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Composites Science and Technology 60 (2000) 833±844

E€ect of wettability and ageing conditions on the physical and


mechanical properties of uniaxially oriented jute-roving-reinforced
polyester composites
A.C. de Albuquerque a, Kuruvilla Joseph a,1, Laura Hecker de Carvalho a,*,
Jose Roberto Morais d'Almeida b
a
Materials Science Engineering Department, Federal University of Paraiba, UFPB/CCT/DEMa-Av. Aprigio Veloso,
882-58109. 970-Campina Grande-PB, Brazil
b
Departamento de Ciencia dos Materiais e Metalurgia (DCMM), Ponti®ca Universiade Catolica do Rio de Janeiro (PUG-RJ),
Rua MarqueÃs de SaÄo Vicente 225, CEP 22453-900, Rio de Janeiro, RJ, Brazil

Received 18 March 1999; received in revised form 26 October 1999; accepted 18 November 1999

Abstract
In order to obtain reliable composite materials in structural applications and to utilise fully the potential of reinforcing ®bres,
both perfect impregnation and strong interfacial bond formation have to be guaranteed. In the present study the tensile, ¯exural,
and impact behaviour of jute roving reinforced polyester composites were investigated as a function of ®bre loading and ®bre sur-
face wettability. Two types of unsaturated polyesters viz; (a) Resana having a wetting agent and (b) Elekeiroz without wetting
agent, were used to study the in¯uence ®bre surface wettability. It was noted that Resana polyester composites showed mechanical
properties superior to those of Elekeiroz composites. The impact strength of the Resana polyester composite with 30% ®bre content
was found to be 80 J/M2, which is about 350% higher than that of the polyester matrix. Jute rovings were alkali treated in 10%
aqueous NaOH solution for 3 h periods under two di€erent conditions, i.e. (a) immersion at room temperature and (b) re¯ux at
100 C. It was observed that jute rovings re¯uxed in alkali for 3 h showed better tensile properties than those treated at room tem-
perature. The mechanical properties of the jute Resana polyester composites were evaluated under three ageing conditions, i.e. (1)
immersion in water at 50 C for 48 h (2) under re¯ux in water for 2 h; and (3) thermal ageing in an air circulating oven at 100 C for
periods up to 8 days. Our results indicate that the composites re¯uxed in water for 2 h showed a slight improvement in their tensile
properties compared to those of immersion-aged composites. It was observed that thermal ageing tended to decrease the composite
mechanical properties, which was attributed to oxidative degradation of both ®bre and matrix. # 2000 Elsevier Science Ltd. All
rights reserved.
Keywords: Jute rovings; Polyester; composites; Ageing; Wettability; Mechanical properties

1. Introduction petroleum-based products, it is important to use natu-


rally occurring alternatives. In many parts of the world,
In recent years short-®bre-reinforced polymer com- apart from agricultural uses, di€erent parts of the plants
posites have gained great importance because of their and fruits of many crops have been found to be viable
advantages of processing, anisotropy in properties and sources of raw materials for industrial purposes. The
easy dispersion. In fact synthetic ®bres such as nylon, use of natural ®bres in polymer matrices is highly bene-
rayon, aramid, glass and carbon are used extensively ®cial because the strength and toughness of the resulting
for the reinforcement of plastics. Nevertheless, these composites are greater than those of the unreinforced
materials are expensive and non-renewable. Because of plastics. Moreover, cellulose-based natural ®bres are
the uncertainties prevailing in the supply and price of strong, light in weight, cheap, abundant and renewable.
Recently, cellulosic products and wastes such as shell
* Corresponding author. ¯our, wood ¯our and pulp have been used as ®llers in
1
Permanent address Ð Department of Chemistry, St. Berchman's polymers, primarily to achieve cost savings [1,2]. Several
college, Changanacherry, Kottayam, Kerala, India. researchers in di€erent parts of the world have reported
0266-3538/00/$ - see front matter # 2000 Elsevier Science Ltd. All rights reserved.
PII: S0266-3538(99)00188-8
834 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

