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discussions, stats, and author profiles for this publication at: https://www.researchgate.net/publication/256923037

Biocomposites reinforced with natural fibers:

2000-2010

Article in Progress in Polymer Science · November 2012

DOI: 10.1016/j.progpolymsci.2012.04.003

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Omar Faruk Andrzej K Bledzki

Ford Motor Company, Canada West Pomeranian University of Technology, …
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Mohini Sain
University of Toronto
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 Progress in Polymer Science 37 (2012) 1552–1596

Contents lists available at SciVerse ScienceDirect

Progress in Polymer Science

journal homepage: www.elsevier.com/locate/ppolysci

Biocomposites reinforced with natural fibers: 2000–2010

Omar Faruk a,d,∗ , Andrzej K. Bledzki a,c , Hans-Peter Fink b , Mohini Sain d
a
Institut für Werkstofftechnik, Kunststoff- und Recyclingtechnik, University of Kassel, Moenchebergstrasse 3, D-34109 Kassel, Germany
b
Fraunhofer Institute for Applied Polymer Research, Geiselbergstrasse 69, D-14476 Potsdam-Golm, Germany
c
West Pomeranian University of Technology, Institute of Material Science and Engineering, 19 Piastow Ave, 70310 Szczecin, Poland
d
Centre for Biocomposites and Biomaterials Processing, University of Toronto, 33 Willcocks Street, Toronto, ON M5S3B3, Canada

a r t i c l e i n f o a b s t r a c t

Article history: Due to environment and sustainability issues, this century has witnessed remarkable
Received 3 August 2011 achievements in green technology in the field of materials science through the devel-
Received in revised form 19 April 2012 opment of biocomposites. The development of high-performance materials made from
Accepted 25 April 2012
natural resources is increasing worldwide. The greatest challenge in working with natural
Available online 2 May 2012
fiber reinforced plastic composites is their large variation in properties and characteristics.
A biocomposite’s properties are influenced by a number of variables, including the fiber
Keywords:
Biocomposites
type, environmental conditions (where the plant fibers are sourced), processing meth-
Natural fiber ods, and any modification of the fiber. It is also known that recently there has been a
Biopolymer surge of interest in the industrial applications of composites containing biofibers reinforced
Nanofiber with biopolymers. Biopolymers have seen a tremendous increase in use as a matrix for
Acetylation biofiber reinforced composites. A comprehensive review of literature (from 2000 to 2010)
Alkylation on the mostly readily utilized natural fibers and biopolymers is presented in this paper.
Silane The overall characteristics of reinforcing fibers used in biocomposites, including source,
Maleated coupling
type, structure, composition, as well as mechanical properties, will be reviewed. More-
Enzyme treatment
over, the modification methods; physical (corona and plasma treatment) and chemical
Thermoplastic
Thermosets (silane, alkaline, acetylation, maleated coupling, and enzyme treatment) will be discussed.
Injection molding The most popular matrices in biofiber reinforced composites based on petrochemical and
Compression molding renewable resources will also be addressed. The wide variety of biocomposite process-
Extrusion ing techniques as well as the factors (moisture content, fiber type and content, coupling
Pultrusion agents and their influence on composites properties) affecting these processes will be dis-
Resin transfer molding cussed. Prior to the processing of biocomposites, semi-finished product manufacturing is
Sheet molding compound also vital, which will be illustrated. Processing technologies for biofiber reinforced compos-
LFT-D method
ites will be discussed based on thermoplastic matrices (compression molding, extrusion,
Tensile
Flexural
injection molding, LFT-D-method, and thermoforming), and thermosets (resin transfer
Impact molding, sheet molding compound). Other implemented processes, i.e., thermoset com-
pression molding and pultrusion and their influence on mechanical performance (tensile,
flexural and impact properties) will also be evaluated. Finally, the review will conclude with
recent developments and future trends of biocomposites as well as key issues that need to
be addressed and resolved.
Crown Copyright © 2012 Published by Elsevier Ltd. All rights reserved.

∗ Corresponding author at: Centre for Biocomposites and Biomaterials Processing, University of Toronto, 33 Willcocks Street, Toronto, ON M5S3B3,
Canada. Tel.: +1 416 9781615; fax: +1 416 9783834.
E-mail address: o.faruk@utoronto.ca (O. Faruk).

0079-6700/$ – see front matter. Crown Copyright © 2012 Published by Elsevier Ltd. All rights reserved.
http://dx.doi.org/10.1016/j.progpolymsci.2012.04.003
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596 1553

Contents

1. Introduction . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2. Reinforcing fibers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2.1. Fiber source . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2.2. Fiber types . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2.2.1. Flax . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1554
2.2.2. Hemp . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1555
2.2.3. Jute . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1555
2.2.4. Kenaf . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1556
2.2.5. Sisal . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1556
2.2.6. Abaca . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1557
2.2.7. Pineapple leaf fiber . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
2.2.8. Ramie . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
2.2.9. Coir . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
2.2.10. Bamboo . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1558
2.2.11. Rice husk . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
2.2.12. Oil palm . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
2.2.13. Bagasse . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
2.3. Structure and chemical composition . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1559
2.4. Properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1560
2.5. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
3. Modification of natural fibers . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
3.1. Physical method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
3.1.1. Corona treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
3.1.2. Plasma treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1562
3.2. Chemical method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1563
3.2.1. Silane treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1563
3.2.2. Alkaline treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1564
3.2.3. Acetylation . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1565
3.2.4. Maleated coupling . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1565
3.2.5. Enzyme treatment . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1567
3.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1567
4. Matrices for biocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1567
4.1. Petrochemical based . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1567
4.1.1. Thermoplastic . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1568
4.1.2. Thermosets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1571
4.2. Bio-based . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1571
4.2.1. PLA (polylactide acid) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1571
4.2.2. PHB (polyhydroxybutyrate) . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1572
4.2.3. Starch . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
4.2.4. Others . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
4.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
5. Processing techniques . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
5.1. Factors influencing processing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
5.1.1. Moisture . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1574
5.1.2. Fiber type and content . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1575
5.1.3. Influence on composites properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1575
5.2. Semi-finished product manufacturing . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1576
5.3. Processing technologies for natural fiber reinforced thermoplastics . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1576
5.3.1. Compression molding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1576
5.3.2. Extrusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1576
5.3.3. Injection molding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1576
5.3.4. Long fiber thermoplastic-direct (LFT-D) method . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1577
5.4. Processing technologies for natural fiber reinforced thermosets . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1578
5.4.1. Resin transfer molding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1578
5.4.2. Sheet molding compound . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1578
5.5. Other processes . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1579
5.5.1. Thermosets compression molding . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1579
5.5.2. Pultrusion . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1579
5.5.3. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1579
6. Performance of biocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1580
6.1. Tensile properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1580
6.2. Flexural properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1581
6.3. Impact properties . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1581
1554 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596

6.4. Summary . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1582

7. Development and future trends of biocomposites . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1582
8. Conclusions . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1584
References . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . . 1584

2. Reinforcing fibers
1. Introduction
An increased awareness that non-renewable resources
There is a growing trend to use biofibers as fillers and/or are becoming scarce and our inevitable dependence on
reinforcers in plastics composites. Their flexibility during renewable resources has arisen. This century could be
processing, highly specific stiffness, and low cost (on a vol- called the cellulosic century, because more and more
umetric basis) make them attractive to manufacturers. This renewable plant resources for products are being discov-
century has witnessed ever-increasing demands for the uti- ered. It has been generally stated that natural fibers are
lization of plastics as important raw materials, more than renewable and sustainable, but they are in fact, neither. The
80% of which are thermoplastics. Biofiber reinforced plas- living plants are renewable and sustainable from which the
tic composites are gaining more and more acceptance in natural fibers are taken, but not the fibers themselves.
structural applications.
Technological development connected with consumer 2.1. Fiber source
demands and expectations continues to increase demands
on global resources, leading to major issues of material The plants, which produce natural fibers, are classified
availability and environmental sustainability. Over the last as primary and secondary depending on their utilization.
few decades biofiber composites have been undergoing a Primary plants are those grown for their fiber content while
remarkable transformation. These materials have become secondary plants are plants in which the fibers are pro-
more and more sufficient as new compositions and pro- duced as a by-product. Jute, hemp, kenaf, and sisal are
cesses have been intensively researched, developed and examples of primary plants. Pineapple, oil palm and coir
consequently applied. The petroleum crisis made biocom- are examples of secondary plants. Table 1 shows the main
posites significantly important and biocomposites have fibers used commercially in composites, which are now
become engineering materials with a very wide range of produced throughout the world [16].
properties. However, like all materials, they are constantly
under competitive pressure from the global market, which 2.2. Fiber types
in turn, necessitates continuous research. The times of
simply mixing plastics with natural waste fillers and char- There are six basic types of natural fibers. They are clas-
acterizing their main properties are gone. sified as follows: bast fibers (jute, flax, hemp, ramie and
The concept of using bio-based plastics as reinforced kenaf), leaf fibers (abaca, sisal and pineapple), seed fibers
matrices for biocomposites is gaining more and more (coir, cotton and kapok), core fibers (kenaf, hemp and jute),
approval day by day. The developments in emerging bio- grass and reed fibers (wheat, corn and rice) and all other
based plastics are spectacular from a technological point of types (wood and roots).
view and mirror their rapid growth in the market place. The
average annual growth rate globally was 38% from 2003 to 2.2.1. Flax
2007. In the same period, the annual growth rate was as Flax, Linum usitatissimum, belongs to the bast fibers. It
high as 48% in Europe. The worldwide capacity of bio-based is grown in temperate regions and is one of the oldest fiber
plastics is expected to increase from 0.36 million metric crops in the world. The bast fiber flax is most frequently
ton (2007) to 2.33 million metric ton by 2013 and to 3.45 used in the higher value-added textile markets. Nowadays,
million metric ton in 2020. The main product in terms of it is widely used in the composites area.
production volumes will be starch-based plastics, PLA and The static and dynamic mechanical properties of non-
PHA [1]. woven based flax fiber reinforced PP composites were
The increasing number of publications during the recent
years including reviews [2–9] and books [10–14] reflect the Table 1
growing importance of these new biocomposites. Bledzki Commercially major fiber sources.

