Journal of Reinforced Plastics and Composites Recent Development in Natural Fiber Reinforced Polypropylene Composites
Ramakrishna Malkapuram, Vivek Kumar and Yuvraj Singh Negi Journal of Reinforced Plastics and Composites 2009; 28; 1169 originally published online Nov 20, 2008; DOI: 10.1177/0731684407087759 The online version of this article can be found at:

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Recent Development in Natural Fiber Reinforced Polypropylene Composites
RAMAKRISHNA MALKAPURAM, VIVEK KUMAR AND YUVRAJ SINGH NEGI* Polymer Science and Technology Program, Department of Paper Technology Indian Institute of Technology Roorkee, Saharanpur Campus Saharanpur, UP, India
ABSTRACT: This review article describes the recent developments of natural fiber reinforced polypropylene (PP) composites. Natural fibers are low-cost, recyclable, and eco-friendly materials. Due to eco-friendly and bio-degradability characteristics of these natural fibers, they are considered as strong candidates to replace the conventional glass and carbon fibers. The chemical, mechanical, and physical properties of natural fibers have distinct properties; depending upon the cellulosic content of the fibers which varies from fiber to fiber. The mechanical properties of composites are influenced mainly by the adhesion between matrix and fibers. Chemical and physical modification methods were incorporated to improve the fiber–matrix adhesion resulting in the enhancement of mechanical properties of the composites. The most important natural fibers are jute, flax, and coir and their novel processing technics to develop natural fiber reinforced composites are also described. KEY WORDS: natural fibers, polypropylene, chemical and physical modifications, processing, properties.



past considerable research and development have been expanded in natural fibers as a reinforcement in thermoplastic resin matrix. These reinforced plastics serve as an inexpensive, biodegradable, renewable, and nontoxic alternative to glass or carbon fibers. The various advantages of natural fibers over man-made glass and carbon fibers are low cost, low density, competitive specific mechanical properties, reduced energy consumption and biodegradability. Thermoplastic materials that currently dominate as matrices for natural fibers are polypropylene(PP), polyethylene, and poly(vinyl chloride) while thermosets, such as phenolics and polyesters, are common matrices. With a view to replacing the wooden fittings, fixtures and furniture, organic matrix resin reinforced with natural fibers such as jute, kenaf, sisal, coir, straw, hemp, banana, pineapple, rice husk, bamboo, etc., have been explored in the past two decades. There is an increasing demand from automotive companies for materials with sound abatement capability as well as reduced weight for fuel efficiency. Natural fibers possess excellent sound absorbing efficiency and are more shatter resistant and have better energy management characteristics than glass fiber reinforced composites. In automotive parts, such composites not only reduce the mass of the component but also lower the
*Author to whom correspondence should be addressed. E-mail:



COMPOSITES, Vol. 28, No. 10/2009


0731-6844/09/10 1169–21 $10.00/0 DOI: 10.1177/0731684407087759 ß SAGE Publications 2009 Los Angeles, London, New Delhi and Singapore
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The modifications of fiber and matrix are discussed and the mechanical properties of composites are described also. rice husk [45–48]. pinewood fiber [38–41]. furniture. energy needed for production by 80%.42–44]. and matrix-to-fiber stress transfer efficiency are vital requirements for the manufacture of reliable. kapok/cotton [57]. bamboo fiber [62]. and date palm fiber [63].51]. wood fiber [13–22].54].sagepub. flax [23–29]. Bledzki and Gassan [2] have stated that the quality of the fiber–matrix interface is significant for the application of natural fibers as reinforcement fibers for plastics. kenaf [55. saw dust [48–50]. However. thereby replacing not so easily renewable fossil fuel-based polymers/plastics. Eco-friendly composites can be made by replacing glass fibers with various types of ligno-cellulose fibers. Other emerging markets are industrial and consumer applications such as tiles.1170 R. Maleated polyolefins are used to modify the matrix. vetiver [60]. These modification methods are of different efficiency for the adhesion between matrix and fiber. MALKAPURAM ET AL.33. such as silanes. eco-friendly natural composites that can possess better mechanical properties and withstand environmental attacks. lugffa sponge fiber [3. The lignocellulosic fibers that have been used in polyolefins include cellulose fiber [4–12]. Performance of the composites is summarized. flower pots. For the purpose of making engineering parts with a wide study on the effect of different coupling agents. It necessitates the use of compatibilizers or coupling agents in order to improve the adhesion between fiber and matrix [3]. pineapple leaf [58]. Cellulosic fibers from other sources have been reported in polyolefin composites by several authors. and marine piers [1]. Complete matrix fusion to facilitate thorough fiber impregnation. jute [1. Development of new composite products from the easily renewable natural materials has a strong potential to deliver novel biodegradable and/or readily recyclable materials suitable for the automotive and packaging at Victoria Univ of Wellington on July 14. maleic anhydride grafted polypropylene (PPgMA) or modification by acetylation. the main problem of natural fiber/polymer composites is the incompatibility between the hydrophilic natural fibers and the hydrophobic thermoplastic matrices.56]. basalt [59]. Such modification of the matrix develops the interactions between the anhydride groups of maleated coupling agents and the hydroxyl groups of natural fibers. The variation in the properties of natural fibers is another important aspect that has to be considered.35–37]. Physical and chemical methods can be used to optimize this interface. In the present article an attempt has been made to review the state of the art of organocellulosic fiber reinforced polyolefin composites. such composites have a distinct disadvantage of load-bearing capability compared to glass fiber reinforced thermoplastics. Matrix or fiber modification is therefore necessary to improve the compatibility between fiber and matrix. bio flour [61]. formation of strong fiber/matrix interfacial bonding. sisal [3. has been reported in the literature. wheat straw [52]. The various types of natural fibers used for such reinforcement are described.33. paper sludge [53].25. Downloaded from http://jrp. 2009 . Cannatis sativa (hemp) [30–35]. However. Demands for natural fibers in plastic composites is forecast to grow at 15–20% annually with a growth rate of 15–20% in automotive applications. LIGNOCELLULOSIC FIBERS OR MATERIALS Several types of lignocellulosic materials have been investigated in PP [4–12]. coconut fiber [33. and 50% or more in selected building applications. A comprehension review of the cellulosic-based materials in composites has appeared recently [2].

