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Composites Science and Technology 64 (2004) 955965 www.elsevier.

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Mechanical properties of sisal/oil palm hybrid ber reinforced natural rubber composites
Maya Jacoba, Sabu Thomasa,*, K.T. Varugheseb
a

School of Chemical Sciences, Mahatma Gandhi University, Priyadarshini Hills P.O. Kottayam, Kerala, 686 560, India b Thermal Research Center, KORADI, Nagpur, 441 111, India Received 8 August 2002; received in revised form 19 June 2003; accepted 25 June 2003

Abstract Natural rubber is reinforced with untreated sisal and oil palm bers chopped to dierent ber lengths. The eects of concentration and modication of ber surface in sisal/oil palm hybrid ber reinforced rubber composites have been studied. Increasing the concentration of bers resulted in reduction of tensile strength and tear strength, but increased modulus of the composites. Composites were prepared using bers treated with varying concentrations of sodium hydroxide solution and for dierent time intervals. The vulcanisation parameters, processability characteristics, and stressstrain properties of these composites were analysed. The rubber/ber interface was improved by the addition of a resorcinol-hexamethylene tetramine bonding system. The reinforcing property of the alkali treated ber was compared with that of untreated ber. The extent of ber alignment and strength of ber-rubber interface adhesion were analysed from the anisotropic swelling measurements. # 2003 Elsevier Ltd. All rights reserved.
Keywords: A. Natural rubber; Fiber composite; B. Polymer-matrix composite; C. Mechanical properties

1. Introduction Fiber reinforced rubber composites are of tremendous importance both in end-use applications and the area of research and development. These composites exhibit the combined behavior of the soft, elastic rubber matrix and the sti, strong brous reinforcement. The development of ber reinforced rubber composites has made available polymers that are harder than aluminum and stier than steel. Generally short ber reinforced rubber composites has become popular in industrial elds because of the processing advantages and increase in strength, stiness, modulus and damping [1,2]. The design of a short ber reinforced rubber composite depends on several factors such as the aspect ratio of the ber, control of ber orientation and dispersion and existence of a strong interface between ber and rubber. Cellulosic bers are derived from many renewable resources and have many desirable properties for reinforcement of thermoplastics such as low density, high
* Corresponding author. Tel.: +91-481-730003; fax: +91-481561190. E-mail address: sabut@vsnl.com, sabuthom@satyam.net.in (S. Thomas). 0266-3538/$ - see front matter # 2003 Elsevier Ltd. All rights reserved. doi:10.1016/S0266-3538(03)00261-6

stiness and low cost [38]. Various natural bers have been used as reinforcement in NR viz. sisal and coir ber as reinforcing llers for NR has been investigated by Varghese et al. [9] and Geethamma et al. [10]. The use of waste silk ber and jute ber in natural rubber has also been studied [11,12]. Recently studies relating to the incorporation of bamboo ber in natural rubber has been investigated by Ismail et al. [13]. Sisal ber is one of the strongest bers, which can be used for several applications [14]. Oil palm empty fruit bunch (OPEFB) and oil palm mesocarp bers are two important types of brous materials left in the palm oil mill. Oil palm bers are hard and tough and have found to be a potential reinforcement in phenol-formaldehyde resin [15]. Among the dierent natural bers sisal and oil palm bers appear to be promising materials because of the high tensile strength of sisal ber and toughness of oil palm ber. Therefore any composite comprising of these two bers will exhibit the above desirable properties of the individual constituents. The present study deals with the optimization of sisal and oil palm ber lengths in natural rubber composites. The inuence of ber loading and ber ratio on mechanical properties was analyzed. Studies of equilibrium swelling in a hydrocarbon solvent were also carried out. The rubber/ber

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interface was improved by the addition of a resorcinolhexamethylene tetramine bonding system. The reinforcing property of the alkali treated ber was also compared with that untreated ber.

2. Experimental Sisal ber was obtained from Sheeba Fibers, Poovancode, Tamil Nadu. Oil palm ber was obtained from Oil Palm India Limited. Natural rubber used for the study was procured from Rubber Research Institute of India, Kottayam. All other ingredients used were of commercial grade.

the ingredients. The composite materials were prepared in a laboratory two-roll mill (150300 mm). The nipgap, mill roll, speed ratio, and the number of passes were kept the same in all the mixes. The samples were milled for sucient time to disperse the bers in the matrix at a mill opening of 1.25 mm. The bonding system consisting of resorcinol and hexamethylene tetramine was incorporated for mixes containing treated bers. The bers were added at the end of the mixing process, taking care to maintain the direction of compound ow, so that the majority of bers followed the direction of the ow.