on the use of natural ®bres as reinforcing agents in studies have been reported on various types of chemical
thermosetting and thermoplastic polymers [3±18]. treatments to jute ®bres. Varma and co-workers [28±30]
Freiscmidt [3] reported the mixing of wood ®bres into have extensively studied various types of chemical
dough-moulding compounds (DMC). McKenzie and treatments on natural ®bres especially jute ®bres. They
Yuritta [4] reported on the improvement in tensile have reported that jute ®bres modi®ed by treatment
strength bought about by the use of wood ®bres as a with Y-aminopropyl trimethoxy silane, isopropyl trii-
®ller in polyethylene and other polymers. Zadorecki and sostearyl titanate and toluene diisocyanate had lower
Michell [5] have studied the e€ects of wood ¯our in moisture regain and are, therefore, potential candidates
phenolics and aminoplastics. The use of aspen in the for reinforcement of organic matrix resins. Some studies
form of chemi-thermo mechanical pulp (CTMP) has on imparting hydrophobicity to jute ®bres have been
been reported by Beshay [6]. Maldas [7,8] and Raj et al. carried out by coating with lignin or polyesteramide
[9,10] have studied the e€ects of di€erent coupling polyol [31]. It has been observed that jute ®bres require
agents and ®bre treatments on the mechanical proper- a large quantity of resin to wet the ®bres due to its por-
ties of thermoplastic composites reinforced with cellu- ous nature and a good portion of this resin is squeezed
lose ®bres. Joseph et al. [11±18] reported on the use of out by the application of pressure during moulding [32].
sisal ®bre as a potential reinforcing agent in poly- Sridhar et al. [26] have reported that lignin coating has
ethylene, natural rubber, and various thermosets such been shown to bring down the resin consumption with-
as epoxy, phenol-formaldehyde, and polyester. out exerting any deleterious e€ect on the properties of
Over the past decade, cellulose ®llers of a ®brous the ®bres. They have also reported that ethylene dia-
nature have been of great importance, because they give mine treatment on jute ®bres impart hydrophobicity
composites with improved mechanical properties com- and thereby reduced the moisture absorption. Anderson
pared to those containing non-®brous ®llers [19±23]. and Tillman [33] have studied the e€ect of acetylation
Lignocellulosic ®bres like sisal, jute, coir, pineapple and on the strength, rot resistance and hydrophobicity of
banana have been used as reinforcements in thermoset jute ®bres, It has been observed that acetylation imparts
matrices. Among these ®bres, jute is of particular inter- hydrophobicity to jute ®bres and also enhance the
est in that its composites have high impact strength in dimensional stability.
addition to having moderate tensile and ¯exural prop- Grafting of vinyl monomers such as methyl metha-
erties compared to other lignocellulosic ®bres [19]. crylate, ethyl acrylate, styrene, acrylonitrile and acryla-
Several studies have been reported on jute-reinforced mide onto jute ®bres have been extensively studied by
polymer composites, especially with epoxy, phenolic, and several researchers [34±38]. Samal et al. [34] have found
polyester matrices [24±27]. Mohan et al. [20] have an increase in moisture absorption of jute ®bres on graft
reported the compressive strength of jute/glass hybrid copolymerization with methacrylate and styrene, but
epoxy composites. Roe and Ansell [24] have studied the with an undesirable loss of tensile strength. Siddique et
mechanical properties of jute reinforced polyester com- al. [35] observed a decrease in moisture anity of jute
posites containing uniaxially oriented jute ®bres. Bhat- on graft copolymerization of arylonitrile, styrene or
tacharya et al. [25] have made composites with jute vinyl acetate. Mohanty et al. [36] have reported that
®bres in a phenolic resin. Sridhar et al. [26] have studied graft copolymerization of acrylonitrile onto acetylated
the tensile, ¯exural and impact properties of unidirectional jute ®bres improved the thermal stability and also the
and bi-directional jute/glass hybrid polyester composites. light fastness rating of jute ®bres dyed with basic dyes.
Varma et al. [27] have studied the mechanical properties Agarwal and Sreenivasan [37] have studied the graft
of hybrid composites of glass and modi®ed jute fabric in copolymerization of vinyl monomers onto jute ®bres
unsaturated polyester resin. An improvement in the using X-rays. Graft copolymeriztion of methyl metha-
mechanical properties of laminates was observed when crylate onto chemically modi®ed jute ®bres using
jute fabric was modi®ed by titanate treatment. KMnO4-malonic acid redox system has been reported
However, owing to the presence of hydroxyl and by Tripathy et al. [38]. It has been concluded that these
other polar groups in various constituents of jute ®bre, surface treatments attempted have been e€ective in
the moisture regain is high which leads to poor wett- improving the interfacial bonding, in reducing the resin
ability with resin and weak interfacial bonding between consumption, in ®lling of higher amount of ®bre and in
®bres and the relatively more hydrophobic matrices. lowering moisture absorption by the composites.
Environmental performance of such composites is gen- However, very limited studies have been reported in
erally poor as a result of delamination under humid the literature on the use of jute rovings as reinforcement
conditions. Therefore, in order to develop composites in polymer matrices. Therefore, a detailed investigation
with better mechanical properties and environmental has been carried out to study the in¯uence of wetting
performance, it is necessary to impart hydrophobicity to agent, alkali treatment and ageing conditions on the
the ®bres by chemical treatment with suitable coupling mechanical properties of uniaxially aligned jute roving
agents or by coating with appropriate resins. Several reinforced polyester composites.
A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844 835

Table 1
Properties of BYK-A515 wetting agent

Chemical characteristics Recommended Non volatile Density at Refractive Flash point


dosage (%) matter (%) 20 C (g/ml) index ( C)