4–22.8 67–78 77.7 0. microfibrillar angle.7 2.5 1.2–74.8 – 1.6 61.2–3.6 – 4–6 – 34.7–7.sagepub.6 82.5 3–7 7–8 1. Fiber Jute Hemp Kenaf Flax Ramie Sunn Sisal Cotton Kapok Coir Banana PALF Density (g/cm3) 1. Mechanical properties of natural fibers.6–20. The natural fibers exhibit considerable variation in diameter along with the length of individual filaments.0 5.16–1.2 0.7 23 10–20 19 – Pectin (wt%) 0.0 – 0.6 70–82 Lignin (wt%) 12–13 3.4 21. A fiber is more ductile if the microfibrils have a spiral orientation to the fiber axis.7 64 36–43 63–67.9 – 2. If the microfibrils are oriented parallel to fiber axis then the fibers are inflexible and rigid.5–1.5 8–11 13.15 – – Diameter (km) 25–200 – – – – – 50–200 – – 100–450 – 20–80 Tensile strength (MPa) 393–773 690 – 345–1100 400–938 1.4 0.6 – – – – Moisture content (wt%) 12. – 1. Table 1.9 468–640 287–800 – 131–175 1.7–5.9–22.3 0.5 Elongation at break (%) 1.3 1.9 413–1627 Young’s modulus (GPa) 13–26.7 at Victoria Univ of Wellington on July 14.9 0.2 15–40 1. The various chemical constituents of a specific natural fiber also vary considerably.4 17. and cell dimension defects are the most important variables that affect the overall properties of the fibers.45 1.5 18.8 5.4 31–39 71 68. in varying quantities.5–12.4 2.6–20. In Table 2 the properties of these fibers are summarized. chemical composition.45 – – 1.3 10 – – 23 3–4 – – Wax (wt%) 0.5 1.17–1. Fiber Jute Hemp Kenaf Flax Ramie Sunn Sisal Henquen Cotton Kapok Coir Banana PALF Cellulose (wt%) 61–71.7 3.Natural Fiber Reinforced Polypropylene Composites 1171 CHEMICAL COMPOSITION OF SOME NATURAL FIBERS In Table 1 cotton has the maximum content of cellulose ranging from 85 to 95%.0 1.8 Table 2.5–9.2 4–8 5.6–76.6 – 1.5 – – 27.1 – 13 41–45 5 5–12 Hemicellulose (wt%) 13.6 2. etc.7 15–19 2.6 Downloaded from http://jrp. pectin wax.6 13. MECHANICAL PROPERTIES OF LIGNOCELLULOSIC MATERIALS The structure. The other fibers have cellulose along with lignin and other components such as hemicellulose.4–128 – 9.1–16. 2009 .3–1.6 10.5 70..5–82. Chemical composition of some natural fibers.7–3.2 1.2 67.0–14.5 0.6 10 – 10 8 10 11 – – – 8 8.7 11.6–0.

restrained layers – coupling agents develop a highly crosslinked interphase region. have values 510). MALKAPURAM ET AL. wettability – coupling agents improve the wetting between polymer and substrate (critical surface tension factor). . Change of Surface Tension The surface energy of fibers is closely related to the hydrophilicity of the fiber. the acid–base reactions at the at Victoria Univ of Wellington on July 14. chemical bonding – coupling agents form covalent bonds with both materials. Chemical Methods Strongly polarized cellulose fibers are inherently incompatible with hydrophobic polymers when two materials are incompatible. In specific strength the natural fibers can be compared with glass fibers. SURFACE MODIFICATIONS OF LIGNOCELLULOSIC FIBERS Physical Methods Reinforcing fibers can be modified by physical and chemical methods. . with a modulus intermediate between that of substrate and of the polymer. 208 for sisal. which include the morphology of the interphase. The lignin content of the fibers influence its structure properties and morphology. Physical methods. calandering. surface energy.sagepub. So the consideration of other concepts appears to be necessary. thermotreatment. it is often possible to bring about compatibility by introducing a third material that has properties intermediate between those of the other two. and 108 for flax while other fibers such as jute. The properties are affected by the chemical constitutents and complex chemical structure of natural fibers. The angle between the axis and the fibril of the fiber (microfibrillar or spiral angle) also affect the strength of the fibers. .1172 R. and hemp. Some investigations are concerned with methods to decrease hydrophilicity. flexible layer. . such as stretching. The development of a definitive theory for the mechanism of bonding by coupling agents in composites is a complex problem. Physical treatments change structural and surface properties of the fiber and thereby influence the mechanical bondings to polymers. weak boundary layers – coupling agents eliminate weak boundary layers. and the production of hybrid yarns do not change the chemical composition of the fibers. 148 for PALF. Least tensile strength is shown by coir fibers which may be attributed to low cellulose content and considerably high microfibrillar (41–458 for coir. 2009 . and the wetting phenomena. There are several mechanisms of coupling in materials: . Mechanical properties are higher if this is smaller. The modification of wood–cellulose fibers with stearic acid hydrophobizes those fibers and improves their Downloaded from http://jrp. The waxy substances of the natural fibers affect the fiber wettability and adhesion characteristics. and . deformable layers – coupling agents produce a tough. The main chemical bonding theory alone is not sufficient. ramie. acid–base effect – coupling agents alter acidity of substrate surface.