5. Measurement of properties 3. Fiber preparation The chemical constituent bers of given in Table 1 [15]. The physical constituents of bers were determined and are given in Table 2. Sisal and oil palm bers were rst separated from undesirable foreign matter and pith material. Oil palm ber was extracted from empty oil palm fruit bunches by retting. The bers were then cleaned of undesirable foreign matter and pith followed by repeated washing and drying in the oven. This ensured the removal of the oily matter present in the ber. The bers were then chopped to dierent lengths. Sisal and oil palm bers of lengths 10 mm and 6 mm were treated for 1 h with sodium hydroxide solutions of varying concentrations viz., 0.5, 1, 2 and 4 and 10% at room temperature. Finally the bers were repeatedly washed with water and air-dried. The ber breakage analysis was carried out by dissolving 1 g of the uncured composite in toluene, followed by the separation of bers from the solution. The distribution of ber length was determined using a travelling microscope. Curing properties were measured in a Monsanto R-100 rheometer, at a temperature of 150  C. Stressstrain measurements were carried out at a crosshead speed of 500 mm per minute. Tensile strength and tear strength was measured according to ASTM methods D412-68 and D624-54, respectively. The tensile tests were done using dumbbell samples cut at dierent angles with respect to the orientation of bers. Green strength measurements were carried out at a stretching rate of 500% min1 using dumb-bell shaped samples obtained from unvulcanized composites. Scanning electron microscopic studies were conducted to analyse the fracture behaviour of the composites. The fracture ends of the tensile and tear specimens were mounted on aluminium stubs and gold coated to avoid electrical charging during examination. Equilibrium swelling measurements of the vulcanizates was performed in toluene at room temperature.

4. Preparation of the composite Formulation of mixes is shown in Table 3. NR was masticated on the mill for 2 min followed by addition of

Table 1 Properties of sisal ber Chemical constituents (%) Cellulose Hemicellulose Lignin Wax Ash Physical properties of sisal ber Diameter (mm) Density ( g/ cm3) Tensile strength ( MPa) Youngs modulus (GPa) Microbrillar angle Elongation at break (%) 78 10 8 2 1

Table 2 Properties of oil palm ber Chemical constituents (%) Cellulose Hemicellulose Lignin Ash content Physical properties of oil palm ber Diameter mm Density g/cc Tensile strength (MPa) Youngs modulus (MPa) Elongation at break% Microbrillar angle ( ) 65 19 2

120140 1.45 530630 1722 2025 37

150500 0.71.55 248 6700 14 46

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Circular shaped samples having a diameter of 2 mm, punched out of tensile sheets were used. The samples were allowed to swell for 72 h in toluene. Anisotropic swelling studies were carried out using rectangular samples cut at dierent angles with respect to orientation of the ber from the tensile sheets and swollen in toluene at room temperature for 3 days.

P Ni Li2 " Lw P Ni L i

6. Results and discussion 6.1. Evaluation of ber breakage The extent of ber breakage during mixing was estimated by immersing 1 g of the unvulcanized mix containing individual sisal and oil palm bers, in toluene to dissolve the rubber component and thus separate the bers intact. The bers were washed with toluene to ensure complete removal of rubber from the surfaces. The washed bers were then collected and examined under a traveling microscope. The control of ber length and aspect ratio of bers in the rubber matrix is dicult because of ber breakage during processing. The severity of ber breakage depends mainly on the type of ber, the initial aspect ratio and the magnitude of stress and strain experienced by the bers during processing [16,17]. The breakage of bers due to high shear forces caused during mixing can be indicated by ber length distribution curve. The distribution of ber lengths can be represented in terms of moments of the distribution. The number and weight average ber lengths can be dened as: P Ni Li " Ln P Ni