Solution of foam destroying polymers, 0.1±0.5 20 0.82 1.440 40


silicone free based on total
formulation

2. Experimental Micro 350). The crosshead speed used on tensile testing


was 0.5 mm/min, while ¯exural testing was conducted at
2.1. Materials used 1.7 mm/min. The modules and elongation at break were
calculated from the load displacement curve. At least
Jute rovings, classi®ed as 10/4 (cord thick-CG), hav- ®ve specimens were tested for each set of samples and
ing an average diameter of 2.5 mm were supplied by the mean values were reported. Izod impact strength
Cia. Textile Castanhal in Brazil. Sodium hydroxide was measured on a TMI testing machine operating with
(NaOH) P.A. was used as received. Elekeiroz S.A and a 2J pendulum.
Resana S.A. supplied the pre-accelerated unsaturated
polyester resins. These resins have essentially the same 2.5. Ageing studies
characteristics except that Resana is formulated with a
wetting agent and Elekeiroz's is not. The wetting agent Thermal ageing was conducted in an air-circulating
used was BYK-A515 supplied by BYK chemicals, Bra- oven operating at 100 C. Test samples were removed
zil. The properties of the wetting agents are given in after 4 and 8 days periods. After being cooled down and
Table 1. conditioned at room temperature, the weights and
dimensions of each specimen were measured. Water
2.2. Fibre alkali treatment ageing studies were carried-out in two ways viz: (a)
under re¯ux in water for 2 h and (b) under immersion in
Jute rovings were alkali treated in 10% aqueous water at 50 C for 2 days. These samples were then dried
NaOH solution for 3 h periods under two di€erent between two sheets of ®lter paper and then the weight of
conditions, i.e. (a) immersion at room temperature and each specimen was measured. The mechanical proper-
(b) re¯ux at 100 C. In both cases, a proportion of 1 ml ties of these samples as a function of ageing were deter-
of 10% NaOH solution was used for every 0.15 g of mined using the procedures mentioned above.
®bre. After treatment the rovings were thoroughly
washed with running water and allowed to dry at room
temperature for 48 h before being used as reinforcement.

2.3. Preparation of composite sheets

Unidirectionally oriented jute rovings reinforced


polyester composites were prepared by aligning jute
rovings in a wooden board having arrays of nails as
shown in Scheme 1. A silicon coated glass plate was
placed at the bottom of the woven rovings, which were
pasted to the glass plate with silicone glue. A rubber
mould was placed over the glass and the polyester resin
mixed with a 1% MEK initiator was applied over the
®bres. Air bubbles were squeezed out by brushing to
ensure wetting of the rovings and the mould was then
carefully closed using silicon coated glass plate. The
system was kept under pressure for 24 h before
demoulding.

2.4. Mechanical testing of the composites


Scheme 1. Schematic diagram of the preparation of unidirectionally
Tensile and ¯exural tests have been carried out in oriented jute rovings± polyester composites; (a) Jute rovings waved in
accordance with ASTM D-638 and ASTM D-256 rules, wooden board having nails, (b) after ®xing the ends of the rovings in a
respectively, in a universal testing machine (Testometrics glass plate using silicone gum and placed in a rubber mould.
836 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

Table 2
In¯uence of wetting agent on the mechanical properties of jute rovings reinforced±polyester composites as a function of ®bre content

Type of resin used Fibre Tensile Young's Elongation at Flexural Flexural Flexural
content strength modulus break strength modulus de¯ection
(%) (MPa) (GPa) (%) (MPa) (GPa) (%)

Elekeiroz 0 46.1 0.68 7.96 72.6 2.19 3.46


10 49 0.8 6.31 72.6 2.5 1.98
20 64.7 0.93 6.7 96.1 3.13 2.64
30 62.8 0.93 6.64 96.1 3.13 2.75
Resana 0 38.1 0.81 5.98 72.7 2.2 2.88
10 48.6 1.29 4.97 71 3.54 1.92
20 63.7 1.39 6 104.7 3.98 2.53
30 68.7 1.4 6.15 115 4.25 2.9