and Gassan have reviewed the reinforcement of the most Fiber source World production (103 ton)
readily used natural fibers in polymer composites up until
Bamboo 30,000
1999 in their review paper [15]. This paper aims to review Jute 2300
more current reinforcement of natural fibers in polymer Kenaf 970
composites from 2000 to 2010. This paper will not address Flax 830
Sisal 378
natural fibers from animals (e.g., silk or wool) or cotton
Hemp 214
or man-made cellulosic fibers. This review also excludes Coir 100
wood fiber or flour. Given the broadscope of this article, it Ramie 100
will inevitably be incomplete, but will hopefully provide Abaca 70
a sensible overview of the most popular natural fibers in Sugar cane bagasse 75,000
Grass 700
polymeric composite materials in the last 11 years.
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
studied considering the effect of zein coupling agent [17].
Zein is a protein, extracted from corn and used as solution.
Composites containing zein coupling agent were found
to possess improved mechanical properties. The storage
modulus of composites was found to increase with zein
coupling agent coating due to enhanced interfacial adhe-
sion.
The tensile mechanical properties of flax fibers are esti-
mated according to their diameter and their location in
the stems [18]. The large scattering of these properties is
ascribed to the variation of the fiber size along its longitu-
dinal axis. The higher values of the mechanical properties
of the fibers issued from the middle of the stems are associ-
ated with the chemical composition of their cell walls. The
mechanical properties of unidirectional flax fiber/epoxy
matrix composites are studied as a function of their fiber
content. The properties of the composites are lower than
those expected from single fiber characteristics.
Various investigations of flax fiber/polypropylene com-
posites have been completed. These studies focus on many
different variables, including: comparison between NMT
(natural fiber thermoplastic mat) and GMT (glass fiber
thermoplastic mat) [19], the influence of fiber/matrix mod-
ification and glass fiber hybridization [20], the effect of fiber
treatment on thermal and crystallization properties [21],
the influence of surface treatment on interface by glycerol
triacetate, thermoplastic starch, ␥-methacryl oxypropyl
trimethoxy-silane and boiled flax yarn [22], comparison of
matrices (PP and PLA) on the composite properties [23],
the effects of material and processing parameters [24], and
the influence of processing methods [25]. Buttler [26] pre-
sented the feasibility of using flax fiber composites in the
coachwork and bus industry.
The effect of bio-technical fiber modification [27], frac-
ture behavior and toughness [28], the influence of alkaline
fiber treatment on unidirectional composites [29], the
effect of processing parameters [30] on the consecutive
decortication stages of flax fibers (retting, scutching, and
hackling) on the flax fiber reinforced epoxy composites
have also been evaluated.
Flax fiber composites reinforced with polyester resin
have been evaluated for thermal degradation and fire
resistance [31], chemical treatments on surface properties
and adhesion [32], and the effect of chemical treat-
ments on water absorption and mechanical properties [33].
Three resins from soybean oil (methacrylated soybean oil,
methacrylic anhydride modified soybean oil, and acetic
anhydride modified soybean oil) were used also as matrices
for flax fiber reinforced biocomposites [34].
2.2.2. Hemp
Another notable bast fiber crop is hemp, which belongs
to the Cannabis family. It is an annual plant that grows
in temperate climates. Hemp is currently the subject of
a European Union subsidy for non-food agriculture, and
a considerable initiative in currently underway for their
further development in Europe.
Composites of PP with hemp fibers, which were func-
tionalized by means of melt grafting reactions with glycidyl
methacrylate (GMA) and prepared by batch mixing, were
examined [35]. The modification of fibers and the PP matrix,
1555
as well as the addition of various compatibilizers were
carried out to improve the fiber–matrix interactions. Com-
pared to the unmodified system, a modified composite
showed improved fiber dispersion in the PP matrix and
higher interfacial adhesion as a consequence of chemical
bonding between the fiber and the polymer (PP/Hemp).
The thermal stability and phase behavior of the composites
was largely affected by the fiber and matrix modification.
Changes in the spherulithic morphology and crystallization
behavior of PP were observed in the composites due to the
nucleating effect of the hemp fibers. Moreover, a marked
increase in the PP isothermal crystallization rate (in the
range 120–138 ◦ C) was recorded with increasing content of
modified hemp. All composites displayed a higher tensile
modulus (about 2.9 GPa) and lower elongation at break as
compared to plain PP; compatibilization with modified PP
(10 phr) resulted in an increased stiffness of the composites
as a result of improved fiber–matrix interfacial adhesion.
Pickering and co-workers [36–38] investigated the
effects of chelator, white rot fungi, and enzyme treatments
on the separation of hemp fibers from bundles, and the
improvement of the interfacial bonding of the hemp fibers
with the PP matrix. The obtained results showed that the
interfacial shear strength of the treated fiber composites
was higher than that for untreated fiber composites. This
verifies that the hemp fiber interfacial bonding with PP was
improved by the white rot fungi treatment. Composites
consisting of hemp fibers treated with chelator concentrate
had the highest tensile strength of 42 MPa, which equals
an increase of 19% compared to composites with untreated
hemp fiber.
Hemp fiber reinforced PP composites exhibited interest-
ing recyclability [39]. The obtained results prove that the
mechanical properties of hemp fiber/PP composites remain
well preserved, despite the number of reprocessing cycles.
The Newtonian viscosity decreases with cycles, indicating a
decrease in molecular weight and chain scissions induced
by reprocessing. The decrease of fiber length with repro-
cessing could be another reason for decrease of viscosity.
Epoxy resins, which were used as a matrix for hemp
fiber reinforced composites, were studied regarding the
effect of fiber architecture on the falling weight impact
properties [40], properties and performances of compos-
ites for curved pipes [41], impact load performance of resin
transfer molded composites [42], micro-mechanics of the
composites [43], the influence of hybrid blends made of
soybean oil and nanoclay [44], and the usefulness of unret-
ted hemp as a source of fiber for biocomposites [45].
Kunanopparat et al. [46,47] studied the feasibility of
wheat gluten as a matrix for hemp fiber reinforced compos-
ites regarding their thermal treatment and plasticization
effect on the mechanical properties.
2.2.3. Jute
Jute is produced from plants of the genus Corchorus,
which includes about 100 species. It is one of the cheap-
est natural fibers and is currently the bast fiber with the
highest production volume. Bangladesh, India and China
provide the best condition for the growth of jute.
Ray and co-workers [48–50] extensively investigated
alkali treated jute fiber reinforced with vinyl ester resin.
1556 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
In their studies, they regarded the dynamic, mechanical,
thermal, and impact fatigue behavior compared to that of
untreated jute fiber–vinyl ester composites. Longer alkali
treatment removed the hemicelluloses and improved the
crystallinity, enabling better fiber dispersion. The dynamic,
mechanical, thermal and impact properties were superior
owing to the alkali treatment, comprising treatment time,
concentration and conditions.
Mohanty et al. [51] investigated effects and influence
of surface modification on the mechanical and biodegrad-
ability of jute/Biopol and jute/PA (Poly Amide) composites.
Enhancements in tensile strength of more than 50%, 30%
in bending strength and 90% in impact strength were
observed in the composites and are comparative to val-
ues achieved for pure Biopol sheets. Degradation studies
showed that after 150 days of compost burial more than
50% weight loss of the jute/Biopol composites occurs.
The effects of hybridization [52] on the tensile prop-
erties of jute–cotton woven fabric reinforced polyester
composites were investigated as functions of the fiber
content, orientation and roving texture. It was observed
that tensile properties along the direction of jute roving
alignment (transverse to cotton roving alignment) increase
steadily with fiber content up to 50% and then show a ten-
dency to decrease. The tensile strength of composites with
50% fiber content parallel to the jute roving is about 220%
higher than pure polyester resin.
Jute fiber reinforced PP composites were evaluated
regarding the effect of matrix modification [53], the influ-
ence of gamma radiation [54], the effect of interfacial
adhesion on creep and dynamic mechanical behavior [55],
the influence of silane coupling agent [56,57], and the effect
of natural rubber [58].
The properties of jute/plastic composites were studied,
including the thermal stability, crystallinity, modification,
trans-esterification, weathering, durability, fiber orien-
tation on frictional and wear behavior, eco-design of
automotive components, and alkylation [59–66].
Polyester resin was used as matrix for jute fiber rein-
forced composites and the relationship between water
absorption and dielectric behavior [67], the elastic prop-
erties, notched strength and fracture criteria [68], impact
damage characterization [69], weathering and thermal
behavior [70], and effect of silane treatment [71] were
examined.
2.2.4. Kenaf
Kenafbelongs to the genus Hibiscus and there are about
300 species. Kenaf is a new crop in the United States
and shows good potential as a raw material for usage
in composite products. Latest advances in decortications
equipment which separates the core from the bast fiber
combined with fiber shortages, have renewed the interest
in kenaf as a fiber source.
Thermoforming has proven to enable the successful
fabrication of kenaf fiber reinforced PP sheets into sheet
form [72]. The optimal fabrication method found for these
materials was at the compression molding process, which
utilizes a layered sifting of a micro-fine PP powder and
chopped kenaf fibers. The fiber content (30 and 40 wt%)
provided adequate reinforcement to increase the strength
of the PP matrix. The kenaf–PP composites compression
molded in this study proved to have superior tensile and
flexural strength when compared to other compression
molded natural fiber composites such as other kenaf, sisal,
and coir reinforced thermoplastics. With the aid of the
elastic modulus data, it was also possible to compare the
economic benefits of using kenaf composites instead of
other natural fibers and E-glass. The manufactured kenaf-
maleated PP composites have a higher modulus/cost and a
higher specific modulus than sisal, coir, and even E-glass.
Thus, they provide an option for replacing existing mate-
rials with a higher strength, lower cost alternative that is
environmentally friendly.
Hybrid composites of wood flour/kenaf fiber and PP
were prepared to investigate the hybrid effect on the com-
posite properties [73]. The results indicated that while
non-hybrid composites of kenaf fiber and wood flour exhib-
ited the highest and lowest modulus values respectively,
the moduli of hybrid composites were closely related to the
fiber to particle ratio of the reinforcements. With the help
of the hybrid mixtures equation it was possible to predict
the elastic modulus of the composites better than when
using the Halpin–Tsai equation.
Variations of the mechanical and thermal properties
induced by the exposure of kenaf fiber reinforced com-
posites with PP to electron beam radiation [74], the
comparison of kenaf/PP composites with feather fiber/PP,
recycled kraft pulp fiber/PP, and recycled news pulp
fiber/PP composites [75] and, surface modified kenaf
fibers with modified polyester resin as matrix [76], and
influence of toughening by natural rubber on kenaf
fibers with polyester resin as matrix [77] were also
evaluated.
2.2.5. Sisal
Sisal is an agave (Agave sisalana) and commercially pro-
duced in Brazil and East Africa. Between 1998–2000 and
2010, the global demand for sisal fiber and its products
is expected to decline by an annual rate of 2.3% as agri-
cultural twine. The traditional market for fibers continues
to be eroded by synthetic substitutes and by the adop-
tion of harvesting technologies that utilizes less or no
twine.
Magnesium hydroxide and zinc borate were incorpo-
rated into sisal/PP composites as flame retardants [78].
Adding flame retardants into sisal/PP composites reduced
the burning rate and increased the thermal stability of the
composites. No synergistic effect was observed when both
magnesium hydroxide and zinc borate were incorporated
into the sisal/PP composites. In addition, the sisal/PP com-
posites exhibited insignificant differences in shear viscosity
at high shear rates indicating that the types of flame retar-
dants used in this study had no impact on the processability
of the composites. The sisal/PP composites which flame
retardants were added to, exhibited tensile and flexural
properties comparable to those of the sisal/PP composites,
which flame retardants had not been added to.
Sisal /PP composites were investigated regarding the
environmental effects on the degradation behavior [79],
the influence of coupling agents on the abrasive wear
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
properties [80], and the effect of ageing on the mechanical
properties [81].
Zhang et al. [82] developed all plant fiber composites
by converting wood flour into thermoplastics using an
appropriate benzylation treatment and compounding both
discontinuous and continuous sisal fibers to produce com-
posites from renewable resources. The degradation tests
demonstrated that the prepared sisal/plasticized wood
flour composites were fully biodegradable. To accelerate
the decomposition process, both cellulose and lignin in the
composites should be considered. The hydrophobicity and
flame resistance of composites is important when regard-
ing practical applications. Molecular modification and/or
incorporation of inorganic additives are proper measures
provided that the composites biodegradability remains
unchanged.
Many other studies were carried out on sisal fiber
reinforced polyester composites regarding their moisture-
absorption properties [83], and fiber treatment with
admicellar [84]. Sisal fiber reinforced phenolic resin com-
posites were investigated with regard to the chemical
modification of such with lignins [85], the modification
using hydroxy terminated polybutadiene rubber [86], the
effect of cure cycles [87], using glyoxal from natural
resources [88], and the effect of alkali treatment [89].
Furthermore epoxy resin was used as a matrix for sisal
fiber reinforced composites and examined regarding the
influence of fiber orientation on the electrical properties
[90], and the degree of reinforcement [91]. Investigations
were also carried out using cement as a matrix for sisal
fiber reinforced composites focusing on their cracking
micro-mechanisms [92], and the effects of accelerated car-
bonation on cementitious roofing [93].
Towo et al. [94,95] prepared the treated sisal fiber com-
posites with an epoxy and polyester resin matrix. Fatigue
evaluation and dynamic thermal analysis tests were per-
formed. Composites containing alkali treated fiber bundles
proved to have better mechanical properties than those
with untreated fiber bundles. Alkali treatment had the
greatest effect on the polyester resin matrices. An improve-
ment in the fatigue lives of composites was observed for
the alkali treatment of sisal fiber bundles. Constant-life dia-
grams of epoxy matrix composites with untreated or alkali
treated fiber bundles show the superiority of the alkali
treated fiber composites regarding low cycle fatigue. Epoxy
matrix composites have a longer fatigue life than polyester
matrix composites. The effect of chemical treatment on
the fatigue life is significantly positive for polyester matrix
composites but has much less influence on the fatigue life
of epoxy matrix composites.
Sisal fibers were also investigated with other matrices,
such as rubber [96,97], phenol formaldehyde [98], cellu-
lose acetate [99], bio polyurethane [100], and polyethylene
[101] regarding their mechanical, morphological, chemical,
and Cure characteristics.
2.2.6. Abaca
The abaca/banana fiber, which comes from the banana
plant, is durable and resistant to seawater. Abaca, the
strongest of the commercially available cellulose fibers, is
indigenous to the Philippines and is currently produced
1557
6
5mm
5mm+MAH-PP
5
Notched charpy impact
strength [mJ/mm²]
4
3
2
1
0
Abaca-PP Flax-PP Jute-PP
Fig. 1. Comparison of notch Charpy strength of abaca/jute/flax fiber–PP
composites with and without MAH–PP.
Adopted from [103]. Copyright 2007. By permission from Budapest Uni-
versity of Technology.
there and in Ecuador. It was once the preferred cordage
fiber for marine applications.
Bledzki et al. [102,103] examined the mechanical prop-
erties of abaca fiber reinforced PP composites regarding
different fiber lengths (5, 25 and 40 mm) and different
compounding processes (mixer-injection molding, mixer-
compression molding and direct compression molding
process). It was observed that, with increasing fiber length
(5–40 mm), the tensile and flexural properties showed an
increasing tendency though not a significant one. Among
the three different compounding processes compared,
the mixer-injection molding process displayed a better
mechanical performance (tensile strength is around 90%
higher) than the other processes.
When abaca fiber PP composites were compared with
jute and flax fiber PP composites, abaca fiber composites
had the best notched Charpy (Fig. 1) and falling weight
impact properties. Abaca fiber composites also showed
higher odor concentration (Fig. 2) compared to jute and
flax fiber composites.
A dynamic mechanical analysis of, polarity parame-
ters of banana fiber reinforced polyester composites were
carried out by Thomas and co-workers [104,105] with spe-
cial reference to the effects of fiber loading, frequency
and temperature. The storage modulus was found to be
highest for composites with 40% fiber loading, indicating
Fig. 2. Comparison of odor emission concentration abaca/jute/flax
fiber–PP composites.
Adopted from [103]. Copyright 2007. By permission from Budapest Uni-
versity of Technology.
1558 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
that the incorporation of abaca fiber in the polyester
matrix induces reinforcing effects at higher temperatures.
Increased dynamic modulus values and low damping val-
ues verified improved interactions between the fiber and
the matrix.
Abaca fibers have been investigated with cement [106],
polyurethane [107], aliphatic polyester resin [108], PP
[109], urea formaldehyde [110], PE [111], polyester [112],
and polyvinyl alcohol [113] as matrices, in order to evaluate
the composites properties.
2.2.7. Pineapple leaf fiber
Pineapple (Ananas comosus) is a tropical plant native
to Brazil. Pineapple leaf fiber is rich in cellulose, rela-
tively inexpensive and abundantly available. Furthermore,
it has the potential for polymer reinforcement. At present
pineapple leaf fibers are a waste product of pineap-
ple cultivation and therefore these relatively inexpensive
pineapple fiber can be obtained for industrial purposes.
Pineapple leaf fiber was reinforced with polycarbon-
ate to produce functional composites [114]. The silane
treated modified pineapple leaf fibers composite exhibited
the highest tensile and impact strengths. The thermogravi-
metric analysis showed that the thermal stability of the
composites is lower than that of neat polycarbonate resin.
In addition, the thermal stability decreased with increasing
pineapple leaf fiber content.
The thermal conductivity and thermal diffusivity of
pineapple leaf fiber reinforced phenol formaldehyde com-
posites were studied using the Transient Plane Source
(TPS) technique [115]. It is found that the effective ther-
mal conductivity and effective thermal diffusivity of the
composites decrease, as compared with pure phenol
formaldehyde as the fraction of fiber loading increases.
The quality enhancement of pineapple leaf fiber has
been attempted using different surface modifications like
dewaxing, alkali treatment, cyanoethylation and grafting
acrylonitrile onto dewaxed fibers [116]. The mechanical
properties reach an optimum at fiber load of 30 wt% and
among all modifications, 10% acrylonitrile grafted fiber
reinforced polyester composite exhibited the maximum
tensile strength (48.36 MPa). However, cyano-ethylated
fiber composites exhibited better flexural and impact
strengths, i.e., 41% and 27% more than the detergent
washed composite respectively.
The influence of surface treatment and fiber content of
pineapple leaf fiber was also investigated with PP [117] and
natural rubber as matrix [118].
2.2.8. Ramie
Ramie belongs to the family Urticaceae (Boehmeria),
which includes about 100 species. Ramie’s popularity as a
textile fiber has been limited largely by regions of produc-
tion and a chemical composition that has required more
extensive pre-treatment than is required of the other com-
mercially important bast fibers.
Ramie fiber reinforced PP composites were fabricated
using a hybrid method of melt-blending and injection
molding processes [119]. Different ramie fiber/PP com-
posites were fabricated by varying the fiber length, fiber
content and method of fiber pre-treatment. The results
exhibited increases in fiber length and fiber content also
show increased tensile strength, flexural strength and com-
pression strength noticeably in turn. Yet, they also result in
negative influences on the impact strength and elongation
behavior of the composites.
Thermoplastic biodegradable composites consisting of
ramie fibers and a PLA/PCL matrix were manufactured
using the in situ polymerization method [120]. The effects
of fiber length and content on the tensile and impact
strengths of this natural-fiber-reinforced biodegradable
composite were discussed, including the influence of a
silane coupling agent for improved interfacial adhesion.
The results showed that the tensile strength and impact
strength were highest when a silane coupling agent was
employed, the ramie fiber length was 5–6 mm and when
the fiber content was 45 wt%.
Bulletproof panels were made from ramie fiber rein-
forced composites by hand lay-up process with epoxy as
a matrix [121]. These prototype bulletproof panels were
believed to be lighter in weight and more economical than
conventional bulletproof panels. Conventional bulletproof
panels are made from ceramic plates, kevlar/aramid com-
posites, and steel-based material, which are popular in
military standard antiballistic equipment today. The bul-
let testing results showed that the panels could resist the
penetration of a high-impact projectile (level II) obtaining
only minimal fractures. Level IV ballistic testing showed
that all prototype panels could not resist the high-impact
velocity of the projectile. Therefore, tests proved that ramie
fibers have sufficient breaking strength and toughness for
level II bullet testing.
Ramie fibers were also reinforced using polyester
[122,123], epoxy–bioresin [124], soy protein [125,126],
epoxy [127] and PP [128] for the matrix.
2.2.9. Coir
Coir husk fibers are located between the husk and
the outer shell of the coconut. As a by-product of the
production of other coconut products, coir production is
largely determined by demand. Abundant quantities of
coconut husk imply that, given the availability of labor and
other inputs, coir producers can adjust relatively rapidly to
market conditions and prices. It is estimated that approx-
imately 10% of all husks are utilized for fiber extraction,
satisfying a growing demand for fiber and coir products.
Characterization and utilization of coir fiber in coir
/natural rubber composites [129], dynamic mechanical
behavior of coir/natural rubber composites [130], durabil-
ity of coir/cement composites [131], the effect acetylation
on the coir/epoxy composites [132], the influence of
treated coir fiber on the physico-mechanical properties of
coir/PP composites [133,134], and the effect of fiber phys-
ical, chemical and surface properties on the thermal and
mechanical properties of coir/PP composites were investi-
gated and evaluated [135].
2.2.10. Bamboo
Bamboo (Bambusa Shreb.) is a perennial plant, which
grows up to 40 m in height in monsoon climates. Generally,
it is used in construction, carpentry, weaving and plaiting
etc. Curtains made of bamboo fiber can absorb ultraviolet
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
radiation in various wavelengths, making it less harmful to
human body.
The development of composites for ecological pur-
poses (eco-composites) using bamboo fibers and their basic
mechanical properties were evaluated [136]. The steam
explosion technique was applied to extract bamboo fibers
from raw bamboo trees. The experimental results showed
that the bamboo fibers (bundles) had a sufficient specific
strength, equivalent to that of conventional glass fibers.
The tensile strength and modulus of PP based composites
increased about 15 and 30% when using steam-exploded
fibers. This increase was due to good impregnation and a
reduction of the number of voids, in comparison to com-
posites using fibers that were mechanically extracted.
The mechanical and thermal properties of bamboo fiber
reinforced epoxy composites [137], the effects of fiber
loading, coupling and bonding agents on the mechani-
cal properties of bamboo fiber/natural rubber composites
[138,139], the isothermal crystallization kinetics of modi-
fied bamboo cellulose/PCL composites [140], the influence
of environmental aging on the mechanical properties of
bamboo/glass fiber reinforced PP hybrid composites [141],
and the effect of ceramic fillers on mechanical properties
of bamboo fiber/epoxy composites [142] were evaluated.
2.2.11. Rice husk
Rice is only one of the large group of cereal grains that
can be used to produce hull fibers. Nowadays wheat, corn,
rye, oats and other cereal crops are used to produce fibers
and investigating to reinforce in composites area.
Ismail et al. [143–147] studied the mechanical prop-
erties of rice husk filled polymer composites and their
relation to fiber loading, coupling agent, processability,
hygrothermal aging, and hybridization effect.
Other studies have focused on: flame retardant prop-
erties of rice husk/PE composites [148], the using of rice
husk as filler for rice husk/PP composites [149], the ther-
mogravimetric analysis of rice husk filled HDPE and PP
composites [150], the enhancement of the processabil-
ity of rice husk/HDPE composites [151], the effect of the
percentage of rice husk content, hydroxyl groups and
size on the flexural, tensile, and impact properties of rice
husk/polyurethane composites [152], nonlinear viscoelas-
tic creep characterization of HDPE-rice husk composites
[153], the effect of the rice husk size and composition on
the injection molding processability of rice husk/PE com-
posites [154], photocatalytic performance of a carbon/TiO2
composite with rice husk [155], the effect of different con-
centrations and sizes of particles of rice husk ash-in the
mechanical properties of rice husk/PP composites [156],
the effect of different coupling agent on rice husk/co-
polymer PP composites [157], dimensional properties of
rice husk/unsaturated polyester composites [158], and car-
bon/silica composites fabricated from rice husk by means
of binder-less hot-pressing [159].
2.2.12. Oil palm
Oil palms (Elaeis) comprise two species of the Arecaceae
or palm family. Nowadays, oil palm empty fruit bunch
fibers possess potential as a reinforcement fiber for plastic.
Thomas et al. [160,161] investigated the stress relaxation
1559
behavior of phenol formaldehyde resins reinforced with oil
palm empty fruit bunch fibers and hybrid composites com-
posed of oil palm fibers and glass fibers. The effects of fiber
loading, fiber treatment, physical ageing and strain level on
the stress relaxation behavior were examined and the rate
of relaxation at different time intervals was calculated in
order to explain gradual changes in relaxation mechanisms.
Abu Baker et al. [162,163] investigated the effect of oil
palm empty fruit bunch and acrylic impact modifier on
mechanical properties and influence of oil extraction of
oil palm empty fruit bunch on the processability of PVC
composites.
The effects of oil extraction, compounding techniques
and fiber loading [164], and the effect of matrix modi-
fication [165] on the mechanical properties of oil palm
empty fruit bunch filled PP composites were examined.
In addition, a comparative study of oil palm empty fruit
bunch fiber/PP composites and oil palm derived cellu-
lose/PP composites [166] were studied. The influence of
chemical modification on oil palm/phenol formaldehyde
composites [167], a comparison of epoxy and polyester
matrixes reinforced with oil palm fibers [168], dielectric
relaxation properties of oil palm/polyester resin compos-
ites [169], the effect of palm tree fiber orientation on
dynamic electrical properties of palm tree fiber-reinforced
polyester composites [170] have also been investigated.
2.2.13. Bagasse
Bagasse is the fibrous residue which remains after
sugarcane stalks are crushed to extract their juice. It is
currently used as a renewable natural fiber for the man-
ufacture of composites materials.
The compression and injection molding processes were
performed in order to evaluate which is the better mix-
ing method for fibers (sugarcane bagasse, bagasse cellulose
and benzylated bagasse) and PP matrixes [171]. The injec-
tion molding process performed under vacuum proved to
work best. Composites were obtained with a homogeneous
distribution of fibers and without blisters. Although, the
composites did not have good adhesion between the fiber
and the matrix according to their mechanical properties.
The effect of botanical components of bagasse on the
setting of bagasse/cement composites [172], design and
optimization of PHB/bagasse fiber composites [173], tribo-
logical properties of bagasse/polyester composites [174],
creep properties of bagasse fiber reinforced PVC and HDPE
composites [175], bagasse/HDPE composites for radia-
tion shielding [176], molecular mobility information of
bagasse fiber and their distribution in bagasse/EVA com-
posites [177], silane treated bagasse fiber reinforcement
for cementitious composites [178], using polyurethane
from castor oil [179], durability of bagasse/PP composites
exposed to rainbow fungus [180], and ecodesign and life
cycle assessment as strategy for automotive components
from bagasse/PP composites [181] were examined.
2.3. Structure and chemical composition
Climatic conditions, age and the degradation process
influence not only the structure of fibers, but also the chem-
ical composition. The major chemical component of a living
1560 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596