where Ln is the number average ber length, Lw the weight average ber length and Ni is the number of bers having length Li.The value of Lw/Ln, the polydispersity index, can be taken as a measure of ber length distribution. The values of Ln, Lw and Lw/Ln are calculated based on 50 bers for the chopped sisal and oil palm bers extracted from the mix. The ber length distribution index of untreated sisal and oil palm bers before and after mixing is given in Table 4. The value of Lw/Ln remains about the same before and after processing, indicating that there is not considerable ber breakage. 6.2. Processing characteristics The processability of the compounds can be studied from the rheographs. The minimum torque in the rheograph gives an indication of the ller content in the rubber while the maximum torque in the rheograph is a measure of crosslink density and stiness in the rubber. In general, for all the mixes the torque initially decreases, then increases and nally levels o. The initial decrease in torque to a minimum value is due to the
Table 4 Fiber length distribution index Sisal Before mixing Ln Lw Lw/ Ln 10.28 8.688 0.845 After mixing 9.89 8.4 0.849 Oil palm Before mixing 11 10.2 0.927 After mixing 10.8 9.8 0.9074

Table 3 Formulation of mixes (G to M) Ingredients NR ZnO Stearic acid Resorcinol Hexaa TDQ CBSb Sulphur Sisal ber Treated Fiber length, (mm) Oil palm ber Treated (NaOH) Fiber length (mm)
a b

G 100 5 1.5 1 0.6 2.5

B 100 5 1.5 1 0.6 2.5 5 10 5 6

C 100 5 1.5 1 0.6 2.5 10 10 10 6

A 100 5 1.5 1 0.6 2.5 15 10 15 6

D 100 5 1.5 1 0.6 2.5 20 10 20 6

E 100 5 1.5 1 0.6 2.5 25 10 25 6

I 100 5 1.5 7.5 4.8 1 0.6 2.5 21 0.5% 1 h 10 9 0.5% 1 h 6

J 100 5 1.5 7.5 4.8 1 0.6 2.5 21 1% 1 h 10 9 1% 1 h 6

K 100 5 1.5 7.5 4.8 1 0.6 2.5 21 2% 1h 10 9 2% 1 h 6

L 100 5 1.5 7.5 4.8 1 0.6 2.5 21 4% 1h 10 9 4% 1 h 6

M 100 5 1.5 7.5 4.8 1 0.6 2.5 21 10% 1 h 10 9 10% 1 h 6

Hexamethylene tetramine. N-Cyclohexylbenzothiazyl sulphenamide.

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softening of the rubber matrix while the increase in torque is due to the crosslinking of rubber. The levelling o is an indication of the completion of curing. It is found that generally the presence of bers increases the maximum torque. 6.2.1. Eect of ber loading Fig. 1 shows the rheographs of mixes G, B, C, A, D, E. The presence of bers generates an increase in viscosity of the mixes. The increment in torque values with increasing ber loadings indicates that as more and more ber gets into the rubber matrix, the mobility of the macromolecular chains of the rubber reduces resulting in more rigid vulcanizates. The cure time was found to be independent of ber loading but the gum compound exhibited higher cure time. The reduction in cure time of the lled vulcanizates was attributed to the higher time the rubber compounds remain on the mill during mixing. As the ber loading increases, the time of incorporation also increases and consequently generates more heat due to friction. Table 5 shows the

maximum torque, minimum torque and cure time of various mixes. 6.2.2. Eect of bonding agent Fig. 2 shows the rheograph of mixes G, A, L. It is seen that the mix containing bonding agent and chemically treated ber has a maximum torque value indicating greater crosslinking. In Table 6 it can be seen that Mix L shows a longer cure time than mix A. This can be attributed to the direct involvement of the bonding agents in the vulcanization resulting in the formation of good bonding between bers and rubber. Earlier studies have indicated that longer cure time is due to better binding between ber and matrix [18]. 6.3. Mechanical properties 6.3.1. Eect of ber loading The eect of ber loading on tensile strength in shortber reinforced natural rubber composites has been widely studied [1921]. Generally, the tensile strength initially drops up to a certain amount of ber and then increases.