). and esterification of cellulose.. The mechanism of reaction can be divided into two steps: activation of the copolymer by heating (t ¼ 1708C) (before fiber treatment). Thus. Then the cellulose molecule cracks and radicals are formed.e. for example vinyl monomer (i.sagepub. Afterward the radical sites of the cellulose are treated with a suitable solution (compatible with the polymer matrix). The resulting co-polymer possesses properties characteristic of both fibrous cellulose and grafted polymer. The cellulose is treated with an aqueous solution with selected ions and is exposed to a high energy radiation.Natural Fiber Reinforced Polypropylene Composites 1173 dispersion in PP. Downloaded from http://jrp. methyl methacrylate. acrylonitrile. polystyrene. 2009 . Impregnation of Fibers A better combination of fiber and polymer is achieved by impregnation of the reinforcing fabrics with polymer matrices compatible to the at Victoria Univ of Wellington on July 14. This reaction is initiated by free radicals of the cellulose molecule. Mechanism of interaction of cellulose fibers with maleated PP . A treatment with poly(vinyl acetate) increases the mechanical properties and moisture repellence. the treatment of cellulose fibers with hot polypropylene–maleic anhydride (MAH–PP) copolymers [3] provides covalent bonds across the interface. etc. a better wettability and a higher interfacial PP chain O HO HO C C O H 2 C C H C O C O C O O Cellulose fiber H 2 C C H C PP chain + H2O CH3 O Cellulose fiber O O C C O H2 C C H C CH3 OH + OH C O C O H2 C C H C CH3 O Cellulose fiber O O H O H C C H2 C C H C CH3 Figure 1. Graft Copolymerization of Matrix An effective method of chemical modification of matrix and natural fibers is graft copolymerization. After this treatment the surface energy of the fibers is increased to a level much closer to the surface energy of the matrix. For example. For this purpose polymer solutions or dispersions of low viscosity are used.

when PMPPIC is used for the modification of the fibers or polymer matrix. by creating a crosslinked network due to covalent bonding. Interaction between PS Matrix and PMPPIC modified cellulose fibers. Cellulose + Lignin O C= O N–H CH2 O C= O N–H CH2 O C =O N–H CH2 CH CH2 CH CH2 CH CH2 Polystyrene Figure 3. which are available for moisture pick-up. so that there is an adhesion between PMPPIC and PS. Polymethylene–polyphenyl–isocyanate (PMPPIC) in pure state or solution in plasticizer can be used. The PP chain permits segmental crystallization and cohesive coupling between the modified fiber and the PP matrix. and . The isocyanatic treatment is reported to be more effective than the treatment with silane. Downloaded from http://jrp. Modification of Lignocellulosic Fibers with Isocyanates The reactivity of cellulosic hydroxyl groups with a variety of reagents can resolve the fibers hydrophobicity such as treatment reduces: . the swelling of the at Victoria Univ of Wellington on July 14.61]. MALKAPURAM ET AL. between matrix and fiber. 2009 . Isocyanates are chemically linked to the cellulose matrix through strong covalent bonds: both PMPPIC and PS contain benzene rings. The mechanical properties of composites reinforced with wood fibers and PVC or PS as resin can be improved by an isocyanate treatment of cellulose fibers [52. the number of cellulose hydroxyl groups. Similar results are obtained. and their delocalized electrons provide strong interactions.sagepub. Triazine Coupling Agents Triazine derivatives form covalent bonds with cellulose fibers. the hydrophilicity of the fiber’s surface. Figure 2.1174 R– N= C= O+ H– O–Cell O R – HN – C – O − Cell R. adhesion is obtained. The triazine derivatives are used to reduce the moisture absorption of cellulose fibers and their composites. Formation of urethane linkage by reaction of isocyanate and hydroxyl groups of cellulose. .

Organosilanes as Coupling Agents Organosilanes are the main group of coupling agents for glass-fiber reinforced polymers. show remarkable improvement in tensile and bending properties when compared to those of the virgin PP specimens. interfacial adhesion. were studied. and uniform distribution of matrix-fibers and the lack of fiber attrition and attenuation during tubular braiding process. and poly(lactic acid) (PLA) composites. at Victoria Univ of Wellington on July 14. which are used in reinforced composites. sisal fibers reinforced PP composites in water at three different temperatures. A line of indents was produced from the fiber to the matrix. They have been developed to couple virtually any polymer to the minerals. The water absorption properties of coir. showing a great loss in mechanical properties of the water-saturated samples compared to the dry samples [3]. 50. [1] have reported that the jute/PP unidirectional composites. A decrease in tensile properties of the composites was demonstrated. orientation. The high-tenacity man-made cellulose filament yarn (rayon tyre cord yarn) reinforced PP. Downloaded from http://jrp. and 708C. 2009 . such as the wettability of resin melts into fiber bundles.Natural Fiber Reinforced Polypropylene Composites Cellulose fiber 1175 H2NR CI N CI N N CI CI N R HN N N CI R HN N H O O N CI N Cellulose fiber Figure 4. depending on nano-indentation depth and spacing [4]. The improvements in the mechanical properties are broadly related to various factors. high impact polystyrene (HIPS). The distinct properties of the transition zone were revealed by 1–4 indents. PROCESSING AND PROPERTIES OF NATURAL FIBER REINFORCED PP COMPOSITES Khondker et al. There was a gradient of hardness and modulus across the interphase region. Modification of cellulose fibers with triazine derivatives. specimens with only 20% of jute fiber (Vf ) content.sagepub. The hardness and elastic modulus of a cellulose fiber-reinforced PP composite were investigated by nano-indentation with a continuous stiffness technic. 23.

3. and notched impact strength are 80 MPa. solution mixing (toluene) followed by extrusion and compression molding Haake rheocord mixer Compression molding through a sheet stacking technic Hydraulic press using film stacking technic Internal mixer and injection molding machine Haake rheocord and injection molding Single-screw extruder and injection molding Reference number 6 26 27 37 41 43 44 55 58 60 62 63 The pultrusion compounding method developed for highly homogeneous composites. compression molding EXPRESS processing (Extrusion press processing) Compression molding Pultrusion technic applied to conventional co-rotating twin-screw extruder and composite specimens prepared by injection molding Heated press in a mold Pultrusion and compression molding Vacuum heating and compression molding Twin-screw extruder and injection molding Single-screw extruder and injection molding Hydraulic press Reference number 1 2 4 5 23 28 29 36 42 57 Table 4. The biggest Downloaded from http://jrp. Short fiber reinforced PP composites. and the uniaxial elastic modulus was considerably enhanced. MALKAPURAM ET AL. 2009 . 85 kJ/m2. In contrast. Charpy unnotched. By increasing draw ratio. similar reinforcing effects are observed. Continuous fiber reinforced PP composites. respectively [5]. morphological and dynamic mechanical properties of PP–cellulose fiber (CF) composites. Table 3. typical values for tensile strength.sagepub. Amash and Zugenmaier [6] investigated the thermal.5 GPa. except for the impact behavior of HIPS. The effects of drawing on the structure and physical properties of PP–CF composites were also at Victoria Univ of Wellington on July 14. Fiber Jute yarn Non wovens of flax and sisal fiber Uni-directional lyocell fiber Hightenacity cellulosefilament yarn (rayon tyre cord yarn) Unidirectional and multidirectional flax fiber Flax fiber yarn Flax fiber yarn Jute fiber yarn Sisal fiber yarn Kapok/cotton fabric Processing technic Tubular braiding technic. modulus. the impact characteristics of PLA are drastically improved increasing the unnotched and notched Charpy strengths by 380% and 200%.1176 R. A high impact resistance level is maintained also at low temperatures where the matrix material becomes brittle. the melting peak of PP shifted to higher temperatures suggesting a constrained melting. where the reinforcing fibers interfere with the impact modification of the matrix polymer. and 12 kJ/m2. For the other matrix materials. Fiber Cellulose fiber Flax fiber Flax fiber Chopped jute fiber Pinewood fiber Sisal fiber Chopped sisal fiber Kenaf fiber Pineapple leaf fibre Vetiver grass Bamboo fiber Date palm leaves Processing technic Twin-screw extruder and hydraulic press Haake rheomix and injection molding Twin-screw extruder and injection molding Shear K-mixer and injection molding Laboratory sigma blade mixer and injection molding Melt mixing (Haake rheocord mixer). For a fiber load of 30 wt%. respectively.