Table 2
Chemical composition of some common natural fibers.

Fiber Cellulose (wt%) Hemicellulose (wt%) Lignin (wt%) Waxes (wt%)

Bagasse 55.2 16.8 25.3 –

Bamboo 26–43 30 21–31 –
Flax 71 18.6–20.6 2.2 1.5
Kenaf 72 20.3 9 –
Jute 61–71 14–20 12–13 0.5
Hemp 68 15 10 0.8
Ramie 68.6–76.2 13–16 0.6–0.7 0.3
Abaca 56–63 20–25 7–9 3
Sisal 65 12 9.9 2
Coir 32–43 0.15–0.25 40–45 –
Oil palm 65 – 29 –
Pineapple 81 – 12.7 –
Curaua 73.6 9.9 7.5 –
Wheat straw 38–45 15–31 12–20 –
Rice husk 35–45 19–25 20 14–17
Rice straw 41–57 33 8–19 8–38

tree is water. However, on dry basis, all plant cell walls
consist mainly of sugar based polymers (cellulose, hemi-
cellulose) that are combined with lignin with lesser amount
of extractives, protein, starch and inorganics. The chemi-
cal components are distributed throughout the cell wall,
which is composed of primary and secondary wall layers.
The chemical composition varies from plant to plant, and
within different parts of the same plant. Table 2 [182–184]
shows the range of the average chemical constituents for a
wide variety of plant types.
2.4. Properties
The properties of natural fibers differ among cited
works, because different fibers were used, different
moisture conditions were present, and different testing
methods were employed. The natural fiber reinforced poly-
mer composites performance depends on several factors,
including fibers chemical composition, cell dimensions,
microfibrillar angle, defects, structure, physical properties,
and mechanical properties, and also the interaction of a
fiber with the polymer. In order to expand the use of natu-
ral fibers for composites and improved their performance,
it is essential to know the fiber characteristics.
The range of the characteristic values, as one of the
drawbacks for all natural products, is remarkably higher
than those of glass-fibers, which can be explained by
differences in the fiber structure due to the overall envi-
ronment conditions during growth. Natural fibers can be
processed in different ways to yield reinforcing elements
with different mechanical properties. Mechanical proper-
ties of natural fibers can be influenced by many factors.
Such as either fiber bundles or ultimate fiber is being
tested. Table 3 [182,183] presents the important physico-
mechanical properties of commonly used natural fibers.
The hydrophilic nature of fibers is a major problem for
all cellulose-fibers if used as reinforcement in plastics. The
moisture content of the fibers is dependent on the content
of non-crystalline parts and the void content of the fibers.
Overall, the hydrophilic nature of natural fibers influences
the mechanical properties. Table 4 [185] shows the equi-
librium moisture content of some natural fibers.
The moisture content at a given relative humidity can
have a great effect on the biological performance of a com-
posite made from natural fibers. For example, a composite
made from abaca fibers would have much greater moisture
content than would a composite made from flax fibers.
The physical properties of each natural fiber are crit-
ical, and include the fiber dimensions, defects, strength
and structure. There are several physical properties that
are important to know about for each natural fiber before
that fiber can be used to reach its highest potential. Fiber
dimensions, defects, strength, variability, crystallinity, and
structure must be taken into consideration.

Table 3
Physico-mechanical properties of natural fibers.

Fiber Tensile strength (MPa) Young’s modulus (GPa) Elongation at break (%) Density [g/cm3 ]

Abaca 400 12 3–10 1.5

Bagasse 290 17 – 1.25
Bamboo 140–230 11–17 – 0.6–1.1
Flax 345–1035 27.6 2.7–3.2 1.5
Hemp 690 70 1.6 1.48
Jute 393–773 26.5 1.5–1.8 1.3
Kenaf 930 53 1.6 –
Sisal 511–635 9.4–22 2.0–2.5 1.5
Ramie 560 24.5 2.5 1.5
Oil palm 248 3.2 25 0.7–1.55
Pineapple 400–627 1.44 14.5 0.8–1.6
Coir 175 4–6 30 1.2
Curaua 500–1150 11.8 3.7–4.3 1.4
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 3. Illustration of a single fiber cell.
Adopted from [186] Copyright 2001. By permission from Springer Publishing.
Knowledge about fiber length and width is important for
comparing different kinds of natural fibers. A high aspect
ratio (length/width) is very important in cellulose based
fiber composites as it give an indication of possible strength
properties. The fiber strength can be an important factor in
selecting a specific natural fiber for a specific application.
Changes in the physical properties can be due to differences
in fiber morphology. Major differences in structure such as
density, cell wall thickness, length and diameter result in
differences in physical properties. It is also interesting to
note that the morphology of the land plant fibers is very
from different to that of water plant fibers.
In between fiber qualities, the cellulose content and
spiral angle is differed from fiber to fiber and also in a sin-
gle fiber design. Natural fiber is a composite of the three
polymers (cellulose, hemicelluloses and lignin), in which
the unidirectional cellulose microfibrils constitute the rein-
forcing elements in the matrix blend of hemicellulose and
lignin. The structure of such a fiber was built as multi-
ply construction with layers P, S1, S2 and S3 of cellulose
microfibrils at different angles to the fiber axis (Fig. 3) [186].
Depending on the single fiber cell layer, the different
spiral angle of those layers will have a pronounced influ-
ence on the properties of the fiber. The elastic modulus
dependency on the spiral angle of the fiber is determined
Table 4
The equilibrium moisture content of different natural fibers at 65% relative
humidity (RH) and 21 ◦ C.
Fiber Equilibrium moisture content (%)
Sisal 11
Hemp 9.0
Jute 12
Flax 7
Abaca 15
Ramie 9
Pineapple 13
Coir 10
Bagasse 8.8
Bamboo 8.9
1561
(Fig. 4) assuming that the fibers (holocellulose fibers) were
lignin-free with a cellulose content of 65 wt% (which is typ-
ical cellulose content for natural fibers [186]). The relative
thickness of the different layers were chosen to be P = 8%,
S1 = 8%, S2 = 76%, and S3 = 8%. It is seen that the elastic mod-
ulus decreases with increasing spiral angle.
Crystallinity values of natural fibers vary in different
parts of the plant. The crystallinity tends to decrease as
the plant matures, but the difference between bast and
core fibers is inconclusive. The permeability of kenaf core
is highest and is closely followed by cotton.
The effect of transcrystallinity on the interface in flax
fiber (green flax, dew-retted flax, Duralin-treated flax
and stearic acid-treated flax fiber)/isotactic PP composites
has been investigated [187,188]. A significant strengthen-
ing of the interface was observed when transcrystallinity
was present. Surface modification (stearation) of flax
fiber also induced transcrystallinity. The interfacial shear
strength increased from 12.75 MPa for the samples with-
out transcrystallinity to 23.05 MPa for the transcrystallized
samples according to the single fiber fragmentation test.
Fig. 4. Correlation between spiral angle and elastic modulus of a natural
fiber.
Adopted from [186]. Copyright 2001. By permission from Springer Pub-
lishing.
1562 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
The chemical composition varies from plant to plant,
and within different parts of the same plant. It also varies
within plants from different geographical regions, ages, cli-
mate and soil conditions.
The chemical properties are influenced by the fiber
growth time (days after planting), the botanical classi-
fication of the fiber and the stalk height. The chemical
composition can also vary within the same part of a plant.
Both the root and stalk core have a higher lignin content
than that of the fibers.
2.5. Summary
There are thousands of different fibers in the world and
in fact only few of these fibers have been studied. Most
research has been carried out to study the potential use
of natural fibers for technical applications and this review
paper has only covered the most widely studied and used
natural fibers in reinforced composites materials. Among
the most popular natural fibers; flax, jute, hemp, sisal,
ramie, and kenaf fibers were extensively researched and
employed in different applications. But nowadays, abaca,
pineapple leaf, coir, oil palm, bagasse, and rice husk fibers
are gaining interest and importance in both research and
applications due to their specific properties and availabil-
ity.
It should be mentioned that there are also shortcom-
ings; a lack of consistency of fiber qualities, high levels of
variability in fiber properties related to the location and
time of harvest, processing conditions, as well as their
sensitivity to temperature, moisture and UV radiation. A
multi-step manufacturing process is required in order to
produce high quality natural fibers, which contributes to
the cost of high-performance natural fibers as well as the
improved mechanical properties of the composites.
3. Modification of natural fibers
The main disadvantages of natural fibers in reinforce-
ment to composites are the poor compatibility between
fiber and matrix and their relative high moisture absorp-
tion. Therefore, natural fiber modifications are considered
in modifying the fiber surface properties to improve their
adhesion with different matrices. An exemplary strength
and stiffness could be achieved with a strong interface
that is very brittle in nature with easy crack propagation
through the matrix and fiber. The efficiency of stress trans-
fer from the matrix to the fiber could be reduced with a
weaker interface.
3.1. Physical method
Physical methods include stretching, calendaring, ther-
motreatment, and the production of hybrid yarns for the
modification of natural fibers. Physical treatments change
structural and surface properties of the fiber and thereby
influence the mechanical bonding of polymers. Physical
treatments do not extensively change the chemical com-
position of the fibers. Therefore the interface is generally
enhanced via an increased mechanical bonding between
the fiber and the matrix.
3.1.1. Corona treatment
Corona treatment is one of the most interesting tech-
niques for surface oxidation activation. This process
changes the surface energy of the cellulose fibers. Corona
discharge treatment on cellulose fiber and hydrophobic
matrix was found to be effective for the improvement of
the compatibilization between hydrophilic fibers and a
hydrophobic matrix.
Tossa jute fibers [189] were corona discharge treated to
improve the mechanical properties of natural fiber/epoxy
composites. Corona-treated fibers exhibited significantly
higher polar components of free surface energy with
increasing treatment energy output. Owing to difficulties
in effective treatment of three-dimensional objects with
corona discharge, the increased polarity of treated yarns is
relatively small. Furthermore a decrease in the yarn tenac-
ity was observed with an increasing corona energy level.
The mechanical properties of corona treated hemp
fiber/PP composites were characterized by tensile and
compressive stress–strain measurements [190]. The treat-
ment of compounds (fibers or matrix) leads to a significant
increase in tensile strength. The modification of cel-
lulosic reinforcements rather than PP matrix allows
greater improvement of the composites properties with an
enhancement of 30% of Young modulus. The observation
of the fracture surfaces enables discussion about adhesion
improvement.
Flax and Hemp fiber mats were corona treated and
the optimum length of corona treatment to improve the
composites’ (with a natural resin matrix) tensile modulus
and strength was determined [191]. The composite ten-
sile breaking strength reaches a maximum earlier, namely
after only 5 min of corona treatment and declines rapidly
afterwards. The fiber appearance confirmed that relatively
short periods of corona treatment are more than suffi-
cient to improve adhesion in the fibers. In addition, it was
also proven that there is no further improvement achieved
when longer corona treatments are applied, because the
surface opening of the fiber does not improve further after
15 min of treatment. However, the degradation of the fibers
proceeds further.
3.1.2. Plasma treatment
Plasma treatment is another physical treatment method
and is, similar to corona treatment. The property of plasma
is exploited by the method to induce changes on the sur-
face of a material. A variety of surface modifications can
be achieved depending on the type and nature of the gases
used. Reactive free radicals and groups can be produced, the
surface energy can be increased or decreased and surface
cross-linking can be introduced.
Polyester composites reinforced with flax fibers, which
were submitted to helium cold plasma treatment, were
investigated by means of water permeation measurements
and mechanical tests [192]. The analysis of the permeation
and mechanical results showed that plasma treatment
improves the fiber/matrix adhesion and enhances the
mechanical property stiffness.
Martin et al. [193] prepared sisal–HDPE composites
and showed that some improvements of the mechanical
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
properties of the composites are achieved due to the
plasma treatments.
Jute fibers were subjected to oxygen plasma treatment
as a function of the plasma power in order to enhance inter-
facial adhesion [194]. The interlaminar shear strength of
plasma treated jute fiber/HDPE composites, which were
exposed to plasma powers of 30 W and 60 W, increased
by approximately 32 and 47%, respectively compared to
untreated composites. In turn, the flexural strength of
untreated composites increases by only 45%. It can be con-
cluded that exposure to plasma powers of 60 W for 15 min
in the studied range is the most suitable parameter for
oxygen plasma treatment of jute fibers and enables the
achievement of the best interfacial adhesion with HDPE.
The influence of plasma treatment on the morphology,
wettability, and fine structure of jute fibers and its impact
on the interfacial adhesion of jute fibers/unsaturated
polyester were investigated [195]. A scanning electron
microscopic micrograph showed the rough surface mor-
phology and degradation of fiber due to an etching
mechanism caused by the plasma. Plasma treatment
resulted in the development of hydrophobicity in fibers.
However, among all treated fiber composites, the flexu-
ral strength of composites prepared with fibers treated for
10 min with plasma only showed an improved mechanical
strength of approximately 14% in comparison to raw fiber
composites.
Jute fibers were treated indifferent plasma reactors
(radio frequency “RF” and low frequency “LF” plasma reac-
tors) using O2 for different plasmapowers to increase the
interface adhesion between the jute fiber and polyester
matrix. The interlaminar shear strength increased from
11.5 MPa for the untreated jute fiber/polyester composite
to 19.8 and 26.3 MPa for LF and RF oxygen plasma treated
jute fiber/polyester composites, respectively. The tensile
and flexural strengths improved of jute fiber/polyester
composites for both plasma systems. It is clear that oxy-
gen plasma treatment of jute fibers by using RF plasma
system showed greater improvement on the mechanical
properties of jute/polyester composites compared to using
LF plasma system [196].
3.2. Chemical method
Cellulose fibers, which are strongly polarized, are inher-
ently incompatible with hydrophobic polymers due to their
hydrophilic nature. In many cases, it is possible to induce
compatibility in two incompatible materials by introducing
a third material that has properties intermediate between
those of the other two. There are several coupling mecha-
nisms in materials (e.g., weak boundary layers, deformable
layers, restrained layers, wettability, chemical bonding,
and acid–base effect).
The development of a definite theory for the mecha-
nism of bonding using coupling agents in composites is a
complex problem. The main chemical bonding theory alone
is not sufficient. So the consideration of other concepts
appears to be necessary. These include the morphology
of the interphase, the acid–base reactions in the interface,
surface energy and the wetting phenomena.
1563
Chemical modifications of natural fibers aimed at
improving the adhesion within the polymer matrix using
different chemicals were investigated.
3.2.1. Silane treatment
The surface energy of fibers is closely related to the
hydrophilic nature of the fiber. Some investigations are
concerned with methods to decrease hydrophilicity. Silane
coupling agents may contribute hydrophilic properties to
the interface, especially when amino-functional silanes,
such as epoxies and urethanes silanes, are used as primers
for reactive polymers. The primer may supply much more
amine functionality than can possibly react with the resin
in the interphase. Those amines, which could not react, are
hydrophilic and therefore responsible for the poor water
resistance of bonds. An effective way to use hydrophilic
silanes is to blend them with hydrophobic silanes such as
pheniltrimethoxysilane. Mixed siloxane primers also have
an improved thermal stability, which is typical for aromatic
silicones.
The surface of the kenaf fiber was modified using a silane
coupling agent to promote adhesion with the PS matrix
[197]. The fiber–matrix adhesion increased through a con-
densation reaction between alkoxysilane and hydroxyl
groups of kenaf cellulose. Due to the fiber modification,
kenaf/PS composites exhibited higher storage modulus and
lower tan ı than those with untreated fiber indicating a
greater interfacial interaction between the matrix resin and
the fiber.
Silane treatment improved the storage modulus of
abaca fiber reinforced polyester composites [198]. Chemi-
cal modifications with silane A174 (␥-methacryl oxypropyl
trimethoxy-silane) and also with NaOH resulted in max-
imum increase of the modulus. The hydrogen-bond
donating acidity is found to be the lowest for fibers treated
with silane A174, after pre-treatment with 0.5% NaOH. On
the contrary, the highest value was noted for fibers treated
with silane A151 (vinyl triethoxysilane). The overall polar-
ity was found to be at a maximum for fibers treated with
silane A151 (vinyl triethoxysilane).
The effects of different chemical treatments on the
fiber–matrix compatibility in terms of the surface energy
and the mechanical properties of composites were
reported [199]. The composites were compounded with
two kinds of flax fibers (natural flax and flax pulp)
and a PP matrix. The applied treatments were vinyl
trimethoxy silane (VTMO), maleic anhydride (MA) and
maleic anhydride-polypropylene copolymer (MAPP). The
three treatments reduced the polar component of the
surface energy of the fiber. Composites containing MAPP-
treated fibers possessed the highest mechanical properties,
while the MA and VTMO-treated fibers obtained similar
values to those of the untreated ones.
Ismail et al. [200,201] treated oil palm empty fruit bunch
and coir fibers with silane coupling agents and found that
with the addition of silane, the scorch time and cure time
increased. Furthermore, the tensile strength, tensile mod-
ulus, tear strength, fatigue life and hardness of oil palm
empty fruit bunch and coir fiber reinforced polyester and
natural rubber composites were enhanced.
1564 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596

