre aspect ratio etc. impact strength of 687.8 J/m. Hybrid composites with

Fig. 5. SEM of tensile fractured surfaces of: (a) and (b) untreated coir-polyester composite; (c) AN-grafted (10%) coir-polyester composite; (d)
alkali treated (5%) coir-polyester.
J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310 1309

10% AN-grafted fibres improve the impact strength by coir composites. In case of surface modified coir fibre
9.32% in comparison to untreated coir hybrid compo- composites, the fibres get masked with the polyester
sites. Bleached (65 C) coir hybrid composites show a resin in the laminate with a stronger adhesion resulting
marginal improvement in IS value. in greater hydrophobicity and lesser water absorption.
The water absorption of glass reinforced coir polyester
3.5. Water absorption composites is less than that of coir polyester composites.
In case of glass reinforced coir-polyester composites the
The water absorption behaviors of untreated and fibres are arranged in randomly close packed manner in
surface modified coir polyester composites as well as which water impermeable glass fibres act as barriers and
coir/glass hybrid polyester composites are studied prevent the contact between water and hydrophilic coir
(Table 2). The extent of water absorption decreases fibres and hence prevent the water absorption of coir
considerably on surface modification of coir fibres. AN- fibres.
grafted fibres (10%) show considerable reduction in
water absorption (4.119%) which again confirm a better 3.6. Scanning electron microscopy
adhesion between AN-grafted fibres with polyester
resin. The water absorption values of alkali treated Interface studies of untreated and surface modified
(5%) and bleached (65 C) coir polyester composites are coir-polyester and glass reinforced coir-polyester com-
also considerably less than the untreated coir polyester posites are carried out to investigate fibre splitting, fibre
composites. In case of untreated coir polyester compo- pull-out, de-bonding, matrix cracking and fibre-matrix
sites the poor wettability and adhesion between untreated interaction by scanning electron microscopy. Fig. 5
coir towards polyester resin are attributed to the hydro- shows a comparison of the tensile fractured surfaces of
philic nature of coir fibre. This hydrophilicity is respon- 10% AN-grafted coir and 5% alkali treated coir com-
sible for the higher percentage water uptake in untreated posites with untreated coir composites. Fig. 5(a) shows

Fig. 6. SEM of impact fractured surfaces of: (a) untreated coir hybrid composite; (b) AN-grafted (10%) coir hybrid composite; (c) bleached (65 C)
coir hybrid composite.
1310 J. Rout et al. / Composites Science and Technology 61 (2001) 1303–1310

Table 2 coir composites. Bleached (65 C) coir composites show


Effect of surface modification on water absorption of coir-polyester better flexural strength (61.6 MPa) which is  20%
and glass/coir polyester hybrid composites
more than the FS of untreated fibre composites. It is
Surface Water absorption (%) also observed that water absorption tendency of the
modification composites decrease by surface modification of fibres as
Coir-polyester Glass/coir-polyester well as hybridization. It can be predicted that with coir
hybrid
fibre reinforcement the best properties of glass-fibre-
Untreated 8.530 5.186 reinforced plastics cannot be achieved, above all
Alkali treated (5%) 4.994 3.147 because of the big difference between the modulus of
Bleached (65 C) 5.861 3.718 elasticity of the glass and coir fibres. However, from the
AN-grafted (10%) 4.119 2.997
above discussions we can say that surface modified coir
fibres and polyester matrix can be molded into a cost-
the fractured surface of untreated coir composite with effective but value added composite materials.
fibre pull outs and many holes that left after the fibres
are pulled out from the matrix when stress is applied.
The failure occurs at the weak fibre/matrix interface. Acknowledgements
Fig. 5(b) shows the incompatibility of untreated fibre
surface with the polyester matrix. The fractured surface A.K.M. and M.M. are thankful to the Department of
of 10% AN-grafted coir composite [Fig. 5(c)] shows a Science and Technology, New Delhi, India and Aero-
reduction in fiber pullout with good dispersion of fibres com Pvt. Ltd., Bhubaneswar, Orissa, India for financial
in the matrix. Fig. 5(d) shows pulled-out fibres along grants to carry out this research work.
with the existence of cracks at the broken fibre ends/
sites in 5% alkali treated coir-polyester composite sug-
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