hemp. kenaf. single-screw extruder and injection molding Twin-screw extruder and compression molding Single-screw extruder and compression molding Twin-screw extruder and injection molding Powder impregnation through compression molding and extrusion followed by injection molding Heated roll mixer and injection molding Brabender internal mixer and compression molding Compression molding using a film stacking method Twin-screw extruder and injection molding Single fiber embedded inside two previously built sheets of PP matrix by compressing at melting point Two roll mill and injection molding 12 12 14 15 16 17 18 19 20 21 22 24 30 31 32 33 34 35 Bleached soft wood pine fibers Pinewood saw dust Granules prepared by single-screw extruder Wood material of radiate pineMixer and hot press (Pinus radiate) Rice husk flour filler Single-screw extruder and injection molding Saw dust/Rice husk Kinetic mixer and injection molding Rice husk Twin-screw extruder and injection molding Rice husk Single-screw extruder and injection molding Saw dust Mixer and compression molding Saw dust Haake rheo mixer and compression molding Luffa fiber Haake rheocord mixer and compression molding Wheat straw fibers Brabender mixer and injection molding Paper sludge Single-screw etruder and compression molding Coconut fiber Haake rheocord mixer and compression molding Layer of kenaf Plied up alternatively and pressed in a heated press Rice husk Pellets processed by twin-screw extruder 38 39 40 45 46 47 48 49 50 51 52 53 54 56 61 Downloaded from http://jrp. luff sponge and cellulose from pulp fiber Cellulose whiskers Rice husk and wood flour fiber Alfa. jute and coir Hemp fiber Jute and hemp fiber Processing technic Brabender mixer and processed by compression molding Solvent mixing followed by hot press Twin-screw extruder and injection molding Brabender mixer and compression molding Melt mixing (plastomill) and compression molding Brabender and hydraulic press 1177 Reference number 3 7 8 9 10 11 Droplet method Hot press High-speed mixer and injection molding Single-screw extruder and compression molding Twin-screw extruder and injection molding Mixer and injection molding Haake rheomix 600 equipped with roller blades rotor and compression molding woodtruder and die Haake rheomix.Natural Fiber Reinforced Polypropylene Composites Table at Victoria Univ of Wellington on July 14. coir. bleached soft wood. Particulate fiber reinforced PP composites. Fiber Sisal.sagepub. Avicel fibers Cellulose fibers Eucalyptus wood. ground corncob and spent brewery grain fibers Cellulose fibers Eucalyptus wood fibers Lignocel fiber Pine free saw dust Kraft pulp of eucalyptus fiber Hard wood dust Aspen pulp fiber Pinewood flour Liquified wood mill Wood fiber Wood fiber Flax (pulp) fiber Chopped hemp fiber Hemp strands Hemp fiber Sisal. 2009 .

The tensile strength and modulus of the lignocellulosic filler–PP composite made with the twin-screw extruding system were improved in the case of the composite made without any compatibilizing agent and significantly improved in the case of the composite made with the compatibilizing at Victoria Univ of Wellington on July 14. MALKAPURAM ET AL. [12] have optimized the fiber treatments for PP/cellulosic-fiber composites. initiation strength was observed by PP modification of fibers resulting in the crack propagation strength. Although the properties of some blends are acceptable for some applications.1178 R. compared with the lower molecular weight PP. Qiu et al. On the other hand. The tensile and Izod impact strength properties of rice-husk flour and wood flour as the reinforcing filler and different compatibilizing agents. The nanocomposites obtained with the surfactant-modified whiskers exhibited enhanced ultimate properties when compared to the neat matrix or to the composites containing the other filler types [7]. The tensile strength of the PP-wood-based composites decreased significantly with increasing wood fiber content and no significant change in modulus of elasticity was found for any weight fraction of wood fiber. 2009 . influence was observed for the samples of PP–spun cellulose and the lowest for neat PP. [11] have investigated that the loading of LDPE with natural fibers leads to a decrease in tensile strength of the pure polymer. the composites derived from higher molecular weight of PP exhibited stronger tensile strength at the same cellulose content. and g-mercaptoproyltrimethoxy silanes (MRPS) displayed good mechanical performances. as compared with those made with the single-screw extruding system. with hexadecyltrimethoxy-silanes (HDS) bearing merely aliphatic chain only a modest enhancement on composite properties was observed [9]. Joly et al. but the similar impact strength of both samples with different extruding processes might be due to the fact that impact test is not discriminating enough to reveal the difference in dispersion status of the present composites [8]. While the modification of cellulose fiber was done by isocyanates for improvement in the rupture. Georgopoulos et al. due to the improved dispersion of the filler. In addition to the fibrillar structure of the oriented PP. Fiber pullout was observed on most of the Downloaded from http://jrp. by optimizing fiber–polymer interface characteristics. by assessing their mechanical properties and the morphological characteristics of their fracture surfaces. Young’s modulus increased due to the higher stiffness of the fibers. The nanocomposite films of isotactic PP reinforced with cellulose whiskers highly dispersed with surfactant were prepared for the first time and compared with either bare or grafted aggregated whiskers.sagepub. The Izod impact strengths of the composites made with the two different extruding systems were almost the same. further improvement is necessary. the degree of dispersion of the fillers might influence the notched impact performance. The mechanical properties of the CFs reinforced polyethylene composites increased with increasing the average fiber length and the composite materials prepared using both matrices and cellulose fibers treated with g-methacryloxypropyltrimethoxy silane (MPS). In one method the grafting of a PP chain by an ester bond capable of co-crystallizing or entangling with the fibers was used. On the other hand. [10] have reported that PP with higher molecular weight revealed stronger interfacial interaction with cellulose fibers in the composites. The tensile properties of the composites made with the twin-screw extruding system were better than those of the composites made with the single-screw extruding system. the highly CF orientation and the efficient compatibilization in composites are responsible for the effects observed in the drawn samples.