Table 5
Variation of the structure and properties of hemp Yarn (hemp 10/1, Rohemp) due to mercerization (22% NaOH).

Mercerization Mercerization Stress at the Degree of conversion Tensile strength Elongation at Tension modulus
temperature time (◦ C) (min) mercerization cell I in cell II (%) (cN/tex) break (%) (cN/tex)

Untreated – 29.8 3.15 1148

4 60 Isometric ≈50 28.5 2.34 1617
10 60 Isometric ≈50 24.9 2.45 1214
20 60 Isometric ≈50 28.2 2.27 1701
10 40 Free shrinkage ≈70 17.6 6.86 357
10 60 Constant load (100 g) ≈40 29.2 2.60 1499

Note: Distance of clamped support = 500 mm, test speed = 250 mm/min.

3.2.2. Alkaline treatment
Alkaline treatment or mercerization is one of the most
used chemical method (removes a certain amount of lignin,
wax and oils covering the external surface of the fiber cell
wall) for natural fibers when used to reinforce thermoplas-
tics and thermosets. The important modification achieved
with alkaline treatment is the disruption of the hydrogen
bonding in the network structure, thereby increasing the
surface roughness.
The effect of alkali treatment on the wetting ability and
coherence of sisal–epoxy composites has been examined
[202]. Treatment of sisal fiber in a 0.5 N solution of sodium
hydroxide resulted in more rigid composites with lower
porosity and higher density. The treatment improved the
adhesion characteristics, due to improved work of adhesion
because it increases the surface tension and surface rough-
ness. The resulting composites showed improvements in
the compressive strength and water resistance. It was also
discovered that the removal of intracrystalline and inter-
crystalline lignin and other waxy surface substances by the
alkali substantially increases the possibility for mechanical
interlocking and chemical bonding.
The effects of alkali treatment of pineapple leaf fiber on
the performance of the pineapple leaf fiber/PLA composites
have been shown [203]. It was found that alkali-treated
fiber reinforced composite offered superior mechanical
properties compared to untreated fiber reinforced com-
posites. This study also suggested that the appropriate
modification of fiber surfaces significantly contributes to
improving the interfacial properties of the biocomposites.
Since improvement of the interfacial adhesion increases
the impact performance, surface properties of fibers can be
greatly modified in terms of different treatments as char-
acterized by an increased surface energy, which improves
wettability of the fiber when compounding with a PLA
matrix. DMA showed that treated fiber composites have a
higher storage modulus, which indicates greater interfacial
bond strength and adhesion between the matrix resin and
the fiber. The alkalized fiber composites have high storage
modulus values, which correspond with their high flexural
modulus.
The effect of alkylation on the tensile properties of
ramie fiber was explored [204]. The load application tech-
nique was employed during alkali treatment, in order to
improve the mechanical properties of the fiber. The ramie
fiber was alkali-treated with a solution containing 15%
NaOH and was subjected to applied loads of 0.049 and
0.098 N. The results showed that the tensile strength of the
treated ramie fiber was by improved 4–18% more than for
untreated ramie fibers. The treated fibers’ Young’s modu-
lus decreased. It should be noted that fracture strains of the
treated ramie fiber drastically increased to 0.045–0.072.
That equals twice to three times higher than those of the
untreated ramie fiber. It was considered that such prop-
erty improvements upon alkylation were correlated with
a change of the morphological and chemical structures in
microfibrils of the fiber.
Jute fibers were subjected to alkali treatment with a
solution containing 5% NaOH for 0, 2, 4, 6 and 8 h at 30 ◦ C
[205]. The modulus of the jute fibers improved by 12%, 68%
and 79% after 4, 6 and 8 h of treatment, respectively. The
tenacity of the fibers improved by 46% after 6 and 8 h treat-
ment and the percentage of breaking strain was reduced
by 23% after 8 h treatment. For 35% of the composites with
fiber treated for 4 h, the flexural strength improved by 20%
from 199.1 to 238.9 MPa. The flexural modulus improved
by 23% from 11.89 to 14.69 GPa and the laminar shear
strength increased by 19% from 0.238 to 0.283 MPa.
Ramie fiber [206], green coconut fiber [207], sisal [208],
jute [209] and coir [210] fibers were alkalized and their
properties evaluated.
The variation of mechanical and structural properties
of hemp yarn upon alkylation in dissimilar conditions was
investigated [211]. Alkylation with a rather high alkali con-
centration (22%) never led to a complete lattice conversion
of cellulose I in cellulose II (Table 5). As expected, the high-
est degree of conversion (70%) was reached by a freely
shrinking yarn. Further, the alkylation of hemp yarn under
isometric conditions or with constant fiber load (100 p) at
a NaOH concentration of 22% results in a crystalline lat-
tice conversion of only 40–50%. However, this occurs only
when combined with the highest strengths and moduli of
the fiber bundles. It was also observed that only the ten-
sile modulus of elasticity exceeds the value of the original
unmodified material.
Table 6
Influence of different fiber treatments on flexural strength of unidirec-
tional flax–PP composites.
Fiber treatment Flexural strength (N/mm2 )
Untreated 77
Mercerizeda 115
MAH–PPb 127
Mercerized + MAH–PP 149
Note: Lengthwise, fiber content: 36 vol%.
a
29% NaOH at 20 ◦ C, 20 min, isometric.
b
1% Licomont AR 504 in toluene, 10 min.
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 5. Influence of acetylation of flax fiber on the degree of polymeriza-
tion and degree of crystallinity of cellulose.
Adopted from [212]. Copyright 2008. By permission from Budapest Uni-
versity of Technology.
Table 6 [211] explicitly shows that, besides the signif-
icant effects of single alkylation and MAH–PP treatments,
a combination of the isometric alkylation procedure (e.g.,
increasing fiber strength) and coupling agents results in
the highest increase of the composite properties (90%) in
comparison to a composite with untreated flax fibers for
reinforcement.
3.2.3. Acetylation
Acetylation is another method of modifying the surface
of natural fibers and making them more hydrophobic. It
describes the introduction of an acetyl functional group
into an organic compound. The main idea of acetylation
is to coat the OH groups of fibers which are responsible
for their hydrophilic character with molecules that have a
more hydrophobic nature.
The influence of acetylation on the structure and prop-
erties of flax fibers were investigated. Modified flax fiber
reinforced PP composites were also prepared [212]. The
effect of acetylation on the degree of polymerization and
crystallinity of flax fiber is illustrated in Fig. 5.
It was observed that the degree of polymerization
slowly decreased while the degree of acetylation increased
until 18%. Once reaching an acetyl content of 18% acetyl
content, the degree of polymerization decreased rapidly
due to vigorous degradation of cellulose. It was also notable
that the degree of crystallinity increased a little bit regard-
ing the degree of acetylation, because of the removal of
lignin and extractibles. After that, the degree of crystallinity
of the cellulose decreased with respect to the degree
of acetylation owing to the decomposition of acetylated
amorphous components on the cellulose surface.
The influences of the degree of acetylation of flax fibers
on the moisture absorption properties are illustrated in
Fig. 6 [212]. At 95% RH, the 3.6%, 12%, 18% and 34% degree
of acetylated flax fibers showed about 14%, 18%, 27% and
42% lower moisture absorption properties than untreated
flax fiber respectively. The moisture absorption properties
decreased proportionally with the increase of acetyl con-
tent of fibers due to the reduction of hydrophilicity of the
fibers.
Seena et al. investigated the effect of acetylation on
abaca fiber reinforced phenol formaldehyde composites
and reported that the tensile strength, tensile modulus and
1565
Fig. 6. Influence of acetylation of flax fibers on the moisture absorption
property at 95% relative humidity.
Adopted from [212]. Copyright 2008. By permission from Budapest Uni-
versity of Technology.
impact strength were found to improve compared to non-
treated abaca fiber composites [213].
Tserki and co-workers [214] investigated the acety-
lation of flax, hemp and wood fibers. A removal of the
non-crystalline constituents of the fibers, an alteration of
the characteristics of the surface topography, a change of
the fiber surface free energy and an improvement of the
stress transfer efficiency in the interface took place.
The effects of acetylation on the biological degradation
and shear strength of coir and oil palm fiber reinforced
polyester composites were evaluated [215,216]. It was
reported that acetylated natural fiber reinforced polyester
composites exhibit higher bio-resistance and less tensile
strength loss compared to composites with silane treated
fiber in biological tests.
Zafeiropoulos and co-workers extensively investigated
the influence of acetylation on the engineering and char-
acterization of the interface in flax fiber/PP composites
[217,218]. Furthermore, they also investigated the applica-
tion of Weibull statistics [219] and Gaussian statistics [220]
to the tensile strength of flax fibers.
3.2.4. Maleated coupling
Nowadays, maleated coupling is widely used to
strengthen natural fiber reinforced composites. The funda-
mental difference with other chemical treatments is that
maleic anhydride is not only used to modify fiber surface
but also the polymeric matrix to achieve better interfa-
cial bonding in between fiber and matrix and improved
mechanical properties in composites. There are numerous
published studies in which the effect of maleic anhydride
grafting on the mechanical properties of natural fibers has
been investigated and it is impossible to list all of them
here. Hence, only a few representative studies are dis-
cussed here.
Mohanty et al. [221] used MAPP as a coupling agent
for the surface modification of jute fibers. It was found
that a fiber loading of 30% with a MAPP concentration
of 0.5% in toluene and 5 min of impregnation time with
6 mm average fiber lengths resulted in the best possible
outcomes. An increase in flexural strength of 72.3% was
observed for the treated composites. In addition to the
PP matrix, Mishra et al. [222] reported that maleic anhy-
dride treatment reduced the water absorption to a great
extent in abaca, hemp and sisal fiber-reinforced novolac
composites. Mechanical properties like Young’s modulus,
1566 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 7. Micrograph of abaca fiber surface morphology (a) unmodified (b) NDS modified (c) fungamix modified.
Adopted from [233]. Copyright 2010. By permission from Elsevier Ltd.
flexural modulus, hardness and impact strength of plant
fiber-reinforced composites increased after maleic anhy-
dride treatment.
The effects of MAH–PP coupling agents on rice-husk
flour reinforced PP composites were evaluated [223]. The
tensile strengths of the composites decreased as the filler
loading increased, but the tensile properties were signifi-
cantly improved with the addition of the coupling agent.
Both the notched and unnotched Izod impact strengths
remained almost the same with the addition of coupling
agents. A morphological study revealed the positive effect
of a compatibilizing agent on interfacial bonding.
Abaca fiber reinforced composites based on
HDPE/Nylon-6 blends were prepared [224]. Maleic
anhydride grafted styrene/ethylene–butylene/styrene tri-
block polymers (SEBS-g-MA) and maleic anhydride grafted
polyethylene (PE-g-MA) were used to enhance the impact
performance and interfacial bonding between the abaca
fibers and the resins. By employing SEBS-g-MA, better
strengths and moduli were obtained for HDPE/Nylon-6
based composites than for corresponding HDPE based
composites. It was found that the addition of SEBS-g-MA
had a positive influence on the reinforcing effect of the
Nylon-6 component in the composites. Thermal analysis
results showed that fractionated crystallization of the
Nylon-6 component in the composites was induced by the
addition of both SEBS-g-MA and PE-g-MA. The thermal
stability of both composite systems differed slightly,
except for an additional decomposition peak, which is
related to the minor Nylon-6 for the composites from the
HDPE/Nylon-6 blends. In combination with SEBS-g-MA,
the addition of Nylon-6 and the increased fiber loading
level led to an increase in the water absorption value of
the composites.
The influence of MAH–PP on the fiber–matrix adhesion
in jute fiber-reinforced PP composites and on the material
behavior under fatigue and impact loadings was inves-
tigated [225]. The fiber–matrix adhesion was improved
by treating the fibers’ surface with the coupling agent
MAH–PP. It was shown that a strong interface is connected
with a higher dynamic modulus and reduction in stiffness
degradation with increasing load cycles and applied max-
imum stresses. The specific damping capacity resulted in
higher values for the composites with poor bonded fibers.
Furthermore, the stronger fiber–matrix adhesion reduced
the loss-energy for non-penetration impact tested com-
posites about roughly 30%. Tests, which were performed
at different temperatures, showed higher loss energies for
cold and warm test conditions compared to those car-
ried out at room temperature. The post-impact dynamic
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 8. Tensile and flexural strength of enzyme treated and unmodified
abaca–PP composites.
Adopted from [233]. Copyright 2010. By permission from Elsevier Ltd.
modulus roughly 40% after 5 impact events and was 30%
lower for composites with poor and good fiber–matrix
adhesion, respectively.
The effectiveness of MAH as coupling agent has dis-
cussed also on thermal and crystallization properties of
sisal fiber/PP composites [226], tensile properties of hilde-
gardia fiber/PP composites [227], wetting behavior of flax
fiber/PP composites [228], transcrystallinity of jute fiber/PP
composites [229], surface properties and water uptake
behavior of flax, hemp fiber reinforced PP composites [230],
effects of micro-sized cellulose based corn fibers as rein-
forcement agents in PP composites [231], and dynamic
mechanical properties of flax and hemp fiber/PP compos-
ites [232].
3.2.5. Enzyme treatment
The use of enzyme technology is becoming increasingly
substantial for the processing of natural fibers. Currently,
the use of enzymes in the field of textile and natural fiber
modification is also rapidly increasing. A major reason for
embracing this technology is the fact that the application
of enzymes is environmentally friendly. The reactions cat-
alyzed are very specific and have a focused performance
[233].
Bledzki et al. [233] investigated PP composites with
enzyme treated abaca fibers. The surface morphologies of
enzyme treated and untreated abaca fibers are shown in
Fig. 7. In Fig. 7a, it was observed that the untreated fiber
surface is rough, containing waxy and protruding parts.
The surface morphology of treated fibers is observed in
Fig. 7b and c. If the waxy material and cuticle in the treated
surface are removed, the surface becomes smoother. Fib-
rillation is also known to occur when the binding materials
are removed from the surface of the treated fibers. Fiber
surface damage was also observed for naturally digested
fibers which occur in natural digestion systems.
The effects of enzyme treatment of abaca fiber on the
tensile and flexural strength are shown in Fig. 8. The tensile
strength of enzyme treated abaca composites was found to
have increased 5–45% due to modification. Natural diges-
tion system (NDS) modified abaca fiber composites showed
little improvement in comparison to unmodified abaca
fiber composites. The tensile strength of fungamix modified
composites increased by 45% as compared to unmodified
fiber composites. A conventional coupling agent (MA–PP)
has a positive effect on the tensile strength. It was found
1567
to improve by 40%. Enzymatic treatment was also investi-
gated with hemp fiber [234,235], and flax fibers [236].
3.3. Summary
Though natural fiber reinforced composites have devel-
oped significantly over the past few years because of their
low cost, low relative density, and high specific strength,
the interfacial adhesion between fiber and matrix is still an
issue. Extensive research was carried out and reported in
literature and reviewed in this paper, showing the impor-
tance of the interface and the influence of various types of
surface modifications on the physical and mechanical prop-
erties of biocomposites. The observed trend lied with the
chemical modification compared to physical modification.
It has also been shown that maleated and silane treat-
ment is becoming a choice method due to beneficial results.
Additive suppliers improved the additives with higher
amounts of anhydride functional groups than previous
grades (used in 1980s and 1990s), which create more sites
for chemical links, resulting in significant performance
improvement at low additive contents. Using coupling
agents reduced the water absorption of the composites
but has not resulted in decreased long term performance.
As described above that enzyme technology to modify the
natural fiber surface, is increasing substantially due to envi-
ronment friendly. In addition, enzyme technology could
be cost effective, improved product quality compared to
mostly use maleated and silane modification.
4. Matrices for biocomposites
The composites’ shape, surface appearance, environ-
mental tolerance and overall durability are dominated
by the matrix while the fibrous reinforcement carries
most of the structural loads, thus providing macroscopic
stiffness and strength. The polymer market is dominated
by commodity plastics with 80% consuming materials
based on non-renewable petroleum resources. Govern-
ments, companies and scientists are driven to find an
alternative matrix to the conventional petroleum based
matrix through public awareness of the environment, cli-
mate change and limited fossil fuel resources. Therefore
biobased plastics, which consist of renewable resources,
have experienced a renaissance in the past few decades.
Fig. 9 shows that the matrices currently used in bio fiber
composites depend on biobased or petroleum based plas-
tics and also on their biodegradability.
4.1. Petrochemical based
The effects of the incorporation of natural fibers
in petrochemical based thermoplastics and thermoset
matrixes were extensively studied. Polypropylene (PP),
polyethylene (PE), polystyrene (PS), and PVC (polyvinyl
chloride) were used for the thermoplastic matrixes.
Polyester, epoxy resin, phenol formaldehyde, and vinyl
esters were used for the thermoset matrices and are
reportedly the most widely used matrices for natural fiber
reinforced polymer composites.
1568 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 9. Current and emerging plastics and their biodegradability.
Adopted from [1].
4.1.1. Thermoplastic
4.1.1.1. PE (polyethylene). Several mechanical properties
(deformation, fracture, thermal diffusivity, thermal con-
ductivity, and specific heat) of flax fiber/HDPE biocom-
posites were evaluated [237,238]. Strength and stiffness
improvement combined with high toughness can be
achieved by varying the fiber volume fraction and con-
trolling the bonding between layers of the composite.
The thermal conductivity, thermal diffusivity, and spe-
cific heat of the flax/HDPE composites decreased with
increasing fiber content, but the thermal conductivity
and thermal diffusivity did not change significantly at
temperatures in the range (170–200 ◦ C) studied. The spe-
cific heat of the biocomposites increased gradually with
temperature.
Traditionally the mechanism of moisture absorption is
defined by diffusion theory; but the relationship between