Fig. 1. Torquetime curve at dierent ber loadings. Fig. 2. Torquetime curve of composite containing bonding agent and treated bers. T 52 58 58.7 59 61.5 61.9 t90 14 7.3 7.2 7 7.5 7.5 Table 6 Cure characteristic of mixes Mix Gum A L Tmax (dNm) 58 66 81 Tmin (dNm) 6 7 7.4 T 52 59 73.6 t90 14 7 8.5

Table 5 Cure characteristics of the various mixes Mix Gum B C A D E Tmax (dNm) 58 64 65.5 66 68 69 Tmin (dNm) 6 6 6.8 7 6.5 7.1

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In the present study the behavior of composites containing 10,20,30,40 and 50 phr untreated sisal and oil palm bers were analyzed. Sisal and oil palm bers were taken in the ratio 50:50. From Fig. 3 it is clear that tensile strength increases up to 30 phr and then declines. The tensile strength in the transverse direction also shows the same trend. Natural rubber inherently possesses high strength due to strain-induced crystallization. When bers are incorporated into NR, the regular arrangement of rubber molecules is disrupted and hence the ability for crystallization is lost. This is the reason why ber reinforced natural rubber composites possess lower tensile strength than gum compounds. When ber reinforced rubber composites is subjected to load, the bers act as carriers of load and stress is transferred from matrix along the bers leading to eective and uniform stress distribution which results in a composite having good mechanical properties. The uniform distribution of stress is dependent on two factors: (a) population of bers, (b) orientation of bers. At low levels of ber loading, the orientation of bers is poor and the bers are not capable of transferring load to one another and stress gets accumulated at certain points of composite leading to low tensile strength. At high levels of ber loading the increased population of bers leads to agglomeration and stress transfer gets blocked. At intermediate levels of loading (30 phr) the

population of the bers is just right for maximum orientation and the bers actively participate in stress transfer. The variation of composite tensile strength with the angle of orientation at dierent levels of ber loading is given in Fig. 4. It is seen that the longitudinal orientation of bers results in maximum tensile strength and as the angle of orientation of bers increases, tensile strength decreases. When bers are longitudinally oriented the bers are aligned in the direction of force and the bers transfer stress uniformly. When transversely oriented, the bers are aligned perpendicular to the direction of load and they cannot take part in stress transfer. Fig. 5 shows the variation of tear strength with ber loading. As loading increases the tear strength at rst decreases and at 30 phr shows an increase. At high ber loadings tear strength is found to decrease as the increased strain in the matrix between closely packed bers increases tearing and reduces the tear strength. Similar results have been observed by Ismail et al. [22]. Fig. 6 presents the variation of elongation at break with ber loading. The value of elongation at break shows a reduction with increasing ber loading. Increased ber loading in the rubber matrix resulted in composites becoming stier and harder. This will reduce the composites resilience and toughness and lead to lower elongation at break.

Fig. 3. Variation of tensile strength with ber loading. (L0longitudinally oriented; P30oriented at 30 ; R45oriented at 45 ; S60 oriented at 60 ; T90transversely oriented).

Fig. 4. Variation of tensile strength with angle of orientation at dierent levels of ber loading.

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The variation of modulus at 100% with ber loading is given in Fig. 7. The values show a steady increase with ber loading. This is because at high ber loadings the composites will be able to withstand more loads.

6.3.2. Eect of ber ratio Composites were prepared varying the ratio of bers while keeping the total ber loading constant (30 phr). Fig. 8 shows the variation of tensile strength with wt. of sisal in total ber content at dierent orientations. It is clear that the composite containing 21 g sisal and 9 g oil palm has maximum tensile strength. This suggests that

Fig. 5. Variation of tear strength with ber loading.

Fig. 7. Variation of modulus at 100% with ber loading.

Fig. 6. Variation of elongation at break with ber loading.

Fig. 8. Variation of tensile strength with ber ratio.

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this is the optimum ratio. It is also seen that as the concentration of sisal ber increases the tensile strength also increases. This suggests that the tensile strength of the composite is dependent more on the weight of sisal rather than oil palm, which could be due to the high strength of sisal ber. 6.4. Extent of ber orientation from green strength measurements The green strength of short ber reinforced composites depends upon the degree of ber orientation and so the latter can be obtained from the expression: SL =SG;L orientation SL =SG;L ST =SG;T

6.5. Equilibrium swelling studies Equilibrium swelling measurements of the vulcanisates was performed in toluene at room temperature. Circular shaped samples, having a diameter of 1.9 mm, punched out of tensile sheets were used. The samples were allowed to swell for 72 h in toluene. 6.5.1. Rubberber interactions The extent of interaction between rubber and ber can be analysed using Kraus [23,24] and Cunneen and Russell and Lorentz Park [25] equation. The Kraus equation is ! Vro f 1m 1f Vrf