Chemical foaming agents have also an effect on surface roughness of the composites which decreased surface roughness of the foamed composites compared to the nonfoamed composites. Downloaded from http://jrp. These results indicate a lack of adhesion between PP and wood fiber [13]. Using standard least-squares parameter estimation procedures and statistical analysis. Finally. maleated PP (MAPP). that is. percentage of MAPP coating on the wood fiber (C ) and type of matrix (M )). was investigated. whereas 85% increase in flexural properties was observed [16]. Tensile and flexural tests are performed on the foamed composites to investigate the dependence of these properties on the density (specific properties) of foamed specimens and compared with nonfoamed composites and MAH–PP has improved the physico-mechanical properties up to 80% [14]. and a nucleating agent on the viscoelastic properties of different types of extruded PP–wood plastic composites manufactured from either a PP homopolymer. [18] have evaluated the tensile and flexural performance of PP–wood fiber composites. The impact fracture behavior of PP/wood fiber composites modified with maleated PP as compatibilizer and poly(butadiene styrene) rubber as impact modifier has been studied by a Charpy impact testing method. tensile modulus (TM) and elongation at yield (E ). Jungil Son and his coworkers analyzed the effect of process additives. Optical microscopy showed that the cells are round and cell sizes are affected by chemical foaming agents. empirical models were built and parameter values and co-variances were computed. Young’s modulus. 2009 . Water absorption and thickness swelling of the composites were also investigated. experimental details regarding the preparation of optimum composites as predicted by empirical models are discussed. The density of microfoamed hard wood fiber–PP composites reduced around 30% and decreased up to 0. While the crack initiation energy is mostly only a little material dependent and reflects the matrix behavior.741 g/cm3 by using an exothermic chemical foaming agent. Tensile strength of composites so prepared increased by almost 45%. The addition of the compatibilizer resulted in greater reinforcement of composites. prepared by using m-TMI-g-PP as the compatibilizer. as indicated by the improvement in mechanical properties. elongation at yield and flexural strength was determined through a 22Á31 factorial design (where the variables chosen were: fiber content (F ).com at Victoria Univ of Wellington on July 14. The effect of these variables on tensile strength. The effect of filler concentration on the mechanical properties of bleached kraft pulp of eucalyptus reinforced PP composites. the crack propagation energy is much more influenced by the morphology [15].sagepub. Both the impact modifier and the compatibilizer toughen the PP matrix enhance the total fracture energy of the modified composites.a-dimethylbenzyl-isocyanate (m-TMI) onto isotactic PP in a twin-screw extruder. Costa et al. The selected responses of flexural data were stress at maximum load (FS) and flexural modulus (FM). Novel compatibilizer (m-TMI-g-PP) with isocyanate functional group was synthesized by grafting m-isopropenyl-a. The mechanical properties (responses) selected from tensile data were stress at maximum load (TS). The analysis of variance of the experimental and predicted data shows that the constructed models provide a fair approximation of actual experimental measurements.Natural Fiber Reinforced Polypropylene Composites 1179 PP composite fracture surfaces examined using SEM. The neat PP and unmodified PP/wood fiber composite exhibit brittle fracture and nearly elastic behavior while the impact modifier and compatibilizer cause elastic to elastic–plastic transition dominated by unstable crack propagation. Tensile and flexural tests of foamed composites were investigated as a dependence of function of density (specific properties) of foamed specimens and compared with nonfoamed composites based on MAH–PP has improved the physico-mechanical properties up to 80%.

a high crystallinity PP. [26] have studied the effect of fiber treatments with maleic anhydride. Downloaded from http://jrp. flax fiber/PP composites also showed transcrystallinity. To analyze the effect of the frequency on the dynamic mechanical properties of the various composites. 5. Addition of flax fiber increased crystallization rate of PP as revealed by DSC. after the interfacial strength is optimized. Keener et al. Peak performance was demonstrated in agrofiber PP composites by selecting a maleated coupler that has the appropriate balance of molecular weight and maleic anhydride content. storage modulus (E0 ). and loss modulus (E00 ) were measured using a dynamic mechanical thermal analyzer. MALKAPURAM ET AL. The UD composites of boiled flax combined with MAA-PP show the best mechanical properties. and alkalization on thermal stability of flax fiber and crystallization of flax fiber/PP composites. thermogravimetry (TG) analysis was used. The use of different methods involves a small discordance in the wettability values. From these results. In order to compare thermal stability of flax fibers. The applied treatments were maleic anhydride (MA). Kinetic parameters have been determined by the Kissinger method. Composites containing MAPP showed highest mechanical properties. The treatment effects on the fibers have been characterized by infrared spectroscopy. Dynamic mechanical thermal properties. vinyltrimethoxy silane. flax treatment did not lead to the expected property improvements for MD composites. Arbelaiz et al. Results showed that all treatments improved thermal stability of flax fibers. 10. maleic anhydride–polypropylene copolymer (MAPP) and vinyl trimethoxy silane (VTMO). maleic anhydride PP copolymer. tensile strength and stiffness) of flax/PP composites are effectively improved by compatibilization of the fiber/matrix interphase.1180 R. The mechanical properties (i. economical manufacturing and the efficient interaction of maleic anhydride with the functional surface of fiber reinforcements. Two technics have been used to determine the surface energy values: the dynamic contact angle method for the long flax fibers and the capillary rise method for the irregular pulps. [25] used maleated coupling agents to strengthen the composites containing fillers and fiber reinforcements. and 25 Hz) and at a heating rate of 58C/min. Nevertheless.. DMA tests were performed over a temperature range of 20–1008C. pressure volume temperature (PVT) measurements and polarized optical microscopy (POM) technics. the internal fiber structure becomes the weakest point [27]. at four different frequencies (1. The most important factor limiting the properties of the composites lies in the intricate structure of the fibers themselves. polymer damping peaks (tan ).e. 2009 . whilst the MA and VTMO-treated fiber showed virtually no improvement compared to untreated ones [24].com at Victoria Univ of Wellington on July 14. The wood–plastic composites were manufactured using 60% pine wood flour and 40% PP on a Davis-Standard Woodtruder. Besides depending on fiber surface treatment and crystallization temperature. the three treatments reduce the polar component of the surface energy of the fiber. Contrary to the UD composites. or a PP impact copolymer using dynamic mechanical thermal analysis. The established role of maleated polyolefins results from two main factors. Van de Valde and Kiekens [23] have analyzed the unidirectional (UD) and multidirectional (MD) flax/PP composites at different process times and temperatures.sagepub. The composites were compounded with two kinds of flax fibers (natural flax and flax pulp) and PP. the activation energy of the various composites was measured using an Arrhenius relationship to investigate the effect of MAPP and the nucleating agent on the measurement of the interphase between the wood and the plastic of the extruded PP wood–plastic composites [19].