2.6. Fracture surface morphology BYK ±A515, which is a highly surface-active air release
additive with ®bre wetting properties. A major limita-
The surface of the fractured specimens were gold tion of all high speed composite processing is the wet-
sputtered and observed on a Zeiss DSM 960 scanning ting of ®bres. Incomplete wetting or impregnation often
electron microscope (SEM) operating with secondary results in the formation of voids or air entrapment.
electron imaging at 10±20 kv. Although the occurrence of voids has been frequently
reported and is recognised as a major problem in com-
posites, the exact mechanism of void formation is not
3. Results and discussion clear due to its complexity [39]. From the theoretical
point of view, wetting can a€ect adhesion in two ways;
3.1. E€ect of ®bre surface wettability (a) incomplete wetting will produce interfacial defects
and thereby lower the adhesive bond strength by ¯aw-
Table 2 shows the e€ect of the matrix on the induced stress concentrations. (b) Good wetting can
mechanical properties of uniaxially oriented jute rovings enhance the adhesive bond strength by increasing the
reinforced-polyester composites. The enhanced thermodynamic work of adhesion, which is directly
mechanical properties exhibited by the composites pre- proportional to the fracture energy of the adhesive bond
pared with Resana's polyester resin are attributed to the [40]. In natural ®bre-reinforced polymer composites due
presence of a wetting agent in its formulation. Although to the divergent behaviour in polarity i.e. natural ®bres
both resins exhibit almost similar strength and modulus, are hydrophilic or polar in nature whereas, most of the
upon the vegetable ®bre addition slightly better tensile polymers are hydrophobic or nonpolar in nature, ®bre
strength and much better (up to 80%) modulus were to matrix adhesion is very poor. The above Table shows
obtained with Resana's. The increase in mechanical that the tensile strength and rigidity of the Resana
properties by the presence of a wetting agent clearly polyester composites increased with ®bre content, indi-
indicates the importance of ®bre surface wettability in cating that even up to 30% of ®bre loading ®bre surface
determining the physical and mechanical properties of wettability and interfacial bond strength are fairly good.
®bre reinforced composites. The wetting agent used was This can be clearly understood from Figs. 1 and 2. The
ability of the interfaces to transfer stresses from the
matrix to ®bre plays an important role in determining

Fig. 1. E€ect of ®bre content on the tensile strength of jute roving Fig. 2. E€ect of ®bre content on the tensile modulus of jute roving
reinforced Elekeiroz and Resana polyester composites. reinforced±Elekeiroz and Resana polyester composites.
A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844 837

the physical and mechanical properties of ®bre-reinforced formation of strong bonds have to be guaranteed for
composites. To utilise the full potential of the reinfor- reliable materials in structural applications. On the
cing ®bres, both perfect impregnation and wetting and other hand, a weak interfacial link providing increased
toughness by promotion of pullout e€ects can be desir-
able and bene®cial for energy-absorption purposes. The
adhesive bond itself may, in principle, be due to chemi-
cal, physical or mechanical (interlocking or anchoring)
links across the interface. Adhesion phenomena are not
only very complex, but they are also not fully under-
stood yet from a scienti®c point of view. Reinforcing
®bres are normally subjected to surface treatments to
improve their compatibility with the matrix. Adhesion
between ®bre and matrix cannot be achieved without
intimate contact i.e. unless the ®bre surface contacts the
resin on a molecular level. Fig. 3 a±c shows the SEM
photomicrographs of the tensile fracture surface of the
jute rovings±Resana polyester and jute±Elekeiroz
polyester composites. The better ®bre±matrix adhesion
in jute±Resana polyester composites can be readily seen
from Fig. 3a and c which shows the existence of poly-
mer particles adhered on the ®bre surface. On the other
hand, the ®bre surface of Elekeiroz polyester composite
is clean (Fig. 3b) without any polymer particles adhered.
As in the case of tensile properties, the ¯exural prop-
erties of all the system increases with ®bre loading. In
this case also, Resana-jute composites showed superior
properties to Elekeiroz±jute composites (Fig. 4). In a
three-point bend test a sample will experience tensile,
compressive and shear loads. In jute-reinforced Resana
composites due to the better ®bre±matrix adhesion, the
fracture starts by tensile fracture of the matrix on the
tensile side of the loading plane. Other cracks that run
in the ®bre direction or the shear plane develop from the
neutral plane. In Elekeiroz±jute composites, however,
there is less tensile fracture, excessive deformation and
virtually no shear plane cracking due to poor ®bre±
matrix adhesion.
In the present work, the data indicate that Resana's
composites display better mechanical properties than
the ones prepared with Elekeiroz's polyester as a matrix.

Fig. 3a. SEM photomicrograph of the tensile fracture surface of jute


roving reinforced±Resana polyester composites. b. SEM photo-
micrograph of the tensile fracture surface of jute roving reinforced±
Elekeiroz polyester composites. c. SEM photomicrograph of the mag-
ni®ed view of tensile fracture surface of jute roving reinforced±Resana Fig. 4. E€ect of ®bre content on the ¯exural modulus of jute roving
polyester composites. reinforced Elekeiroz and Resana polyester composites.
838 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

Table 3
In¯uence of di€erent alkali treatment on the mechanical properties of jute rovings reinforced ±Resana polyester composites as a function of ®bre
content

Type of alkali Fibre Tensile Young's Elongation Flexural Flexural Flexural Impact
treatment content strength modulus at break strength modulus de¯ection strength
(%) vol % (GPa) (GPa) (%) (MPa) (GPa) (%) (J/m)