Fiber

where S=green strength and subscripts G, L and T represents gum, longitudinal and transverse respectively. The eect of ber loading on percentage orientation is shown in Fig. 9. The percentage orientation is the lowest when the ber loading is small i.e. 10 phr. At low ber loading the bers can randomly move around leading to increased chaoticity and decreased levels of orientation. As the ber loading increases, percentage orientation increases with the maximum value for composite containing 30 phr ber. At 40 phr ber loading, the percentage orientation decreases indicating that the bers cannot orient themselves due to entanglement caused by the increased population of bers.

where Vro=volume fraction of rubber gum vulcanizates, f=volume fraction of ber, m=polymer - ber interaction parameter, f=volume of ller / total volume of recipe, Vrf is the volume fraction of elastomer in the solvent swollen lled sample and is given by the equation by Ellis and Welding [26].
1 d fwp p 1 d fwpp1 As p s

Vrf

Fig. 9. Eect of ber loading with on percentage orientation.

where d=deswollen wt. of sample, f=volume fraction of ber, w=initial weight of sample, pp=density of polymer, ps=density of solvent, As=amount of solvent absorbed by sample, Vro=volume fraction of elastomer in solvent swollen unlled sample. Since Eq. (7) is in the form of a straight line, a plot of Vro/Vrf versus f/ 1f should give a straight line, whose slope (m) will be a direct measure of reinforcement of the ber. The ratio Vro/Vrf represents the degree of restriction of the swelling of the rubber matrix due to the presence of ber. According to the theory by Kraus, reinforcing llers will have a negative higher slope. The Kraus plot and Vro/Vrf values are given in Fig. 10 and Table 7 respectively. In the present case it is observed that as the ber loading increases, the solvent uptake of the sample decreases. This causes an increase in Vrf values, which will decrease the ratio of Vro/Vrf since Vro is a constant. It can be seen from the graph that Vro/Vrf decreases with ber loading. This behavior leads to a negative slope indicating the reinforcement eect of the bers. From Table 7, mix L has the lowest Vro/Vrf value. This can be associated with enhanced ber- rubber adhesion in the composite due to the presence of bonding agent and alkali treated ber. Since there is better

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bonding between ber and matrix, there is a strong interface, which restricts the entry of solvent. The CunneenRussell equation is Vro ae z b Vrf 6

where Vro and Vrf are the same, z is the weight fraction of ber, a and b are constants. Here a plot of Vro/Vrf versus ez should give a straight line with a positive slope as shown in Fig. 11. This shows that as ber loading increases the extent of reinforcement also increases. The Lorentz Park equation is Qf ae z b Qg 7

The subscripts f and g refer to lled and gum vulcanisates respectively. Table 8 shows the Qf/Qg values at variable ber loading. The higher the Qf/Qg values, the lower will be the extent of interaction between ber and matrix. It can be seen from Table 8 that as ber loading increases Qf/Qg decreases which indicates greater extent of interaction between rubber matrix and bers. The ratio Qf/Qg has lowest value for mix L. This conrms that maximum interaction between ber and matrix occurs in presence of bonding agent and alkali treated ber. A plot of Qf/Qg (Fig. 12) versus ez gives a straight line with positive slope which conrms the above ndings. 6.5.2. Swelling index and crosslink density determination The swelling index which is a measure of the swelling resistance of the rubber compound, is calculated using the equation: As W1 100

where Q is dened as the amount of solvent absorbed by 1 g of rubber and is given by the equation . Q Swollen wt:-dried wt: Original wt: x 100=formula wt: 8

Swelling

index

Table 8 Mixes B C A D E L Qf/Qg 1.191 1.1128 1.054 1.00516 0.9289 0.4295

Fig. 10. Variation of Vro/Vrf with f / 1f (Kraus plot). Table 7 Mixes B C A D E L Vro/Vrf 1.147 1.0915 1.0079 1.056 0.8581 0.4396

Fig. 11. Variation of Vro/Vrf with ez (CunneenRussel plot).