the microscopic structure-infinite 3D-network and the
moisture absorption could not be explained. Wang et al.
[239] introduced the percolation theory and a percolation
model was developed to estimate the critical accessible
fiber ratio; the moisture absorption and electrical conduc-
tion behavior of composites. At high fiber loading when
fibers are highly connected, the diffusion process is the
dominant mechanism; while at low fiber loading close to
and below the percolation threshold, the formation of a
continuous network is key. Hence, percolation is the dom-
inant mechanism. The model can be used to estimate the
threshold value which can in turn be used to explain mois-
ture absorption and electrical conduction behavior. Fig. 10
shows the increment of electrical conductivity with the
increasing moisture content of the composite with 65% rice
hull fiber loading. The composite started showing conduc-
tivity after it absorbed approximately 50% of maximum
moisture. After this, conductivity increased quickly with
further moisture absorption. The pattern of the increment
of electrical conductivity suggests a diffusion process of
moisture absorption.
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 10. The moisture absorption and electrical conductivity for
HDPE–rice hull composite with 65% fiber content.
Adopted from [239]. Copyright 2006. By permission from Elsevier Ltd.
The hygrothermal weathering properties of rice hull
reinforced HDPE composites were studied by Wang et al.
[240]. The samples (50% rice hull and 50% HDPE) absorbed
4.5% moisture after 2000 h of exposure to a relative humid-
ity (RH) of 93% at 40 ◦ C. The walls of the samples swelled
significantly (7.1%) in thickness and ultimately developed
about 5 mm of longitudinal bowing (Fig. 11) based on 61 cm
long boards. Both expansion and bowing were partially
recovered after another 2000 h exposure to 20% RH at 40 ◦ C.
Deformation results in increased moisture contents.
Temperature also played a significant role by causing direct
thermal expansion or contraction and by affecting the rate
and the amount of moisture adsorption.
Sisal fiber reinforced PE [241] and HDPE [242,243]
composites were examined regarding their interfa-
cial properties, isothermal crystallization behavior and
mechanical properties. Sisal fiber treatment with stearic
acid increased the interfacial shear strength by 23%
compared to untreated fibers in sisal/PE composites. Per-
manganate (KMnO4 ) and dicumyl peroxide (DCP) roughen
the fiber surface and introduced mechanical interlocking
with the HDPE. Sisal fiber reinforced HDPE shows a stable
de-bonding process with Permanganate and DCP treat-
ment. Silane treated sisal fiber reinforced HDPE exhibits an
unstable debonding process. A high crystallization rate and
short crystallization half time were observed for sisal/HDPE
composites compared to neat HDPE. This demonstrates the
strong nucleating abilities of sisal fibers. With increasing
Fig. 11. Partial recovery of bowing (a) before recovery: 5.00 mm of bowing (b) after recovery: 3.00 mm of bowing.
Adopted from [240]. Copyright 2005. By permission from Elsevier Ltd.
1569
fiber content, the crystallization activation energy of the
composites decreased.
Similar investigations (PE as matrix) were carried
out using soya powder [244], curaua [245], rape straw
[246,247], hemp [248], rice straw [249], bagasse [250] rice
hull fibers [251] and LDPE as matrixes with wheat straw
[252], abaca, bagasse and rice straw fibers [253].
4.1.1.2. PP (polypropylene). The thermo-mechanical
behavior of hemp fibers was studied with focus on man-
ufacturing high performance natural fiber reinforced PP
composites. Hemp fibers subjected to quasi-static tensile
experiments and temperature-controlled harmonic tests
revealed a complex behavior, involving several mecha-
nisms [254]. The hemp fiber behavior was affected by
temperature and acted not only as an activation factor, but
also as a degradation factor with respect to the visco-elastic
properties of the fibers. It was discovered that PP–hemp
fiber composites with relatively high performance can be
achieved with some specific mechanical properties.
The effect of sisal fiber degradation and aging on the
PP/sisal fiber composites was investigated. The fiber mat
production method allowed the fibers to avoid much of the
processing degradation, which is often encountered dur-
ing conventional shear mixing processes [255]. The best
possible mechanical properties for the sisal fiber/PP com-
posites were achieved when the fiber length was greater
than 10 mm and the fiber mass fraction was in the range of
15–35%. The aged sisal fiber showed lower tenacity, break-
ing strength and elongation with in comparison to fresh
sisal fibers. On the contrary, in sisal/PP composites, aged
sisal fiber composites exhibited better mechanical proper-
ties than fresh sisal fiber/PP composites [256].
Rana et al. [257] observed an increase in impact strength
in jute fiber/PP composites as a result of fiber loading. It
was also found that both the impact and tensile properties
showed increasing trends with the addition of compati-
bilizers. However, the opposite was true for the flexural
properties. Improvements of physico-mechanical proper-
ties achieved by post-treatment [258], and the interfacial
and durability evaluation [259,260] of jute fiber/PP com-
posites were studied.
The environmental performance of hemp fiber rein-
forced PP composites based on natural fiber mat thermo-
plastic (NMT) was evaluated by quantifying carbon storage
potential and CO2 emissions. The results were compared
with commercially available glass fiber composites [261].
1570 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 12. CO2 emissions per ton composite and reduction in emissions by
substituting glass fiber with hemp fibers.
Adopted from [261]. Copyright 2003. By permission from Elsevier Ltd.
Fig. 12 shows CO2 emissions in ton/ton of composite for
both natural and glass fibers. These values are estimated
by converting energy into CO2 emissions using standard
conversion factors for different fossil fuels. The heat energy
liberated by incineration of hemp fiber and PP is also added
in non-renewable energy requirements to make calcula-
tions simpler. The results demonstrate a net reduction in
emissions of 3 ton CO2 /ton of product if glass fibers are sub-
stituted by hemp fibers.
The potential of wheat straw fibers to be used as rein-
forcing additives for PP prepared with the influence of
different processes (mechanical and chemical processes)
was investigated [262]. Fibers prepared by mechanical
and chemical processes were characterized with respect
to their chemical composition, morphology, physical,
mechanical and thermal properties. The fibers prepared by
chemical processes exhibited better mechanical, physical
and thermal properties.
The morphology of the wheat straw fiber surfaces pro-
cessed by mechanical and chemical means is shown in
Fig. 13. Surface of wheat straw fibers by different methods (a) mechanical processing and (b) chemical processing.
Adopted from [262]. Copyright 2006. By permission from Elsevier Ltd.
Fig. 14. TGA curves of wheat straw fibers prepared by different processes.
Adopted from [262]. Copyright 2006. By permission from Elsevier Ltd.
the SEM photomicrographs (Fig. 13). The surface of the
chemically processed fibers was more uniform and homo-
geneous while the fibers processed mechanically exhibit
more surface irregularities. Mechanically processed fibers
still contained the cellular residues such as lignin and hemi-
cellulose, which cement the fibers together.
The influence of chemical and mechanical processes on
the TGA of the wheat straw fibers is shown in Fig. 14.
The onset of degradation of wheat straw fibers prepared
by mechanical and chemical processes were 217 ◦ C and
242 ◦ C respectively indicating the suitability of these fibers
for processing with thermoplastics, especially polyolefins.
The higher onset of degradation temperature indicates the
improved thermal stability of the fibers prepared by chem-
ical processing.
Similar to PE, PP is also widely used as a matrix in
combination with different natural fibers: such as hemp
[263,264], flax [265–267], kenaf [268,269], oil palm [270],
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
date palm [271], coir [272,273], bamboo [274,275], abaca
[276,277], rice hull [278–280], jute [281,282], and wheat
straw [283].
4.1.1.3. PS (polystyrene) and PVC (polyvinyl chloride). Only
limited studies were reported regarding the usage of PS
and PVC as matrixes for natural fibers. The thermal and
dynamic mechanical behavior [284], as well as the rheolog-
ical [285] and mechanical properties [286] of PS composites
reinforced with sisal fibers were studied. The PS compos-
ites reinforced with agave fiber were also studied regarding
their fiber surface modification [287]. The impact proper-
ties of PVC composites reinforced with bamboo fibers [288],
the interfacial modification of bagasse fiber [289] and the
thermal degradation of abaca fiber [290] reinforced PVC
composites were also evaluated.
4.1.2. Thermosets
4.1.2.1. Polyester. The possibility of using date palm fibers
as reinforcement in polyester composites was investigated
[291]. Flexural properties and impact strength of date palm
fiber/polyester composites were found to be influenced by
fiber content and fiber treatment method. Soda treated
fibers exhibited higher mechanical properties compared
to untreated fiber/polyester composites. The fiber frac-
tion and fiber length for this system were optimized for
9 wt% and 2 cm, respectively. Water absorption was lightly
affected by surface modification of the fibers and was rel-
atively low.
The hybrid effect on the mechanical properties of abaca
and sisal fiber reinforced polyester composites was eval-
uated [292]. A positive hybrid effect was observed for
the flexural properties. The tensile strength was found
to be increased when the volume fraction of banana was
increased. A negative effect was observed for the impact
properties. Recent works regarding sisal and jute fiber
[293], sisal [294], abaca [295], abaca and sisal [296], flax
[297], jute fibers [298], sisal, abaca and bamboo fiber [299]
reinforced polyester composites have been developed.
4.1.2.2. Epoxy. The excellent properties of epoxy (good
adhesion, mechanical properties, low moisture content,
little shrinkage, and processing ease) make it one of the
best matrix materials for composites. The effect of fiber
treatment on the mechanical properties of unidirectional
sisal/epoxy composites was reported [300]. Ganan et al.
[301] evaluated the mechanical and thermal properties
of sisal/epoxy composites as a function of fiber modifica-
tion. Kenaf [302], hemp and flax [303], oil palm [304], sisal
[305,306], flax [307], sisal and hemp [308], flax, hemp and
kenaf [309], lantana camara fiber [310] and sugar palm fiber
[311] were reinforced with an epoxy matrix. Their mechan-
ical properties, processing methods, water absorption, and
fracture toughness were evaluated.
4.1.2.3. Phenolic. Phenolic resins show superior fire resis-
tance to other thermosetting resins. Sreekala et al.
[312–316] extensively investigated oil palm fiber rein-
forcement in phenolic resins. The fiber surface modifi-
cation [312], a comparison of mechanical properties to
glass fiber/phenolic resin composites [313], the dynamic
1571
mechanical properties regarding the fiber content and
hybrid fiber ratio [314], the water absorption [315] and
stress–relaxation behavior [316] of oil palm/phenolic resin
composites were evaluated. Bamboo [317], jute [318,319],
date palm fiber [320], and grewia optiva fiber [321] were
also investigated with phenol formaldehyde resin as a
matrix.
4.2. Bio-based
Public concern about the environment, climate change
and limited fossil fuel resources are important driving
forces, which motivate researchers to find alternatives to
crude oil. Bio-based plastics may offer important contri-
butions by reducing the dependence on fossil fuels and, in
turn the related environmental impacts. Biopolymers have
experienced a renaissance in the recent years. Many new
polymers were developed from renewable resources, such
as starch, which is a naturally occurring polymer that was
re-discovered as a plastic material. Others are poly lactic
acid (PLA) that can be produced via lactic acid from fer-
mentable sugar and polyhydroxyalkanoate (PHAs), which
can be produced from vegetable oils next to other bio-based
feed stocks.
4.2.1. PLA (polylactide acid)
Kenaf fiber reinforced PLA composites were studied
extensively. Investigations have been undertaken con-
cerning chemical modifications such as alkylation [322]
and silane treatments [323], the biodegradability [324]
and the mechanical and dynamic mechanical proper-
ties [325]. The alkali treated fiber reinforced composites,
followed by silane-treated fiber reinforced composite pos-
sessed significantly improved mechanical properties. The
heat deflection temperature (HDT) of the kenaf rein-
forced PLA composites was significantly higher than that
of neat PLA resin. The biodegradability of kenaf/PLA com-
posites corresponds to the weight of the composites,
which decreased approximately 38% after four weeks of
decomposition. Young’s modulus (6.3 GPa) and the ten-
sile strength (62 MPa) of the kenaf/PLA composites (fiber
content = 70 vol%) were comparable to those of traditional
composites. In addition, the storage modulus of the com-
posite remained unchanged until the melting point of PLA
was reached.
The interfacial characterization of flax fiber/PLA com-
posites was performed on a micro-scale using the
microbond testing method [326]. The interfacial mecha-
nisms of flax/PLA biocomposite were exposed to varying
thermal treatments (i.e., different cooling rates and anneal-
ing to release thermal stress). The treatments resulted in
different micro-structures and residual stress states inside
the material. Cooling kinetics is shown to modify the inter-
facial properties and when the cooling rate is slow, the
interfacial properties improve. In addition, a high degree
of crystallinity was measured, including transcrystallinity
around the flax fiber. The higher crystalline morphology of
the PLA results in an improvement of the tensile and shear
properties and higher residual compressive stress.
Bledzki et al. [327] investigated PLA biocomposites with
abaca and man-made cellulose fibers and compared these
1572 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
200
(a)
160
120
[MPa]
80
40
0
PLA PLA/abaca PLA/cellulose PP
10000
(b)
8000
6000
[MPa]
4000
2000
0
PLA PLA/abaca PLA/cellulose PP
Fig. 15. Tensile and flexural properties [(a) strength and (b) modulus] of
PLA and PP composites (fiber content 30 wt%).
Adopted from [327]. Copyright 2009. By permission from Elsevier Ltd.
to PP composites. The composites were processed using
combined molding technology: first a two-step extrusion
coating process was carried out and consecutively an injec-
tion molding was completed. With man-made cellulose
of 30 wt%, the tensile strength and modulus increased by
factors of 1.45 and 1.75 times in comparison to neat PLA.
Reinforcing with abaca fibers (30 wt%) enhanced both the
E-modulus and the tensile strength by factors of 2.40 and
1.20, respectively (Fig. 15).
The fibers’ length distribution in pellets after com-
pounding and in samples after injection molding is
depicted in Fig. 16. The measurement was evaluated using
approximately 500 fibers. A significant decrease in the fiber
length after compounding on the single-screw extruder
can be observed, from the cut length of 15 mm to about
1–2 mm. Moreover, the injection molded samples show
merely an insignificant drop in length, when put side
by side to pellets. This indicates to massive fiber length
reduction during extrusion processes. Processing on the
single-screw extruder already affected the length signif-
icantly. Compounding on twin-screw extruders, which is
often carried out during composite processing, can exceed-
ingly influence the fiber length even more. The minimal
fiber length achieved during compounding is not being
affected during the injection molding process; however,
the occurrence of the fiber length seems to be more uni-
form. As a result, most of the fibers, which remain longer
than 2 mm after compounding, are shortened less than
2 mm during injection molding.
PLA as a matrix for biocomposites reinforced with
biofiber was extensively investigated for jute fiber
[328–331], flax fiber [332,333], kenaf [334,335], coir [336],
bamboo [337] and cellulose fibers [338,339]. Special atten-
tion was paid to the influence of chemical treatments,
processing techniques, coupling agents, micro-fibrillated
Tensile strength
fiber bundles, and reinforcement using man-made cellu-
Flexural strength
lose fibers.
The mechanical properties of PLA reinforced with flax
fibers [340], the influence of the additives on the inter-
facial strength [341], as well as the effects of recycling
[342] and sea water aging [343] on the mechanical prop-
erties was investigated. It was found that the composite
strength is about 50% better compared to similar PP/flax
fiber composites, which are used in many automotive pan-
PP/abaca PP/cellulose els today. The different additives significantly influenced
the interfacial strength of the PLA/flax fiber composites
while extraction with acetone had no effect compared to
Tensile modulus
the untreated fibers. The use of TDP (4,40-thiodiphenol)
Flexural modulus
imparted the most significant increase in interfacial shear
strength whilst HBP (Hyper Branched Polyester) had an
opposing effect. The repeated injection molding cycles
were influenced by many parameters; i.e., the reinforce-
ment geometry, the molecular weight of PLA and, the
thermal and rheological behavior. The tensile stiffness of
PLA is hardly affected by seawater at temperatures approx-
PP/abaca PP/cellulose
imately of 40 ◦ C, but the composite does loses stiffness and
strength. The interfacial adhesion weakens more due to wet
aging. Cracks also appear in the PLA and flax fibers after
longer periods of time.
Huda et al. [344,345] examined the effect of reinforc-
ing recycled newspaper, the addition of silane and talc
on the thermal and mechanical properties of PLA/recycled
newspaper fiber composites. The results indicated that
the addition of fibers increased the thermal stability of
the composites compared to neat PLA. The heat deflec-
tion temperature of the PLA/recycled newspaper fiber
composites was found to be comparable to that of the
glass fiber-reinforced PLA composites. The silane treated
talc reinforced PLA/recycled newspaper fiber hybrid com-
posites flexural and impact strength was found to be
significantly higher than that of those made without
silane treated composites. The silane treated hybrid
composites showed improved properties such as a flex-
ural strength of 132 MPa and a flexural modulus of
15.3 GPa, while the untreated composites exhibited flexu-
ral strength and modulus values of only 77 MPa and 6.7 GPa,
respectively.
PLA and PHBV were compounded with man-made
cellulose; jute and abaca fibers and their mechanical
performance were studied and compared to PP based
composites [346]. It is clearly seen in Table 7 that the
tested biopolymer based composites clearly show better
or comparable mechanical characteristic values than the
‘common’ natural fiber reinforced PP composites.
4.2.2. PHB (polyhydroxybutyrate)
The biopolymer polyhydroxybutyrate (PHB) was also
reinforced with flax fiber. Barkoula et al. [347] investigated
the effects of fiber and copolymer HV (hydroxyvalerate)
contents, the biodegradability, and the influence of man-
ufacturing methods (compression molding of non-woven
mats and injection molding of short fiber compounds) and
processing conditions (cooling temperature and anneal-
ing) on the mechanical properties of the composites. It
can be concluded that the addition of flax fibers, along
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596 1573