In a series of experiments carried out with yarns of two different flax fiber contents. Kenaf. [34] investigated the optimization of New Zealand grown hemp fiber reinforced PP at Victoria Univ of Wellington on July 14.sagepub. the preheating and die temperatures and also the pulling speed. was developed to improve the prediction of composite tensile properties [29]. Coir fiber composites displayed the lowest mechanical properties. and sisal composites showed comparable tensile strength and modulus properties but in impact properties hemp appears to outperform kenaf. [38] studied the PP-based composites. Doan et al.88 GPa. In most cases the specific properties of the natural fiber composites were found to compare favorably with those of glass [33].2 MPa. The optimum growing period was found to be 114 days. [36] investigated the effect of maleic anhydride grafted PP (MAPP) coupling agents on the properties of jute fiber/PP composites. Effect of impact modifier on 0. The modification of fibers (hemp–GMA) and polyolefin matrix (PP-g-GMA). were carried out to improve the fiber–matrix interactions. A complete characterization of each profile was conducted in order to examine the influence of processing parameters on the profile quality. The tensile strength of hemp strand/PP composites can be as high as 80% of the mechanical properties of glass fiber/PP composites [31]. SEBS. hemp. and had a tensile strength of 47. All composites displayed higher tensile modulus (2. 2009 . 4. ´ s et al. functionalized by means of melt grafting reactions with glycidyl methacrylate (GMA) were prepared by batch mixing. The mechanical properties were evaluated by performing three-point bending as well as Charpy impact tests [28]. SEBS-g-GMA). supplemented with parameters of composite porosity content and anisotropy of fiber properties. compatibilization with PP-g-GMA (10 phr) resulted in an increased stiffness of the composites as consequence of an improved fiber–matrix interfacial adhesion [32]. Tensile modulus increased only by 12% after incorporation of untreated fibers to PP matrix. The composites of isotactic PP with hemp fibers (Cannabis sativa). which are the most relevant parameters regarding the potential future pultrusion of natural fiber composite profiles at industrial scale. respectively. and 14 wt% indicated that both impact and tensile properties showed increasing trend with the compatibilizer but the reverse was true for the flexural properties [37]. Rectangular cross-sectional profiles produced by using a self-designed pultrusion line. reinforced with surface modified Girone pine fibers. but their impact strength was higher than that of jute and kenaf composites. Pickering et al. The strongest composite consisted of PP with 40 wt% fiber and 3 wt% MAPP. A modified version of the ‘rule-of-mixtures’. The tensile modulus. the pultrusion parameters were varied. as well as the addition of various compatibilizers (PP-g-GMA.Natural Fiber Reinforced Polypropylene Composites 1181 Pultrusion technic developed for flax reinforced PP commingled yarn containing discontinuous flax and PP fibers. and a Young’s modulus of 4. Unidirectional composites from filament wound nontreated flax yarns and PP fabricated foils composite have exhibited axial stiffness and strength in the range 27–29 and 251–321 MPa. In particular. impact strength and the ultimate tensile stress of kenaf reinforced PP composites were found to increase with increasing fiber weight fraction. The addition of 2 wt% MAPP to PP matrices improved the adhesion strength with jute fibers and the mechanical properties of composites. 9. Treatment with silane led to a significant rise (about 60% compared with Downloaded from http://jrp.9 GPa) and lower elongation at break as compared to plain PP. producing fibers with an average tensile strength of 857 MPa and a Young’s modulus of 58 GPa.