Case Ia 0 38.1 0.81 5.98 72.7 2.20 2.88 20.8


10 48.6 1.29 4.97 71.0 3.54 1.92 26.2
20 63.7 1.39 6.00 104.7 3.98 2.53 50
30 68.7 1.4 6.15 115.0 4.25 2.90 84.2
Case IIb 0 ± ± ± ± ± ± ±
10 50.0 1.16 5.4 69.4 3.24 2.33 24
20 64.8 0.98 6.7 89.7 4.02 2.64 47.1
30 61.8 1.22 6.6 96.0 4.31 2.75 80
Case IIIc 0 ± ± ± ± ± ± ±
10 51.1 1.15 6.2 71.8 3.33 3.0 19.4
20 71.8 0.97 7.7 78.3 4.92 2.61 38.5
30 63.2 1.15 6.8 90.5 4.54 2.83 38.5
a
Case I: Untreated.
b
Case II: Immersion in 10% aqueous NaOH solution for 3 h at room temperature.
c
Case III: Rel¯uxed in 10% aqueous NaOH solution for 3 h.

This was taken to be due to a more ecient matrix to observed that the ®bre surface has a rough topography.
®bre stress transfer as a result of better wettability and The better-®bre adhesion can be readily seen from the
interfacial adhesion obtained with the former. There- ®gure. The existence of polyester particles adhered on
fore, further studies were conducted on composites the ®bre surface can be observed in alkali treated ®bre
having Resana's polyester as a matrix as these displayed composites. Therefore, development of a rough surface
better mechanical properties. topography enhancement in and aspect ratio o€er better
®bre±matrix interface adhesion and an increase in
3.2. E€ect of alkali treatment mechanical properties. This is clearly shown by the
decrease in the composite's impact strength, which is
Table 3 shows the e€ect of di€erent alkali treatment even more important at higher ®bre content (Fig. 6).
on the mechanical properties of jute rovings reinforced Impact strength is very sensitive to adhesion and,
Resana polyester composites. Our results show that the usually, very strong interfaces have a detrimental e€ect
harsher ®bre treatment (jute rovings re¯uxed in 10% on impact properties. It is generally accepted that the
aqueous NaOH solution for 3 h) tends to produce toughness of a ®bre-reinforced composite is dependent
composites with better mechanical strength, higher mainly on the ®bre stress±strain behaviour [41]. Jute
elongation at break, lower elastic modulus, higher ¯ex- ®bres are comparatively strong ®bres with high failure
ural modulus and signi®cantly lower impact strength
than similar composites reinforced with untreated or
mildly treated (3 h immersion in 10% aqueous NaOH
solution at room temperature) jute rovings. Table 3 also
shows that these e€ects are more pronounced at higher
®bre contents. This may be due to the fact that during
harsher alkali treatment, the alkali will penetrate into
the rovings more e€ectively and produce more sites for
polymer impregnation. In addition to this, alkali treat-
ment improves the ®bre surface adhesive characteristics
by removing natural and arti®cial impurities, thereby
producing a rough surface topography. Moreover,
alkali treatment leads to ®bre ®brillation, i.e. breaking
down of the composite ®bre bundle into smaller ®bres.
In other words, alkali treatment reduces ®bre diameter
and thereby increases the aspect ratio. Fig. 5 is the SEM
photomicrograph of the fracture surface of alkali trea- Fig. 5. SEM photomicrograph of the tensile fracture surface of alkali
ted jute roving reinforced polyester composite. It can be treated Jute roving reinforced±Resana polyester composites.
A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844 839

little ®bre pullout. This is very clear evidence for the


above two conditions i.e. in ®bre reinforced composites,
a signi®cant part of the energy absorption during
impact takes place through the ®bre-pullout process. In
alkali re¯uxed jute±polyester composites the ®bre pull-
out is very small due to better ®bre±matrix mechanical
interlocking. This is strong supporting evidence for
better physical interactions occurring at the ®bre±matrix
interface due to the removal of soluble extractives and,
thereby producing more sites for polymer penetration.
Fig. 6. E€ect of alkali treatment on the impact strength of jute roving
reinforced±Resana polyester composites as a function of ®bre content. The tensile strength values also support this conclusion.
It is apparent that maximum strength and maximum
toughness cannot be achieved simultaneously and the
strain and therefore, impart a high work of fracture to composites must be designed for an optimum combina-
the composites. The ®bre pullout, interface fracture and tion of the desired mechanical properties.
delamination are the major contributions toward the
high toughness of these composites. It is interesting to 3.3. E€ect of water ageing
note that alkali re¯uxed jute roving composites show
the least values in their impact strength. In general, the The e€ect of ageing in water on the tensile properties
energy-absorbing mechanisms built in the composite of jute roving reinforced Resana polyester composites as
include, (a) utilisation of the energy required to debond a function of ®bre content are presented in Table 4. The
the ®bres and pulls them completely out of the matrix, ®bres employed were not surface treated. It can be seen
(b) use of a weak interface between the ®bre and the that mechanical properties of pure polyester resin show
matrix [42]. It is clear that the conditions leading to (a) a slight increase after water ageing, may be due to the
and (b) are at odds with those required for good sti€- post curing e€ect. From the above table, it can be
ness and strength of the composites. In most ®bre-rein- observed that the overall mechanical properties of water
forced composites, a signi®cant part of energy aged composites are inferior to those of unaged com-
absorption during impact takes place through the ®bre posites especially at higher ®bre loading. However, in
pullout process. The impact strength of alkali re¯uxed re¯uxed composites (composites re¯uxed in boiling
samples at 30% ®bre loading is 110% less than those of water for 2 h), the tensile strength values are superior to
untreated and room temperature alkali treated samples. those of samples immersed in water for 48 h. This can
As discussed earlier, the low impact strength of alkali be clearly understood from Fig. 7. This may be attrib-
re¯uxed jute±polyester composites is due to the better uted to the fact that the rate of di€usion of water into
mechanical interlocking of the ®bre and matrix, which the composite is time dependent. The enhancement in
resulted in the fracture of ®bre at the crack-plane with tensile properties of the re¯uxed composites may be due