Fig. 16. The fiber length of abaca/PLA composites after different processes.
Adopted from [327]. Copyright 2009. By permission from Elsevier Ltd.

with controlled processing conditions, is a convenient tech-
nique to toughen the PHB matrix. The injection molded
composites exhibited lower impact strength than other
manufactured composites. The tensile strength dropped
significantly in the initial stage of degradation and was
more gradual in later stages of biodegradation.
The interfacial improvement of PHB/flax composites
was also evaluated. The addition of TDP at various con-
centrations (up to 10% v/v) brought advantageous changes
in the dynamic flexural properties and thermal stability
(favorable shift of degradation temperatures to higher val-
ues). With increases of the TDP content, improvements
were observed in the fiber–matrix bonding and a change in
the matrix from brittle to ductile [348]. Zini et al. [349] illus-
trated that composites prepared by compression molding
using long fiber mats showed better mechanical properties
compared to composites obtained by batch mixing fibers
with molten polymer. Chemically modified (by acetylation
or by short-chain-PEG grafting) fibers exhibit better adhe-
sion and the best results were obtained with acetylated
fibers.
Several lines of transgenic flax were produced by over-
expressing the PHB synthesis genes [350]. It was revealed
that the cellulose in fibers from the transgenic plants was
more highly structured than in fibers from the control
plants and PHB was strongly bound to the cellulose of the
fibers by covalent ester and hydrogen bonds. The PHB/flax
composite with fibers from transgenic plants was signifi-
cantly stronger and stiffer than the composites with fibers
from the control plants.
Polyhydroxybutyrate-co-valerate (PHBV) bioplastic
was reinforced with hemp [351], coir [352], and bamboo

Table 7
Mechanical properties of PLA, PHBV and PP based natural fiber reinforced composites.

Matrix Fiber Tensile E-modulus (GPa) Tensile strength (MPa) Tensile elongation-at-break (%)

PLA – 3.4 ± 0.23 63.5 ± 0.4 3.3 ± 0.5

Man-made cellulose 5.8 ± 0.15 92.0 ± 4.7 1.9 ± 03
Abaca 8.0 ± 0.34 74.0 ± 0.7 1.44 ± 0.1
Jute 9.6 ± 0.36 81.9 ± 2.9 1.8 ± 0.0
PHBV/ecoflex – 2.14 ± 0.07 27.3 ± 0.3 7.0 ± 1.1
Man-made cellulose 4.4 ± 0.34 41.7 ± 3.8 2.3 ± 1.0
Abaca 4.4 ± 0.06 28.0 ± 1.3 0.9 ± 0.1
Jute 7.0 ± 0.26 35.2 ± 1.3 0.8 ± 0.0
PP – 1.5 ± 0.03 29.2 ± 0.4 >50
Man-made cellulose 3.7 ± 0.11 71.6 ± 2.7 3.5 ± 0.5
Abaca 4.9 ± 0.11 42.0 ± 0.5 1.7 ± 0.2
Jute 5.8 ± 0.47 47.9 ± 2.7 1.4 ± 0.1
1574 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
[353] fibers. The mechanical, thermo-mechanical and
morphological properties were evaluated.
4.2.3. Starch
Alvarez et al. [354–356] developed composites by mix-
ing biodegradable starch matrixes with sisal fibers. The
thermal, melt rheological and creep properties were inves-
tigated extensively. It was reported that the shear rate is the
most influential processing condition regarding the mate-
rial structure. The intercalation effectiveness of the matrix
in the fibers is directly linked to the rheological behavior.
The addition of sisal fibers to the polymeric matrix pro-
motes a significant improvement of the composite creep
resistance and thermal properties.
Investigations were carried out using starch as the
matrix of composites with kenaf, bagasse [357], curaua
[358], coir [359], bamboo [360], sisal [361], hemp
[362,363], abaca and bagasse [364] fibers, wheat straw
fibers [365], and kenaf fibers [366].
4.2.4. Others
A soy based biodegradable resin matrix was applied
to cellulose from papers [367], flax [368], sisal [369]
and pineapple leaf [370] fiber reinforced composites.
Biodegradable resins have been tested, including cashew
nut shells [371,372] with hemp and kenaf fibers, poly-
butylene succinate (PBS) with jute fibers [373,374] bamboo
fibers [375], and hemp fibers [376], and polycaprolactone
(PCL) with flax fibers [377] and bamboo fibers [378].
4.3. Summary
The petroleum derived thermoplastics PP and PE are
the two most commonly employed thermoplastics in nat-
ural fiber reinforced composites. Day by day, there is great
interest in developing biocomposites with a thermoplastic
rather than thermoset matrix, mainly due to their recy-
clability. Also the choice of a thermoplastic matrix fits well
within the eco-theme of biocomposites, but there are some
important limitations on the recyclability and mechanical
performance of thermoplastics. Generally, the mechanical
properties of thermosets exhibit higher than the ther-
moplastic (lower modulus and strength). In addition, a
dramatic loss in properties is observed above the glass
transition temperature, which leads to decrease in other
thermally sensitive properties such as creep resistance. On
the contrary, thermoplastics show greater fracture tough-
ness than thermosets and thus are more useful in resisting
impact loads. Another remarkable change was the intro-
duction of biopolymers in recent years with the aim of
decreasing reliance on petroleum-based thermoplastics.
The availability and outstanding mechanical properties of
biopolymer PLA has led to this matrix system being one
of the most thoroughly investigated in the biocomposites
research area.
5. Processing techniques
Generally, natural fiber reinforced plastic composites
are manufactured by using traditional manufacturing tech-
niques (designed for conventional fiber reinforced polymer
Fig. 17. Water absorption of HDPE composites with and without compat-
ibilizers.
Adopted from [380]. Copyright 2007. By permission from Elsevier Ltd.
composites and thermoplastics). The processing tech-
niques includes compounding, mixing, extrusion, injection
molding, compression molding, and resin transfer mold-
ing (RTM) and above mentioned techniques have been
well developed and accumulated experience has proofed
their successability for producing composites with control-
lable quality. Innovative technologies and process solutions
should be intensively researched to get the high strength
engineering composites which is related to their new appli-
cations area.
5.1. Factors influencing processing
5.1.1. Moisture
The moisture content at a given relative humidity can
have a great effect on the biological performance of a com-
posite made from natural fibers and therefore fiber drying
before processing is a significant step. A composite made
from pennywort fibers would have much greater moisture
content (57%) at 90% RH humidity than would a composite
made from bamboo fibers (15%). The pennywort product
would be much more prone to decay as compared to the
bamboo product. Moisture content of natural fibers with
time under different conditions (relative humidity) and for
different fiber treatments were analyzed [379]. It was evi-
dent that the moisture content as well as the rate at which
it accumulates is directly related to the ambient relative
humidity. Fiber treatment can reduce both the moisture
content level and the rate of absorption very significantly.
It should be noted that bio based polymers can be more
sensitive to moisture than natural fibers.
Panthapulakkal and Sain investigated the effect of com-
patibilizer on the water absorption behavior of HDPE
composites with different fillers (wheat straw, cornstalk,
and corncob). This is shown in Fig. 17 [380]. Presence of
compatibilizer had no effect on the water absorption of
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596 1575

Fig. 18. Compounding methods for injection molding of natural fiber reinforced thermoplastics.
Adopted from [383]. Copyright 2006. By permission from Institute for Materials Technology of the University of Kassel, Germany.

corncob filled composites. Wheat straw and cornstalk filled
composites showed a decrease in the water uptake with
the incorporation of compatibilzers. This indicates that, the
flaws and gaps at the interface of the filler and HDPE are
the main factors for moisture diffusion in the composites
without compatibilizer. As observed in mechanical prop-
erties, the observed reduction in water uptake is higher in
wheat straw filled composites compared to cornstalk filled
composites. After 40 days of water absorption, percentage
reduction in the water uptake of composites is 19%, 12%
and 0% respectively for wheat straw, corn stalk and corncob
filled composites.
It is already seen that the enhanced water content
can drastically affect mechanical properties (such as, com-
pression, flexural and tensile) of the composites [381].
Nowadays new extruder screw design (higher L/D ratio)
allows better degassing and, consequently, lower mois-
ture content. In addition, the machine’s barrel must be
redesigned.
5.1.2. Fiber type and content
The natural fiber type and content is generally essen-
tial for furthering the sustainability of the composite. In
addition, natural fibers length (short or long), aspect ratio
(length/diameter), chemical compositions (such as rice
husk contains higher silicates than flax or jute fiber) have
an great influence on the processing and therefore process-
ing parameters and accessories should be developed. The
compounding process significantly influences the shorten-
ing, fibrillation, as well as the thermal deterioration of the
fibers in early stages; the final properties of the product
are already determined at the beginning of the production
process [382]. Fig. 18 shows the different compounding
processes for injection molding of natural reinforced ther-
moplastics [383].
5.1.3. Influence on composites properties
As described above, the natural fiber type has strongly
influence on the performance of the composite. There are