MALKAPURAM ET AL. No significant influence of chemicals added in the samples was found on surface roughness values of the samples manufactured from particle and fiber of radiata pine.44] prepared sisal fiber reinforced PP composites by melt-mixing and solution-mixing methods. Wechsler and Hiziroglu [40] have studied wood–plastic composite (WPC) specimens having 60 and 80% particle and fiber of radiata pine (Pinus radiata) mixed with PP (plastic). The methods enhanced the tensile properties of the composites. namely Structor TR 016 which is a coupling agent. followed by MPS. The tensile properties for PP. Three different types of wood/PP mixture were prepared: (1) PP–untreated wood. and the tensile strength was increased by about 10%.5 to 1. Borysiak and Doczekalska [39] studied the wood sawdust/PP composites based on polish timber species pine wood (Pinus silvestris L. Young’s modulus improvements compared to the unreinforced matrix of 77 and 177% were obtained using PMPPIC and MAPP. were obtained using PMPPIC and MAPP. and (3) PP–esterified wood with maleic anhydride. Joseph et al. and their combinations. It was found that treated fiber composites show superior properties compared to the untreated system. This is attributed to the nucleating effects Downloaded from http://jrp. The particle-based samples had rougher surface characteristics than those of fiber-based ones. (2) PP–NaOH treated wood. 20. high temperature (HT) and low temperature (LT) specimens were compared. DSC measurements exhibited an increase in the crystallization temperature and crystallinity. separately and combined. substantially greater than reported elsewhere in the literature. The effect of fiber content and chemical treatments on the thermal properties of sisal/PP composites was also evaluated. It was observed that the incorporation of 10 wt% of sisal fibers increases Young’s modulus by about 150%. 2009 . The chemical treatment of wood caused changes of crystal conversion and half crystallization time of PP matrix. and g-aminopropyltrimethoxysilane (AMPS). upon the addition of fibers to the PP matrix. A modest improvement compared to the unreinforced matrix strength of 4% and much greater improvement of 123%. flexural modulus increased by 6.) as a softwood species and beech wood (Fagus silvatica L.1182 R. Thickness swelling of the samples were also improved by the presence of additives in the panels. respectively. Based on the initial finding of this study static bending properties of the samples enhanced by the above chemicals were added into both particle and fiber-based specimens.0 mm. Micrographs taken on a scanning electron microscope (SEM) revealed that coupling agent and pigment resulted in more homogeneous mixture of wood and plastic together. and 8% in the presence of MPS. and MRPS. and four different additives. The size of wood saw dust ranged from 0. It is interesting that crystallization of PP depends on the kind of wood. Flexural modulus was amplified by 130% with fiber addition and modestly enhanced after silane treatment compared with that of untreated fibers. 5. HDS.sagepub. [43. the kinetic parameters of crystallization of PP by differential scanning calorimetry (DSC) were investigated. CIBA UV filter coating (TINUVIN 123S). The processing of sisal fiber reinforced PP composites by injection molding was reported by Li and his coworkers. respectively. CIBA blue pigment (Irgalite). Pickering and Ji [41] studied the effects of poly[methylene (polyphenyl isocyanate)] (PMPPIC) and MAPP coupling agents. AMPS. The reinforcement efficiency for LT specimens is slightly higher than HT samples [42]. respectively. on the strength and Young’s modulus of New Zealand radiata pine-reinforced PP composites. that of unfilled matrix) in tensile modulus. CIBA anti-microbial agent (IRGAGUARD F3510) as fungicide.) as a hardwood species. A higher effect was noted for MRPS. In this at Victoria Univ of Wellington on July 14. HDS.

resulting in the formation of transcrystalline regions. Suarez et al. six test temperatures (À30. and in the tensile test.Natural Fiber Reinforced Polypropylene Composites 1183 of the fiber surfaces. The analysis of variance of the experimental and predicted data show that the constructed models provide a fair approximation of actual experimental measurements. and its mechanical and morphological properties examined as a function of the amount of compatibilizing agent used. respectively. In the sample preparation. and maleic anhydride grafted polypropylene (MAPP) were at Victoria Univ of Wellington on July 14. The effects of coupling agents on the mechanical. The addition of higher MAPP content to the PP composites produces better adhesion of saw dust to PP matrix and an increase in the tensile strength. and 40 wt%) and three levels of compatibilizing agent content (1. 500. Both the notched and the unnotched Izod impact strengths were almost the same with the addition of compatibilizing agent. [45] prepared a particle-reinforced composite. In order to enhance the interfacial interactions between the PP matrix and the luffa fiber. elongation at yield. 80. and flexural strength was determined through a 22Á31 factorial design. The interfacial interactions Downloaded from http://jrp. but the tensile properties were significantly improved with the addition of the compatibilizing agent.sagepub. 50. (3-aminopropyl)-triethoxysilane (AS). [46] studied flammability of PP. Young’s modulus. 20. 10. and water sorption properties of luffa fiber (LF)/(PP) composites were studied. 3-(trimethoxysilyl)-1-propanethiol (MS). three different types of coupling agents. Sain et al. The tensile strengths of the composites decreased as the filler loading increased. Tensile strength and Young’s modulus increased with employment of the coupling agents accompanied by a decrease in water absorption with treatment due to the better adhesion between the fiber and the matrix. 20. [50] studied the morphological behavior of composites of PP or PP plus MAPP and saw dust coated with 22. experimental details regarding the preparation of optimum composites as predicted by empirical models were discussed. 3. and 5 wt%) were used. type of matrix (PP or MAPP) and composition (10. The maximum improvement in the mechanical properties was obtained for the MS treated LF composites. 0. the melting peak of the PP component was shifted to higher temperatures suggesting a constrained melting. rice husk filled PP composites. 20. in that rice-husk flour as the reinforcing filler and PP as the thermoplastic matrix polymer. and flame retarding effect of magnesium hydroxide for these composites by horizontal burning rate and oxygen index tests. four levels of filler loading (10. 30. compared to the composite without flame retardant Coutinho et al. Han-Seung yang et al. On increasing the fiber content. The tensile properties of composites with up to 10% MAPP have not been improved by increasing MAPP content. This has been attributed to the poor filler/matrix adhesion.4 wt% MAPP were prepared under fixed processing conditions (mixing temperature. Despite the presence of a coupling agent. or 30 wt%) on the tensile and flexural performance of PP–wood fiber composites was studied. [49] studied the influence of the amount of MAPP coating of vinyl-tris (2-methoxy ethoxy) silane treated woodfibers (2 or 10 wt%). The tensile properties of the untreated and treated composites were determined as a function of filler loading. 100. 2009 . and 1500 mm/min) were used. morphological. and 1108C) and five crosshead speeds (2. rate of rotation and mixing time). The effect of these variables on tensile strength. the addition of flame-retardants shows a negative impact on the tensile and flexural properties of the composites and the properties show a reduction of 17 and 15%. The PP composites containing 2–15 wt% of LF were prepared in a torque rheometer. SEM was performed to analyze the tensile fracture surfaces and the interfacial fiber/matrix adhesion. Finally.