Table 4
In¯uence of water ageing on the mechanical properties of jute rovings reinforced±Resana polyester composites as a function of ®bre content

Type of Fibre Tensile Young's Elongation Flexural Flexural Flexural Impact


water ageing content Strength modulus at break strength modulus de¯ection strength
(%) (MPa) (GPa) (%) (MPa) (GPa) (%) (J/m)

Case Ia 0 38.1 0.81 5.98 72.7 2.20 2.88 20.8


10 48.6 1.29 4.97 71.0 3.54 1.92 26.2
20 63.7 1.39 6.00 104.7 3.98 2.53 50
30 68.7 1.4 6.15 115.0 4.25 2.90 84.2
Case IIb 0 39 0.92 5.0 73 3.61 3.49 20.5
10 31 1.59 3.41 57.4 4.39 2.46 29.0
20 49.5 1.23 4.23 103.7 5.64 2.72 48.7
30 60.8 1.15 5.55 115.5 7.91 2.71 79.5
Case IIIc 0 39 0.85 5.8 73.4 2.35 3.51 21.0
10 45.2 1.36 4.35 65.8 3.73 2.13 27.3
20 60.1 1.09 5.55 103.5 4.02 2.65 49.8
30 66.8 1.12 6.14 110.9 5.15 2.70 83.7
a
Case I: Unaged.
b
Case II: Immersion in water at 50 C for 48 h.
c
Case III: Re¯uxed in water for 2 h.
840 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

to the better mechanical interlocking between ®bre and associated with the increased water absorption of natural
matrix due to the limited swelling of the ®bre by low ®bres due to the presence of hydrophilic ÿOH groups.
water absorption. The in¯uence of water uptake on the Therefore due to high water content after exposure in
mechanical properties of jute ®bre reinforced poly- water for 48 h, the sti€ness of the cellulose ®bre drops
propylene composites was studied by Karmaker and co- considerably. This has been explained as being due to
workers [43]. They have observed that the swelling of the softening of the described zones of the cellulose
jute ®bres in composite material has a positive e€ect on micro®brils [45,46]. In fact, because of the excessive
the mechanical properties. When the ®bre absorbs a absorption of water, the intermolecular hydrogen
small amount of water, the ®bres tend to swell slightly. bonding in the cellulose ®bre might be reduced by the
This results in the development of a strong mechanical formation of intermolecular hydrogen bonding between
interlocking between the ®bre and the matrix. So at very cellulose molecules and water molecules, which lead to
low water absorption, the natural ®bre reinforced-poly- the deterioration of the module [47].
mer composites show a slight increase in their mechan- Fig. 10 shows the in¯uence of water ageing on the
ical properties. However, in the case of composites ¯exural strength of jute roving-polyester composites as
which were immersed in cold water for 48 h, the ®bres a function of ®bre loading. It can be seen that the ¯ex-
absorb more water and swell considerably. This exces- ural strength values of the jute-PP composites are found
sive water absorption and the resultant uncontrolled to be less than the neat resin at low weight fraction of
swelling of the ®bres leads to matrix cracking and ulti- the ®bre. However, an increase in ®bre content from 10
mate debonding of the ®bres. It has been reported that to 30% increases the ¯exural strength by 80%. The low
the water absorption of cellulose ®bre±polymer compo-
sites depends on the concentration of the ®bre [44]. This
can be clearly understood from Fig. 8, which shows the
change in water absorption with change in ®bre content.
It is seen that as the ®bre content increases, the water
absorption also increases.
Fig. 9 shows the e€ect of water ageing on the tensile
modulus of jute±polyester composites as a function of
®bre loading. From the above ®gure, it can be observed
that, water aged composites show a decrease in their
modulus values with ®bre loading. However, in the case
of unaged composites the modulus values increase with
®bre loading. Since the modulus of the matrix is con-
stant, the relative packing eciencies of the ®bre, ®bre
sti€ness and the ®bre±matrix adhesion are the impor-
tant parameters in determining the modulus of the
composites. Therefore, due to the better ®bre±matrix
adhesion and sti€ness of ®bres in Resana±jute compo-
sites, these composites show better modulus values than Fig. 8. E€ect of water absorption on the increase in weight of jute
water aged composites. The decrease in modulus values roving reinforced±Resana polyester composites as a function of ®bre
with ®bre loading observed in water aged composites is content.