Fig. 19. Influence of different natural fibers on the tensile and Charpy notched impact strength (+23 ◦ C) of PLA biocomposites (fiber content 30 wt%).
Adopted from [387]. Copyright 2008. By permission from Woodhead Publishing Ltd.
1576 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 20. Influence of abaca fiber content on odor concentration of abaca/PP
composites.
Adopted from [387]. Copyright 2008. By permission from Woodhead Pub-
lishing Ltd.
numerous types of natural fibers, which differ regarding
their chemical structure [384–386]. The influence of the
type of natural fiber on some mechanical parameters of
PLA biocomposites is presented in Fig. 19 [387].
In general, increasing fiber content in the composites
increases the composite’s stiffness significantly. Addition-
ally its strength is increased through the addition of natural
fibers [388,389]. Higher fiber content improves the impact
strength. Unfortunately, increased fiber content increases
the composite’s odor (Fig. 20) as well as the water uptake
[387]. Moreover, the composite’s ductility can be affected.
The fiber length and its geometry also play a decisive role in
composites. Usually, most mechanical properties of a fiber
can be enhanced by increasing the aspect ratio [390].
In addition, the use of one appropriate additive (cou-
pling agents, lubricants, light stabilizers, colorants, flame
retardants, foaming agents, odor reduction agents, and bio-
cides) in very small quantities (0.5–5%) can significantly
improve most of physical, chemical or mechanical proper-
ties of natural fiber composite material [391].
5.2. Semi-finished product manufacturing
Mat production is one of the initial steps in semi-
finished product manufacturing. Fiber mats (fiber fleece)
from natural fibers could be manufactured by carding
method, aerodynamic fleece making, the fiber spreading
process, and wet fleece production. The other step is the
production of slivers and fiber yarns. The fiber prepara-
tion (opening, mixing, and carding) is similar to fleece
production. Granule production is the other important
step in the manufacture of semi-finished products. Natural
fiber granules can be produced via pelleting, compounding,
pultrusion and the pull-drill process regarding the homo-
geneity of the granules and the desired fiber lengths.
5.3. Processing technologies for natural fiber reinforced
thermoplastics
5.3.1. Compression molding
The pressure method is very popular in the manu-
facture of natural fiber composites because of its high
reproducibility and low cycle time. The two methods in
use are compression and flow compression molding. The
processes differ concerning the kind of semi-finished prod-
uct used and its cutting. In the compression molding
process, flat semi-finished products or hybrid fleeces are
usually used that are either larger than the form or are cut
exactly to the size of the desired part.
Whole and split wheat straws with lengths up to 10 cm
were used with PP to make lightweight composites by
means of the compression molding process [392]. The
effects of the wheat straw concentration, length, and split
configuration (half, quarter, and mechanically split) on
the flexural and tensile properties of the composites were
investigated. Compared with whole wheat straws–PP com-
posites, mechanically split wheat straw–PP composites
have a flexural strength that is higher by 69%. They also
have a 39% higher modulus of elasticity, 18% higher impact
resistance properties, 69% higher tensile strength and a 26%
higher Young’s modulus. Compared with jute–PP compos-
ites, mechanically split wheat straw–PP composites have
a 114% higher flexural strength, 38% higher modulus of
elasticity. In addition, they also have a 10% higher tensile
strength, 140% higher Young’s modulus, a 50% lower impact
resistance and better sound absorption properties.
The compression molding process was tested for jute
fiber with PP [393], an ethylene propylene co-polymer
[394] and, baggase fibers with PET composites [395].
Also the abrasive wear behavior, interfacial adhesion, and
degradability were evaluated.
5.3.2. Extrusion
The extrusion process is used by the plastics industry
for the production of granules and also in the continuous
production of semi-finished products or components. Sin-
gle screw as well as twin-screw extruders that run either
co- or counter-rotating may be used for this process. Single
screw extruders are used when the mixing effect does not
have to be very high. Owing to the excellent mixing effect of
the twin-screw extruder the natural fiber materials can be
homogenously distributed and wetted in the thermoplastic
melt.
HDPE composites with bagasse [396] and curaua [397]
fibers reinforced HDPE composites were obtained by
extrusion process. The effects of coupling agents on the
mechanical and thermal properties of those composites
were investigated and evaluated. Curaua fibers were also
reinforced with PA-6 by using a co-rotating twin-screw
extruder [398]. The fiber contents of 20 wt%, 30 wt% or
40 wt% and fiber lengths of 0.1 or 10 mm were studied.
Fibers were treated with N2 plasma or washed with NaOH
solution, to improve their adhesion to PA-6. The tensile
and flexural properties of this composite are better than
unfilled, but are still lower than those of glass fiber rein-
forced polyamide-6.
5.3.3. Injection molding
It is possible to produce complex geometric compo-
nents with functional elements fast and also in great
numbers by injection molding. It offers a number of advan-
tages (economics of scale, minimal warping and shrinkage,
high function integration, use of recycled materials) as
compared to compression molding [399] and hardly any
finishing needed.
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596 1577

Table 8
Tensile strength and modulus of PP and PP/hemp fiber/glass fiber hybrid composites before and after aging (A. 0 wt% glass fiber, B. 5 wt% glass fiber, C.
10 wt% glass fiber, D. 15 wt% glass fiber).

Sample designation Tensile strength (MPa) Tensile modulus (GPa)

Original Wet sample Retention (%) Original Wet sample Retention (%)

PP 30.1 ± 0.1 29.9 ± 0.5 99 1.10 ± 0.03 0.89 ± 0.03 81

A 52.5 ± 0.5 34 ± 0.6 65 3.77 ± 0.05 1.64 ± 0.04 44
B 53.7 ± 1.6 34.8 ± 1.6 65 4.07 ± 0.05 1.74 ± 0.03 43
C 57.9 ± 0.7 34.9 ± 0.9 60 4.25 ± 0.04 2.04 ± 0.05 48
D 59.5 ± 0.9 35.5 ± 0.5 65 4.4 ± 0.01 2.32 ± 0.12 53

Pickering and his co-workers [400–403] extensively
investigated hemp fiber reinforced PP composites used
in the injection molding process. Their investigations
included fiber treatments and modifications, model predic-
tions of micro-mechanics and strengths, the optimization
of hemp fiber quality, and the influence of bag retting and,
white rot fungal treatments.
The effect of surface treatment on the injection molded
pineapple leaf fiber reinforced polycarbonate composites
was evaluated [404]. The modified pineapple leaf fibers
composite produces enhanced mechanical properties. The
results from the thermogravimetric analysis showed that
the thermal stability of the composites is lower than that
of neat polycarbonate resin and that the thermal stabil-
ity decreased with increasing pineapple leaf fiber content.
Injection molded jute [405] and sisal [406] fiber reinforced
PP composites were also investigated regarding their ther-
mal, hydrothermal and, dynamic mechanical behavior. The
introduction of the pre-impregnation technique was also
examined.
Panthapulakkal and Sain investigated the influence of
water absorption on the tensile properties of injection
molded short hemp fiber/glass fiber-reinforced polypropy-
lene hybrid composites [407]. Tensile tests were performed
on wet samples after the saturation level (3624 h) is
reached (Table 8). A significant reduction in strength and
stiffness is observed for all composites because of the
changes to the fibers, mainly natural fibers, and the inter-
face between the matrix and fiber, as the effect of water
absorption on PP matrix is only secondary. Swelling of nat-
ural fiber as a result of prolonged exposure to water, leads
to at reduction in the stiffness of the fibers. The loss in
strength and modulus values of the hemp fiber composites
are believed to be the inability of the swelled natural fiber
to carry the stress transferred from the matrix through the
disrupted interface as a result of water absorption. Despite
the reduction in the equilibrium moisture content in hybrid
composites, glass fibers did not alter the degradation of the
hemp fiber composites.
Injection molded flax, hemp, core hemp, bleached kraft
pulp (BKP) and wood flour reinforced PP composites were
prepared and the effect of MAPP on the mechanical prop-
erties was investigated [408]. Table 9 clearly indicated that
the BKP–PP composites have the highest tensile and flex-
ural strength and unnotched impact strength. Flax and
hemp-filled PP composites have similar strength prop-
erties. In comparison, wood flour-filled PP composites
have the lowest mechanical strength. Such a trend can be
attributed to the actual fiber length in the composites. It has
been observed that after compounding, the fiber length of
flax and hemp decrease significantly, whereas that of BKP
fibers dose not change much. This is possibly due to the
fact that the flax and hemp bundles are prone to being torn
down to very small size by the high-shear force from the
melted PP. To preserve the fiber length, less severe treat-
ment is necessary but at the cost of poor dispersion of fibers
in the resin matrix. The poor strength of wood flour rein-
forced composites is due to the low aspect ratio of wood
flour particles, which is far below the critical fiber length
required for reinforcement.
Bledzki et al. [409] investigated the different separation
processes (mechanical, refiner and enzymatic separation)
with injection molded hemp and partially with flax and
wheat straw reinforced PP composites. It was found that
thermomechanical processed hemp fiber–PP composites
possessed better mechanical properties compared to other
process and composites.
5.3.4. Long fiber thermoplastic-direct (LFT-D) method
Different methods [410] to directly process natural
fibers with the LFT-D-process are shown (Fig. 21). Express
method, which is the basic thought of the combined extru-
sion and press method to combine the natural fiber mats
with the polymer melt directly in the pressing tool. A film
of molten polymer is placed into the pressing tool with the
help of an adjustable extruder and a natural fiber fleece
is added to the molten mass and the layers are pressed
together. Another possibility to process natural fibers with

Table 9
Effect of filler type on mechanical strength performance of filledPP composites (40% filler, 2% compatibilizer).

Fiber type BKP Flax Milled hemp Core hemp Wood hour

Tensile (MPa) 50 42 42 29 35
Tensile modulus (GPa) 3.0 3.2 3.0 2.3 2.9
Flexural (MPa) 78 67 70 52 59
Flexural modulus (GPa) 3.3 3.4 3.5 2.6 3.0
Notched Izod (J/m) 40 44 42 20 28
U-notched Izod (J/m) 205 150 145 100 105
1578 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596

Fig. 21. Express method and direct extrusion of natural fibers.

Adopted from [410]. Copyright 2002. By permission from Institute for Materials Technology of the University of Kassel, Germany.

the LFT-D-method is to directly feed off fiber yarns or sliv-

ers into either a twin screw extruder or directly into an
injection molding machine. Research has shown that it is
possible to retain the long fiber structure through an opti-
mal configuration of the screws; however, the handling of
slivers is rather problematic in an industrial application
(extrusion with high throughput).