1184 R. Composites with lignin as a compatibilizer possess higher flexural properties as compared to the control composites. The increase of heating time contributed to better wetting between kenaf and PP. [54] studied the effect and mechanical properties of lignin as a compatibilizer in the coconut fiber–PP. and physical. Wheat straw fiber reinforced PP composites exhibited significantly enhanced properties compared to virgin PP. The tensile modulus and tensile strength of the composites were found to be increasing with fiber content in accordance with the rule of mixtures. Results show that fiber modification gives a significant improvement to the thermal properties of the plant fibers. Jang and Lee [53] fabricated the paper sludge/PP composites. The effects of the number of kenaf layers. and antimony trioxide were introduced into the composites for improvement of the flame retardancy and was measured with the UL94 test. [58] investigated the tensile and flexural behaviors of pineapple leaf fiber–PP composites as a function of volume at Victoria Univ of Wellington on July 14. The improvement in the interfacial interaction was also confirmed by the Pukanszky model. with acetylation showing slightly less rigidity compared to other treatments on either the fiber or the composites. Rozman et al. Shibata et al. MALKAPURAM ET AL. This is because more kenaf layers caused better contact between kenaf and PP and prevented PP fibers from shrinking by heating. mechanical. Mwaikambo et al. The flexural modulus increased with increasing number of kenaf layers and heating time. [56] fabricated the lightweight laminate composites made from kenaf and PP fibers by press forming. Thermal and mechanical properties of the composites were investigated. Treating the reinforcement with acetic anhydride and sodium hydroxide has modified the fabric (fibers). physical. The increase of the number of kenaf layers contributed to homogeneous PP dispersion in the composite board. Panthapulakka et al. MAiPP reinforced with the plant fibers gave better flexural strength and the same flexural modulus at lower fiber content compared with glass fiber reinforced MAiPP. Composites of PP filled with 30% wheat straw fibers were prepared and their mechanical properties were also evaluated. These results indicate that wheat straw fibers can be used as potential reinforcing materials for making thermoplastic composites. The results also show that tensile properties do not improve as lignin is incorporated. and kenaf weight fraction on the flexural modulus of the composite specimen were investigated. This was due to the poor dispersion of the fibers under the processing conditions used. Flame retardants like Saytex8010. Arib et al. [57] showed that kapok/cotton fabric has been used as reinforcement for conventional PP and maleic anhydride grafted PP resins. However. the strength properties of the composites were less for chemically prepared fiber filled composites. and thermal properties. Downloaded from http://jrp. SEM results display some proof of an enhanced compatibility at the interfacial region. The modified PP improved the tensile modulus and had the least toughness of the kapok/cotton reinforced composites. 2009 . The fibers prepared by chemical process exhibited better mechanical. whereas tests on the mechanical properties of the composites showed poor tensile strength. Mg(OH)2. and thermal properties. Fibers prepared by mechanical and chemical processes were characterized with respect to their chemical composition. mechanical properties. and water resistance of composites.sagepub. morphology. Good agreement was obtained between the experimental data and the model prediction [51]. improved the filler compatibility. heating time. [52] studied the potential of wheat straw fibers prepared by mechanical and chemical processes as reinforcing additives for thermoplastics was investigated. TPP. Mercerization and weathering were found to impart toughness to the materials.

the fibers were treated with the reaction mixture of maleic acid anhydride and sunflower oil. Hemp. and impact strength decreased with increasing vetiver content. Kim et al. The hybrid effect in these composites was examined as a function of fiber content and fiber combination. and Young’s modulus of the composites. An increase in vetiver content led to an increase in viscosity. When compared to PP. The chemical treatment of the vetiver grass improved the mechanical properties of the composites. The effect of two different types of MAPE polymer. In order to achieve a sufficient interfacial adhesion. MA-grafted high-density polyethylene (HDPE-MA) and MA-grafted linear LDPE (LLDPE-MA). Acoustic emission methods revealed that there is a correlation between the physical parameters of sound waves that occurred during failure and the mechanical properties.Natural Fiber Reinforced Polypropylene Composites 1185 ´ ny [59] manufactured the basalt fiber reinforced. With increasing MAPP and MAPE content. glass. Ruksakulpiwat et al. and carbon fibers were applied besides basalt fiber in these composites. to bio-flour-filled. needle-punching. tensile strength. vetiver–PP composites exhibited higher tensile strength and Young’s modulus but lower elongation at break and impact strength. elongation at break. the thermal stability. The strength properties of hybrid composites improved owing to surface treatment and this was proven by mechanical tests and microscopic analysis. [61] investigated the effect on thermal properties of the addition of two different compatibilizing agents. storage modulus (E_ ). heat distortion temperature. and pressing. On the other hand. maleic anhydride (MA)-grafted polypropylene (MAPP) and MA-grafted polyethylene (MAPE). crystallization temperature. PP matrix hybrid composites Cziga in the process of carding. the decomposition temperature. was also examined. PP. [60] prepared the injection molded vetiver–PP composites at various ratios of vetiver content and vetiver length. as well. and low density polyethylene (LDPE) composites. tan max peak temperature (glass transition temperature: Tg) and loss modulus (Emax) peak temperature (.

however. Injection molded samples were exposed in water at 258C for up to 6 months and at 758C for up to 3 months. 65.and MAPE-treated composites was slightly increased with increasing MAPP and MAPE content. Attenuated total reflectance (FTIR-ATR) analysis confirmed this result by demonstrating the changed chemical structures of the composites following MAPP and MAPE addition. Tensile strength and elastic modulus of BFRP and BGRP samples have shown moderate reduction after aging at 258C after 6 months. Results suggest that BGRP has better fatigue resistance than BFRP at all load levels tested. Liao et al. they were reduced considerably after aging at 758C for 3 months. The thermal stability. BFRP and BGRP samples were also loaded cyclically at maximum cyclic load of 35. and 80% of their ultimate tensile stress. were studied. 2009 . [62] have studied the resistance of bamboo fiber reinforced PP composite (BFRP) and bamboo-glass fiber reinforced PP hybrid composite (BGRP) to hygrothermal aging.sagepub. and their fatigue behavior under cyclic tensile load. This enhancement of thermal stability and properties could be attributed to an improvement in the interfacial adhesion and compatibility between the rice husk flour (RHF) and the matrix due to the treatment of compatibilizing agent. 50. Moisture absorption and tensile strength degradation are suppressed by using MAPP as a coupling agent in both types of composite systems. The melting temperature (Tm) of the composites was not significantly changed but the crystallinity (Xc) of at Victoria Univ of Wellington on July 14. relaxation) were slightly increased. E_ and E__ of MAPE-treated composites were not significantly affected by the two different MAPE polymers. Downloaded from http://jrp.

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