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where As=amount of solvent absorbed by sample W1=initial weight of sample before swelling. The diusion mechanism in rubbers is essentially connected with the ability of the polymer to provide pathways for the solvent to progress in the form of randomly generated voids. As the void formation decreases with ber addition, the solvent uptake also decreases. Table 9 shows the swelling index values of composites at dierent ber loadings and in presence of bonding agent. Mix L shows the minimum swelling index value indicating that the presence of bonding

agent binds the alkali treated ber and rubber so that swelling is highly restricted in the composite. The extent of crosslinking can be established by determining the Vrf of the composites. Table 10 shows the Vrf values. The higher Vrf value for mix L indicates better adhesion and higher degree of crosslinking. A comparison of crosslink density has also been made from the reciprocal swelling values 1/Q where Q is dened as the amount of solvent absorbed by 1 g of rubber. Table 11 shows the apparent crosslinking values in various mixes. Mix L shows the maximum crosslink density indicating maximum interaction between ber and matrix. The reinforcing eect of the bers can be supported by the cross-linked density values. It can be seen in Fig. 13 that as the ber loading increases the cross-link density values are also found to increase. This eect can be explained using the basic equations used for swelling: 1= 3 2 Mc r Vs Vrf =ln 1 Vrf Vrf Vrf 10

Table 11 Apparent crosslink density values Mixes Gum B C A D E L 1/Q 0.1399 0.1432 0.1473 0.15015 0.1552 0.1766 0.388

Fig. 12. Variation of Qf/Qg with ez (LorentzPark plot).

Table 9 Samples G B C A D E L Swelling index 540.6 474.8 470.6 469.4 422.9 349.6 166

Table 10 Mixes B C A D E L Vrf 0.1098 0.1102 0.1158 0.1196 0.1254 0.1473

Fig. 13. Variation of crosslink density values with ber loading.

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where Mc=molecular weight of polymer between crosslinks, pr=density of polymer, Vs=molar volume of solvent =interaction parameter  is given by Hildebrand equation 2 Vs s p  RT

mum for composite at lower ber loading and therefore it absorbs a maximum quantity of solvent indicating poor reinforcement. 6.6. Anisotropic swelling studies

11

where =lattice constant, Vs=molar volume, R=universal gas constant, T=absolute temperature, s=solubility parameter of solvent, p=solubility parameter of polymer, Vrf=volume fraction of elastomer in the solvent swollen lled sample. As loading increases the amount of solvent absorbed by sample decreases which leads to increase in Vrf values and this in turn increases cross-link density values as shown in Fig. 13. The crosslink density value is mini-

For short ber reinforced rubber composites, the swelling ratio in any direction forming an angle y with the ber orientation is given by the expression: 2 2 2 12 a2  a2 T aL sin  aL where aL and aT are the dimensional swelling ratios in the longitudinal and transverse directions, respectively. Fig. 14 shows dimensional swelling variation with angle  in accordance with the above equation where various values of  were assumed. For all the mixes, the swelling increases with  and is found to be maximum when  becomes 90  C. The line corresponding to gum compound

Table 12 Slope values from anisotropic swelling studies Mixes Gum B C A D E Slope values 0.1427 0.153 0.153 0.1983 0.1673 0.1522

Fig. 15. Eect of tensile strength on alkali concentration.

Fig. 14. Swelling variation as a function of the angle of measurement, .

Fig. 16. (a) SEM tensile fracture surface of sisal /oil palm ber lled natural rubber composites at 30 phr loading at magnication100. (b) SEM tensile fracture surface of sisal /oil palm ber lled natural rubber composites at 30 phr loading in presence of bonding agents and alkali treated bers at magnication100.

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which does not contain bers is positioned above those for the other mixes. This shows that short bers restrict the transport of solvent into the composite. The extent of ber alignment can be understood from the slope values given in Table 12. It has been reported [27] that the steeper the line the higher the degree of ber alignment. Mix A shows the maximum slope value among the various mixes. It shows that the composite containing 30 phr ber has the highest degree of ber alignment. 6.7. Eect of alkali treatment Sisal and oil palm bers (of lengths 10 and 6 mm) were subjected to alkali treatment. The bers were treated with dierent concentrations of NaOH (0.5, 1, 2, 4 and 10%) for 1 h at room temperature. After treatment the diameter and weight of the bers were found to decrease due to the removal of lignin. Composites were prepared with sisal and oil palm bers (of lengths 10 and 6 mm) that were treated with varying concentrations of NaOH solution for 1 h. The variation of tensile strength with chemical treatment is given in Fig. 15. It is seen that alkali treated composites show an increase in tensile strength as compared to untreated composites. Maximum tensile strength was shown by composite containing bers treated with 4% NaOH. It has been reported that alkali treatment increases the roughness of ber surface, hence increasing the surface area available for contact with the matrix [28]. The better adhesion between sisal and oil palm bers is evident in SEM micrographs. Fig. 16 a shows the tensile fracture surface of sisal and oil palm lled natural rubber composites. It can be seen that there are a few holes after the bers are pulled out from the rubber matrix indicating poor wetting between the bers and matrix. However for similar composites but with the presence of bonding agents and treated bers (Fig. 16b) better adhesion between ber and rubber matrix can be seen. The bers are well wetted by the rubber matrix and there is ber breakage due to strong adhesion.