Fig. 7. E€ect of ®bre content on the tensile strength of jute roving Fig. 9. E€ect of water ageing on the tensile modulus of jute roving
reinforced±Resana polyester composites after water ageing. reinforced±Resana polyester composites as a function of ®bre content.
A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844 841

¯exural strength values observed at lower ®bre weight 3.4. E€ect of thermal ageing
fraction might be due to the insucient ®bre loading.
However, the water-aged composites show inferior ¯ex- Fig. 12 shows the in¯uence of thermal ageing on the
ural properties than to composites at higher ®bre load- weight loss of jute-polyester composites as a function of
ing. This can be explained on the basis of increased ®bre loading. It can be seen that after 8 days of ageing
water absorption at higher ®bre loading, which decrea- in a hot air oven, the weight of pure polymer itself is
ses the sti€ness of the ®bre. slightly reduced. This may be due to the liberation of
Fig. 11 shows the e€ect of ®bre loading on the impact volatile components from the polymer. But in jute rov-
strength of jute±Resana composites having aged and ing reinforced composites, the weight loss increases with
unaged specimens. It is interesting to note that the ®bre loading due to the liberation of volatile compo-
impact values of all the composites show an increase in nents from the ®bre. As the ®bre content increases, the
tendency but the increase is more pronounced in com- amount of volatile components liberated will also
posites which were re¯uxed in water for 2 h and unaged increase. From Table 5 it can be observed that thermal
composites. It is also seen that impact strength of ageing decreases the tensile strength of all the compo-
unaged composites is slightly higher than water sites considerably. It is interesting to note that after 4
immersed samples at all ®bre loading. In all the cases, days of thermal ageing the strength of pure polyester
the work of fracture (impact strength) of the composites resin increases slightly due to the post curing e€ect. On
is found to increase linearly with the weight fraction of the other hand after 8 days of thermal ageing the
the ®bre and the work of fracture for 30% unaged strength decreased considerably. The reduction in com-
composites is found to be 80 J/M2. It is about 350% posite properties observed may be due to two reasons,
greater than those of pure polyester resin. (1) the oxidative degradation of both the polymer and
the ®bre (2) due to the prolonged heating, volatile com-
ponents of the ®bre surface are liberated o€ and the
®bre may get shrunk. When lignocellulosic materials are
heated, they undergo physical and chemical changes
[48,49]. Physical properties a€ected include enthalpy,
weight, strength, colour and crystallinity. Chemical
changes include reduction of the degree of polymerisa-
tion by bond scission, creation of free radicals, forma-
tion of carbonyls, carboxyls and peroxide groups
(especially in the presence of air), evolution of water,
carbon monoxide and carbon dioxide and ®nally decom-
position at elevated temperature [48]. Although the com-
ponents of lignocellulosic material are supposed to remain
stable up to 160 C, the degradation reaction may initiate
slowly for prolonged heating at 80 C [49]. The SEM pho-
Fig. 10. E€ect of water ageing on the ¯exural strength of jute rooving tomicrographs of the tensile failure surfaces of the thermal
reinforced±Resana polyester composites as a function of ®bre content. aged jute±Resana polyester composites indicate the
shrinkage of ®bre during thermal ageing (Fig. 13). Due
to the shrinkage, ®bre±polymer interface becomes so

Fig. 11. E€ect of water ageing on the impact strength of jute roving Fig. 12. E€ect of thermal ageing on the weight loss of jute roving
Reinforced±Resana polyester composites as a function of ®bre content. reinforced±Resana polyester composites as a function of ®bre content.
842 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

Table 5
In¯uence of thermal ageing on the mechanical properties of jute rovings reinforced±Resana polyester composites as a function of ®bre content

Period of thermal Fibre Tensile Young's Elongation Flexural Flexural Flexural Impact
ageing (days) content strength modulus at break strength modulus de¯ection strength
(%) (MPa) (GPa) (%) (MPa) (GPa) (%) (J/m)

Case Ia 0 38.1 0.81 5.98 72.7 2.20 2.88 20.8


10 48.6 1.29 4.97 71.0 3.54 1.92 26.2
20 63.7 1.39 6.00 104.7 3.98 2.53 50
30 68.7 1.4 6.15 115.0 4.25 2.90 84.2
Case IIb 0 39.3 1.5 3.22 55.9 3.38 1.5 19.0
10 40.0 2.11 2.37 48.5 4.12 1.35 19.5
20 57.3 2.10 3.33 83.8 6.33 1.47 33.0
30 62.1 2.29 3.57 101.6 8.93 1.68 55.8
Case IIIc 0 28.6 1.37 2.56 34.9 3.95 0.93 9.7
10 25 1.98 1.43 47.2 5.89 1.10 16.8
20 52.1 2.07 3.12 79.6 7.21 1.32 25.0
30 60.8 2.43 3.01 104.2 9.52 1.69 40.4
a
Case I: Unaged.
b
Case II:Thermal aged at 100 C for 4 days.
c
Case III:Thermal aged at 100 C for 8 days.