the longitudinal direction are superior to those in the transverse direction. Addition of sisal and oil palm bers led to increase of tensile strength and tear strength but increased modulus. The extent of adhesion between ber and rubber matrix was found to increase on alkali treatment of bers. From the mechanical properties the alkali treated bers exhibited better tensile properties than untreated composites. Processing characteristics were found to be independent of ber loading and modication of ber surface. Swelling studies revealed that composites containing bonding agents and alkali treated bers showed higher crosslink density and betteradhesion. Anisotropic swelling studies indicated that the presence of short bers restricted the entry of solvent.

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[1] [2] [3] [4] [5] [6] [7] [8] [9] [10] [11] [12] [13] [14] [15] [16] [17] [18] [19] [20] Goettler LA, Shen KS. Rubber Chem Technol 1983;56:620. Setua DK, De SK. J Mater Sci 1984;8:8. Oksman K, Clemons C. J Appl Polym Sci 1998;67:1503. Raj RG, Kokta BV, Maldas D, Daneault C. J Appl Polym Sci 1989;37:1089. Park BD, Balatinecz J. J Polym Compos 1997;18:79. Sandi AR, Rowell RM, Cauleld Df. Polym News 1996;20:7. Raj RG, Kokta BV, Maldas D, Daneault C. J Appl Polym Sci 1991;31:1358. Yam KL, Gogoi BK, Lai CC, Selke SE. Polym Eng Sci 1990; 30:693. Varghese S, Kuriakose B, Thomas S, Koshy TA. Indian J Nat Rubb Res 1991;4(1):5567. Geethamma VG, Joseph R, Thomas S. J Appl Polym Sci 1995; 55:583. Setua DK, De SK. Rubber Chem Technol 1983;56:808. Arumugam N, Tamareselvy K, Venkata Rao K, Rajalingam P. J Appl Polym Sci 1989;37:2645. Ismail H, Shuhelmy, Edyham MR. Eur Polym J 2002;38:3947. Iannace S, Ali R, Nicolais L. J App Polym Sci 2001;79:108491. Sreekala MS, Thomas S, Neelakantan NR. J Polym Eng 1997; 16:265. De SK, Murty VM. Polym Engg Rev London 1984;4:313. Pramanik PK, Khastgir DK, Saha TN. Plastics, Rubber and Composites Processing and Applications 1991;15:18994. Chakraborty SK, Setua DK, De SK. Rubb Chem Technol 1982; 55:1286. Geethamma VG, Thomas Mathew K, Lakshminarayanan R, Thomas S. Polymer 1998;39:148391. Prasantha Kumar R, Geethakumari Amma ML, Thomas S. J Appl Polym Sci 1995;58:597. Varghese S, Kuriakose B, Thomas S. Plast Rubb Comp Proc Appl 1993;20:930. Ismail H, Rosnah N, Rozman HD. Polymer 1997;38:16. Kraus C. J Appl Polym Sci 1963;7:861. Kraus C. Rubb Chem Tech 1965;38:1070. Lorentz O, Parks CR. J Polym Sci 1961;50:299. Ellis B, Welding GN. Techniques of polymer science. London: Society of the Chemical Industry; 1964. Noguchi T, Ashida M, Mashimo S. Nippon Gomu Kyokaishi 1984;57:171. Li Y, Mai Y-W, Ye L. Comp Sci Tech 2000;60:203755.

7. Conclusions

[21] [22] [23] [24] [25] [26] [27] [28]

The processability characteristics and mechanical properties of sisal/oil palm hybrid ber reinforced natural rubber composites have been investigated as a function of ber loading, ratio and treatment. Fiber breakage analysis revealed that the extent of breaking was low. The mechanical properties of the composites in

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