weak that it will a€ect the ®bre-matrix physical inter- showed the maximum values and unaged composites
locking. The result would be a complete ®bre pullout. exhibited the least values. It can be observed from Table 2
Fig. 14 shows the in¯uence of thermal ageing on the that the ¯exural properties of the composites showed
tensile modulus of jute-polyester composites as a func- the same trend as in the case of tensile properties.
tion of ®bre content. It can be seen that thermally aged Fig. 16 shows the impact strength of thermally aged
composites exhibit a superior tensile modulus than and unaged composites as a function of ®bre loading. It
unaged composites. The tensile modulus of pure polye- can be seen that thermal ageing on the composites
ster resin also shows signi®cant increase in their mod- decreases the impact strength considerably due to the
ulus values with thermal ageing. This increase may be degradation of the ®bre and the matrix. Due to the
due to the increased sti€ness of both the polymer and prolonged ageing in hot air oven, the ®bres and matrix
the ®bres. The changes occurring in elongation values become more brittle and this will cause negatively on
with thermal ageing (Fig. 15) support this fact. From the resistance to impact of these materials.
this ®gure it can be seen that elongation values decrease
with thermal ageing both in the case of pure polymer 3.5. E€ect of ®bre orientation
and ®lled polymer. This clearly indicated the increasing
sti€ness that occurred in polymer and ®bre due to pro- Figs. 17 and 18 show the e€ect of jute roving orien-
longed ageing in a hot air oven. The changes are just a tation on the tensile strength and elongation at break
reverse of modulus values, i.e. 4 days aged composites values of jute roving reinforced-polyester composites as

Fig. 13. SEM photomicrograph of the tensile fracture surface of Fig. 14. E€ect of thermal ageing on the tensile modulus of jute roving
thermal aged jute roving reinforced±Resana polyester composites. reinforced±Resana polyester composites as a function of ®bre content.
A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844 843

Fig. 15. E€ect of thermal ageing on the elongation at break of jute


roving reinforced±Resana polyester composites as a function of ®bre Fig. 17. E€ect of ®bre orientation on the tensile strength of jute rov-
content. ing reinforced±Resana polyester composites.

Fig. 16. E€ect of ®bre content on the impact strength of jute roving Fig. 18. E€ect of ®bre orientation on the elongation at break values of
reinforced± Resana polyester composites after thermal ageing. jute roving reinforced ±Resana polyester composites.

a function of ®bre content. From the above ®gures it cracks progress in the direction of ®bre alignment. The
can be seen that tensile properties of longitudinally transversely oriented ®bres act as barriers that prevent
oriented composite are much higher than those of the distribution of stress throughout the matrix. This
transversely oriented composites. It is obvious that causes a higher concentration of localised stress and
change in tensile strength is almost independent of ®bre results in both poor and variable mechanical properties.
content when the transversely oriented composites are
considered. Orientation of ®bres plays a vital role in the
performance of composite materials. Unidirectionally 4. Conclusion
oriented composites are inherently anisotropic in that
maximum strength and modulus are achieved along the The e€ect of ®bre surface wettability, alkali treatment
direction of ®bre alignment. In the transverse direction, and di€erent ageing conditions on the physical and
reinforcement is virtually non-existent and therefore mechanical properties of longitudinally oriented jute
fracture usually occurs at very low tensile stress. When rovings reinforced polyester composites were evaluated
the ®bres are aligned perpendicular to the direction of as a function of ®bre content. The tensile properties of
force, ®bres are not in conjunction with the matrix in the longitudinal composites were compared with those
increasing the strength of the composites. The higher of transversely oriented composites. The strength (ten-
tensile strength values observed in longitudinal direction sile, ¯exural) and modulus of the longitudinal compo-
show the anisotropic behaviour of the composites. sites increased with ®bre content as predicted in
Greater hindrance to the fracture front is experienced, accordance with the rule of mixtures. The impact
when the ®bres are oriented longitudinally (i.e. perpen- strength also increased linearly with the ®bre loading.
dicular to the fracture surface) to the applied force. The work of fracture (impact strength) of the composite
Breakage and pullout of ®bres takes place mainly when with 30% ®bre loading was found to be 80J/M. It is
the ®bres are oriented in the longitudinal direction, about 350% greater than those of pure polyester resin.
whereas, for transversely oriented ®bre composites, the The high toughness of this composite places it in the
844 A.C. de Albuquerque et al. / Composites Science and Technology 60 (2000) 833±844

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