5.4. Processing technologies for natural fiber reinforced

thermosets

5.4.1. Resin transfer molding

Resin transfer molding (RTM) is a method for the
production of component parts made of fiber-plastic com-
posites. During the RTM procedure, dry semi-finished fiber
Fig. 22. Comparison of RTM experiment and corrected model for a pure
parts are streamed and consequently soaked with reaction resin system.
resin by a pressure gradient within a closed vessel. The fol- Adopted from [411]. Copyright 2004. By permission from Elsevier Ltd.
lowing methods can be distinguished with regard to the
admission by the pressure gradient: high pressure injec- and their cure simulation, interfacial adhesion, and flow
tion, twin wall injection, vacuum injection, and differential visualization were evaluated.
pressure injection. The effects of fiber surface modification [415] were
Hemp fiber-unsaturated polyester composites were evaluated. A comparison of the RTM process to the com-
manufactured using a resin transfer molding (RTM) pro- pression molding process [416] of sisal fiber reinforced
cess [411]. RTM composites with various fiber contents, polyester composites was made. Composites containing
up to 20.6% by volume, were manufactured. The wetting flax and hemp fiber with bio-resin [417], flax and jute fiber
of the fibers was very good. The resin injection time was with epoxy and polyester resin [418], and jute fiber with
observed to increase dramatically at high fiber contents polyester resin [419] were also prepared using the RTM
due to the low permeability of the mat. Keeping a constant process.
mold temperature is the key to obtain fast and homoge-
neous curing of the part. The cure of the resin in the mold 5.4.2. Sheet molding compound
was simulated. The results given by the modified model The sheet molding compound (SMC) material made of
are presented in Fig. 22. The predicted temperatures were natural fibers and a special resin based on vegetable oil
in very good agreement with the experimental data. The and carbohydrates represents an effective alternative to
model predicted the degree of cure and the rate of cure of the established systems within the technically specialized
the resin with time as well. sector. Procedural modifications are not necessary in com-
The hemp fiber composites manufactured with RTM parison to conventional SMC production of component
process were found to have a very homogeneous structure
Table 10
with no noticeable defects [412]. The tensile, flexural and Mechanical properties of 20 vol% glass fiber, 20 vol% hemp fiber and
impact properties of these materials was found to increase 35 vol% hemp fiber-reinforced unsaturated polyester composites.
linearly with increasing fiber content (Table 10). It was
20 vol% 20 vol% 35 vol% hemp
observed that the optimum properties were not reached in glass fibers hemp fibers
this study and that fiber content higher than 35 vol% should fibers
yield better mechanical properties. When compared to a Tensile strength (MPa) 85.0 32.9 60.2
glass fiber composite however these natural fiber compos- Tensile modulus (GPa) 1.719 1.421 1.736
ites had much lower performances. Flexural strength (MPa) 175.9 54.0 112.9
Hemp fiber reinforced polyester [413] and phenolic Flexural modulus (CPa) 7.74 5.02 6.38
Impact strength (kJ/m2 ) 60.8 4.8 14.2
resin [414] composites were prepared using RTM process
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 23. Thermoset mat compression process and ready component part; raw and covered by all functional and decorative details.
Adopted from [423]. Copyright 2006. By permission from Institute for Materials Technology of the University of Kassel, Germany.
parts [420]. The middle bumper part for a city bus was
manufactured with standard tools. The risk potential for
the fabricator is lower, both during production and treat-
ment of the prepregs which are made of natural fibers and
vegetable oil. Emissions do not occur; hence, there is no
need for breathing protection [421]. Flax fiber reinforced
SMC material was developed and the processing param-
eters regarding the physico-mechanical properties were
optimized [422].
5.5. Other processes
5.5.1. Thermosets compression molding
The thermosets compression process uses mats made of
natural fibers. As shown in Fig. 23, the mats are just sprayed,
not moistened, with resin and compressed into their final
contour in a hot tool; due to the air-permeability the parts
can be covered easily in a vacuum covering process [423].
The dynamic and static mechanical properties of short
abaca/sisal hybrid fiber reinforced polyester composite
achieved using the thermoset compression molding pro-
cess were determined [424]. Dynamic properties, such as
the storage modulus, damping behavior and static mechan-
ical properties (i.e., tensile, flexural and impact properties)
were investigated as a function of the total fiber volume
fraction and the relative volume fraction of the two fibers.
The storage modulus was found to increase with fiber vol-
ume fraction above the glass transition temperature (Tg ) of
the matrix. A maximum value was obtained at a volume
fraction of 0.40. The tensile modulus and flexural strength
were found to be the highest at a volume fraction of 0.40,
which indicates effective stress transfer between the fiber
and the matrix. Sisal/polyester composites displayed the
best damping behavior and highest impact strengths com-
pared to abaca/polyester and hybrid composites. However,
maximum stress transfer between the fiber and the matrix
was obtained in composites with a volume ratio of banana
and sisal equal to 3:1. The tensile strength and flexural
modulus reached their maximum at this volume ratio,
while the impact strength reached its minimum.
The thermal conductivity, diffusivity and specific heat
of thermoset compression molded polyester/natural fiber
(abaca/sisal) composites were investigated for several fiber
surface treatments as functions of the filler concentration
[425]. The thermo-physical behavior of hybrid pineap-
ple leaf fiber (PALF) and glass fiber reinforced polyester
1579
composites were also evaluated regarding the constant
total fiber loading equal to 0.40 volume fraction by vary-
ing the ratio of PALF and glass. The results show that
the chemical treatment of the fibers reduces the com-
posite thermal contact resistance. Hybridization of natural
fibers with glass allows a significantly better heat trans-
port ability of the composite. The thermal conductivity,
which is measured in the direction transverse to the plane
of composite plate, could be well represented by a series
prediction model.
5.5.2. Pultrusion
Fibers are pulled from a creel through a resin bath and
then on through a heated die. The impregnation of the fiber
controls of the resin content and curing of the materials into
their final shape is completed using the die. Although pul-
trusion is a continuous process, which produces a profile
of constant cross-sections, a variant known as pulforming
allows for some variation to be introduced into the cross-
sections.
Flax fiber reinforced PP composites were developed by
means of the thermoplastic pultrusion process and their
physic-mechanical properties were evaluated [426]. The
water absorption behavior of pultruded jute fiber rein-
forced unsaturated polyester composites was found to
follow so-called pseudo-Fickian behavior [427]. The flex-
ural and compression properties were found to decrease
with the increase in water uptake in percentage. These
flexural and compression behaviors were attributed to the
plasticization of the matrix-fiber interface and the swelling
of the jute fibers.
Pultruded kenaf fiber [428], jute fiber [429] and hybrid
jute/glass and kenaf/glass fiber [430] composites were
investigated and their flexural behavior using acoustic
emission, dynamic properties and degradation of compres-
sive properties were evaluated.
5.5.3. Summary
In recent years the processing and production tech-
nologies for biocomposites have also advanced. To date,
injection molding, extrusion, compression molding, sheet
molding and resin transfer molding are the major man-
ufacturing processes for natural fiber reinforced plastic
composites. But new downstream and auxiliary equipment
has been designed. Such as: unique heating and single
or dual venting systems for in-line drying, high-intensity
1580 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
spray-cooling tanks, a variety of new configurations
of feeding (gravimetric or vertical crammer) systems,
combinations of extrusion-injection molding or extrusion-
compression molding as well as screw, die, and mold
design. Although the majority of biocomposites produced
today by the processes mentioned above, the manufactur-
ers are improving the feasibility of using other processes
like pultrusion and so on.
6. Performance of biocomposites
It is important to be knowledgeable of certain mechan-
ical properties of each natural fiber in order to be able to
exploit the highest potential of it. Among these properties
are the tensile, flexural, impacts, dynamic mechanical and
creep properties. In general, natural fibers are suitable for
reinforcing plastics, due to their relatively high strength,
stiffness and low density.
6.1. Tensile properties
The tensile properties are among the most widely tested
properties of natural fiber reinforced composites. The fiber
strength can be an important factor regarding the selec-
tion of a specific natural fiber for a specific application. A
tensile test reflects the average property through the thick-
ness, whereas a flexural test is strongly influenced by the
properties of the specimen closest to the top and bottom
surfaces. The stresses in a tensile test are uniform through-
out the specimen cross-section, whereas the stresses in
flexure vary from zero in the middle to maximum in the
top and bottom surfaces.
The comparison of the tensile properties of the
HDPE/hemp fiber composites showed that the silane
treatment and the matrix-resin pre-impregnation of the
fiber produced a significant increase in tensile strength,
while the tensile modulus remained relatively unaffected
[431,432]. The longitudinal tensile strength increased from
71.8 MPa to 79.3 MPa for the silane treated fibers, which
equals an increase of approximately 10%. The increase
in the transverse tensile strength from 2.75 MPa for the
untreated fibers to 3.95 MPa for the treated fibers is higher,
representing an increase of 43%. It is evident that the
behavior is fiber dominated, as the longitudinal fiber direc-
tion, is 1900% higher compared to transverse direction.
Fiber surface modification has little impact. However, the
improvement in the fiber–matrix interactions plays a more
important role for the matrix and/or interphase dominated
behavior.
Rice husk reinforced PP composites with filler load-
ings of 10 wt%, 20 wt%, 30 wt% and 40 wt% were designed
[433]. Six test temperatures (−30, 0, 20, 50, 80 and 110 ◦ C)
and five levels of crosshead speed (2, 10, 100, 500 and
1500 mm/min) were designed during tensile testing. The
tensile strengths of the composites decreased slightly as
the filler loading increased. The tensile modulus improved
with increasing filler loading. As the crosshead speed
increased, the composite became more brittle. At lower
test temperatures (−30 and 0 ◦ C), the composites exhib-
ited strong and brittle properties similar to glass fiber, but
the tensile strength and modulus decreased due to the glass
transition of the matrix polymer PP as the test temperature
was increased from 0 to 20 ◦ C.
A study on the effect of alkaline treatment on tensile
properties of sugar palm fiber reinforced epoxy compos-
ites was investigated [434]. The treatment was carried
out using different concentrations of sodium hydroxide
(NaOH) solutions and varying soaking periods. It was
observed that as the alkali concentration and the length of
soaking periods increased, the tensile strength decreased.
However, the tensile modulus results are much higher than
those of untreated fiber composite specimens, thus proving
the effectiveness of the treatment.
Composites consisting of aliphatic polyester (Bionolle)
with flax fibers were prepared via batch mixing [435].
The effects of processing conditions on the fiber length
distribution and the dependence of the composite ten-
sile properties on the fiber content were investigated. The
tensile modulus changes with the amount of fiber con-
tent according to the modified rule-of-mixture equation.
The tensile strength of Bionolle/flax composites tends to
decrease with fiber loading, showing that there is no adhe-
sion between the matrix and the fibers. Flax fibers with
chemically modified surfaces were also tested as reinforc-
ing agents. An increase in tensile strength of 30% was
observed when flax fibers (25 vol%) were substituted with
fibers containing acetate groups. No significant strength
changes were observed in composites containing fibers
with valerate groups or polyethylene glycol chains grafted
at the surface.
The following investigations were completed with ther-
moplastic matrices; the effect of moisture absorption of
sisal fiber/PP composites [436], the influence of surface
treatment (NaOH solution) of coir fiber/PP composites
[437], the surface esterification of bagasse/LDPE com-
posites [438], the surface modification of olive husk/PP
composites [439], the performance of hybrid jute/betel nut
fiber reinforced PP [440], and the effects of surface treat-
ments of luffa fiber/PP composites [441]. It was observed
that the tensile properties were influenced by all the men-
tioned factors.
The tensile properties of natural fiber reinforced ther-
mosets were investigated regarding the siloxane treatment
of jute fiber/polyester and epoxy composites [442], the
temperature and loading rate effects of kenaf fiber/epoxy
composites [443], the effects of a differing geometry
of abaca fiber/epoxy composites [444], the influence of
moisture absorption of bamboo/vinylester composites
[445], the effect of oil palm fibers volume fraction of
oil palm/polyester composites [446], and the influence
of the fiber orientation and the volume fraction of alfa
fiber/polyester composites [447].
The effects of hybridization and the chemical modi-
fication of oil palm/sisal fiber reinforced natural rubber
composites [448,449], the effects of high temperature on
ramie fiber/biodegradable resin composites [450], effect of
biodegradable matrix type (PLA, PHBV, PBS) on regenerated
cellulose fiber/biopolymer composites [451], the influence
of bio based coupling agent on bamboo fiber/PLA and PBS
composites [452], preparation of sandwich composite pan-
els for building applications from jute/polyester [453], and
the structural and mechanical characterization of sugar
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
beet pulp/PLA composites [454] on the tensile properties
were evaluated.
Rao et al. [455] investigated the tensile properties of
bamboo, date palm, abaca, oil palm, sisal, coir and vakka
fibers regarding their fiber cross sections, atmospheric
moisture content and density.
6.2. Flexural properties
The flexural stiffness is a criterion of measuring
deformability. The flexural stiffness of a structure is a func-
tion based upon two essential properties: the first is the
elastic modulus (stress per unit strain) of the material that
composes it; and the second is the moment of inertia, a
function of the cross-sectional geometry.
Zampaloni et al. [456] focused on the fabrication of
kenaf fiber reinforced PP sheets that could be thermo-
formed for a wide variety of applications with properties
that are comparable to existing synthetic composites. The
optimal fabrication method determined for these materi-
als was determined to be a compression molding process
which utilized a layered sifting of a microfine PP powder
and chopped kenaf fibers. When comparing the flexu-
ral strengths of the kenaf fiber/PP composite materials,
40% kenaf/PP composites performed significantly better
than the 30% kenaf/PP composites. The flexural strength
of 40% kenaf/PP was equivalent to the flax/PP, larger than
the hemp/PP and almost doubles that of the coir/PP and
sisal/PP composites. The flexural strength of 30% kenaf/PP
composites showed results equivalent to those of the 40%
hemp/PP composites, while also outperforming the coir/PP
and sisal/PP composites.
Composites of PP and HDPE reinforced with 20 wt%
curaua fibers were prepared and the effect of screw rotation
speed was evaluated by measuring the flexural properties
of the composites [457]. The yield stress in flexural tests for
the composites with PP and HDPE matrixes, decreased with
the increase in screw rotation speed. For HDPE a higher rate
of decrease was shown. However, the flexural modulus was
not affected by the screw rotation speed. The elongation
at break exhibited different behavior; this effect strength-
ened HDPE at screw rotations above 300 rpm, and slightly
increased for PP composites above 350 rpm.
The effect of acetylation [458] on the flexural proper-
ties of bagasse/PP composites (properties decreased due
to acetylation), and the effect of different maleated cou-
pling agents (flexural properties increased above 60% with
optimum loading of coupling agent) on jute and flax fiber
reinforced PP composites [459] have been evaluated.
Composites were fabricated using abaca fiber with vary-
ing fiber lengths and fiber loading [460]. The analysis of
the flexural properties revealed the optimum length of
abaca fibers required for abaca fiber/phenol formaldehyde
resin composites. The flexural strength and modulus val-
ues increased with fiber length for composites with short
fibers. Furthermore, the maximum flexural strength and
modulus values were obtained for 40 mm fibers. Due to
fiber loading up to 45%, the flexural modulus increased
to about 25%. The flexural strength also showed good
enhancement, because of increasing fiber loading.
1581
The flexural properties of coir fiber/polyester compos-
ites were evaluated [461]. Composites were prepared using
two molding pressures and with amounts of coir fiber up
to 80 wt%. When the fiber amount equaled up to 50 wt%,
rigid composites were obtained. Higher fiber amounts
resulted in composite performances similar to that of flex-
ible agglomerates. The results obtained for the flexural
strength made it possible to compare the technical perfor-
mance of the composites with that of other conventional
materials.
The flexural properties of thermoset resins, such as car-
danol reinforced with hemp, ramie, jute and flax fibers
[462], epoxy resin with coir fibers [463], and hemp, kenaf,
flax and henequen fibers [464], polyester resin reinforced
bagasse fibers [465], coir and oil palm fibers [466], hemp
and kenaf fibers [467], were also investigated.
Biocomposites were fabricated from chopped hemp
fiber and cellulose ester biodegradable plastic via two dif-
ferent processes: powder impregnation by compression
molding and an extrusion process followed by an injec-
tion molding process [468]. Fabricated through process
extrusion followed by injection molding process of hemp
(30 wt%) fiber reinforced cellulose acetate biocomposite
exhibited flexural strength of 78 MPa and modulus of elas-
ticity of 5.6 GPa as contrast to 55 MPa and 3.7 GPa for the
corresponding hemp fiber/PP based composite. The corre-
sponding biocomposites showed superior flexural strength
and modulus values during the extrusion and ensuing
injection molding processes, as compared to biocompos-
ites powder impregnated through compression molding
process.
Biodegradable composites were prepared with the melt
blending technique using PCL and oil palm empty fruit
bunch fiber [469]. Since oil palm fiber is not compati-
ble with PCL, a binder (polyvinyl pyrrolidone), was used
to improve the interaction between PCL and the fibers.
The composites produced were irradiated with the aid
of an electron beam to improve the mechanical proper-
ties. The flexural strength and modulus of the composites
were improved by an additional 1% by weight of poly(vinyl
pyrrolidone) and irradiated with a 10 kGy electron beam.
6.3. Impact properties
Impact strength is the ability of a material to resist
fracture under stress applied at high speed. Biofiber rein-
forced plastic composites have properties that can compete
with the properties of glass fiber thermoplastic compos-
ites, especially concerning specific properties. However,
one property, namely the impact strength is often listed
among the major disadvantages of biofiber reinforced com-
posites. In recent years, the development of new fiber
manufacturing techniques and improved composite pro-
cessing methods along with enhancement of fiber/matrix
adhesion has improved the current situation somewhat.
Jute fiber was treated with o-hydroxybenzenedi-
azonium salt (o-HBDS) in alkaline media [470]. Treated and
untreated jute fiber reinforced PP composites were pre-
pared with different weight fractions (20, 25, 30, and 35%)
of jute fiber. The increase of Charpy impact strength was
1582 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
found to be exceptionally high (in some cases ∼200%) as
compared to those of literature values.
Composite panels consisting of virgin and recycled
HDPE and four types of rice straw components includ-
ing rice husk, rice straw leaf, rice straw stem, and whole
rice straw were made via melt compounding and com-
pression molding [471]. Composite panels with rice husk
exhibited better impact strength than composites panels
made of other straw fibers. Minor differences concerning
the impact properties existed among leaf, stem, and whole
straw fibers. The recycled HDPE resin and its composites
possessed a significantly better impact strength compared
to the virgin HDPE systems. This was attributed to the addi-
tives used during initial processing.
Recycled HDPE composites were reinforced with
bagasse fibers and the influence of coupling agent
types/concentrations on the composite impact prop-
erties were studied [472]. The addition of maleated
polyethylene (MAPE), carboxylated polyethylene (CAPE),
and titanium-derived mixture (TDM) improved the com-
patibility between the bagasse fiber and recycled HDPE.
The impact properties of the resultant composites were
comparable with those of virgin HDPE composites. The bet-
ter impact strength of the composites was achieved, when
a MAPE coupling agent was used. The impact strength
increased with increasing MAPE content.
Oil palm empty fruit bunch fiber reinforced composite
was studied. The effects of fiber loading and impact mod-
ifiers, namely chlorinated polyethylene (CPE) and acrylic,
on the impact properties of oil palm fiber filled-PVC com-
posites were of particular interest [473]. The results from
the impact test showed that the unfilled PVC samples of
both impact modifiers change from brittle to ductile with
increasing impact modifier concentration. The incorpo-
ration of fibers into unmodified PVC and modified PVC
resulted in the reduction of the impact strength. As the fiber
content increased from 10 to 40 phr, the impact strength
reduced about 40% and 30% for acrylic-modified PVC
and CPE-modified PVC, respectively. The impact strength
reduction was only marginal for unmodified PVC compos-
ites. The impact modifier enhanced the impact strength of
fiber reinforced PVC composites. However, the effective-
ness decreased with increased fiber loadings. The impact
strength of CPE-modified PVC was higher than acrylic-
modified PVC at fiber contents of 20 phr and higher.
The impact properties regarding the influence of the
fiber microstructure of sisal, abaca, jute and flax fiber rein-
forced PP composites [474], the processing methods for
flax fiber/PP composites [475], and the effect of impact
modifiers (natural rubber and ethylene propylene diene
monomer) on grass fiber/PP composites [476] were inves-
tigated.
Hemp fiber reinforced unsaturated polyester compos-
ites were subjected to low velocity impact tests in order
to study the effects of non-woven hemp fiber reinforce-
ment on their impact properties [477,478]. The composite
specimen containing 0, 0.06, 0.10, 0.15, 0.21 and 0.26
fiber volume fractions (Vf ) were prepared and their impact
responses were compared with samples containing an
equivalent fiber volume fraction of chopped strand mat
E-glass fiber reinforcement. A significant improvement in
the load bearing capability and impact energy absorption
was found after the introduction hemp fiber as reinforce-
ment. The results indicated a clear correlation between
fiber volume fractions, stiffness of the composite lami-
nate, impact load and total absorbed energy. Unreinforced
unsaturated polyester control specimens exhibited brittle
fracture behavior with a lower peak load, lower impact
energy and less time until failure occurred than hemp rein-
forced unsaturated polyester composites. The impact test
results showed that the total energy absorbed by 0.21 fiber
volume fraction (four layers) of hemp reinforced specimens
is comparable to the energy absorbed by the equivalent
fiber volume fraction of chopped strand mat E-glass fiber
reinforced unsaturated polyester composite specimens.
The effects of the bi-dimensional orientation of leaf stalk
fibers from peach palms (peach palm powder and weave)
on the impact strength behavior of polyester/fiber rein-
forced composites were studied [479]. The Izod impact data
obtained for the composites with only woven material was
considerably superior to that of composites containing only
powder, suggesting that the reinforcement in the form of
powder is inefficient, independent of the size range of the
particles used.
The impact strength of the bamboo fiber/PLA com-
posites decreased after addition of bamboo fiber [480].
The impact strength of treated fiber reinforced compos-
ites improved after the addition of treated fibers. Good
fiber/matrix adhesion provides an effective resistance
to crack propagation during impact tests. The impact
strength increased significantly (33%) for silane treated
bamboo fiber/PLA composites compared to untreated bam-
boo fiber/PLA composites with 30 wt% fiber content.
The toughness of the short fiber reinforced composites
can be influenced by a number of factors, such as the intrin-
sic properties of the matrix, the fiber volume fraction, and
interfacial bond strength. Therefore, strong interactions
between the hydroxyl groups of biofibers and the coupling
agents are needed to overcome the incompatibility prob-
lem. In doing so, the impact, tensile and flexural strengths
of biofiber reinforced composites can be increased.
6.4. Summary
Tensile, flexural and impact properties are the most
commonly investigated mechanical properties of natu-
ral fiber reinforced plastic composites. Impact strength
is one of the undesirable weak points of these materi-
als in terms of mechanical performance. Besides these
tensile, flexural and impact properties, the long-term per-
formance (creep behavior), dynamic mechanical behavior,
compressive properties are also investigated for natural
fiber composites. To improve performance to the desired
level, still much work is to be done considering fiber pro-
cessing, non-linear behavior, fiber–matrix adhesion, fiber
dispersion, composite manufacturing with optimized pro-
cessing parameters.
7. Development and future trends of biocomposites
The advanced natural fiber reinforced polymer com-
posite contributes to enhancing the development of
 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
biocomposites in regards of performance and sustainabil-
ity. Biocomposites have created substantial commercial
markets for value-added products especially in automo-
tive sector. However, in order to be able to expand into
other markets, such as commercial construction and con-
sumer goods, composites need to achieve high-quality
performance, serviceability, durability, and reliability
standards.
In recent years, the major advancement lies within the
establishment of nanotechnology (i.e., reinforcing as well
as producing nanocrystalline cellulose from natural fibers).
Natural fibers consist of approximately 30–40% cellulose
and about half of that is crystalline cellulose. The nanocrys-
talline cellulose may be only one-tenth as strong as carbon
nanotubes but it costs 50–1000 times less to produce.
Wood pulp has often been used as the starting material
for research on nano cellulose production. In the literature
there are reports of cellulose nano/microfibril extraction
from diverse non-wood sources including hemp fibers
[481,482], sugar beet pulp [483,484], potato pulp [485],
swede root [486], bagasse [487–491], sisal [492,493], algae
[494], stems of cacti [495,496], banana rachis [497], flax
fibers [498,499], plantain [500], water hyacinth [501], bam-
boo [502], coir [503], pea hull [504], pineapple leaf [505],
and wheat straw [506].
Alemdar and Sain investigated the reinforcing poten-
tial of composites comprising a starch-based thermoplastic
polymer and cellulose nanofibers obtained from agro-
residues [507]. Cellulose nanofibers were isolated from
wheat straw by a chemi-mechanical technique and deter-
mined to have diameters in the range of 10–80 nm and
lengths of several thousand nanometers. Fig. 24 shows
the structure of the wheat straw fibers after the chem-
ical treatment. These images visually suggest the partial
removal of hemicelluloses, lignin and pectin after chemi-
cal treatment, which are the cementing materials around
the fiber-bundles. It is clear from the image that the aver-
age diameter of the fibers is about 10–15 ␮m, which is
lower than the average size of the fiber bundles, 25–125 ␮m
before chemical treatment. TEM image (Fig. 24b) for the
nanofibers obtained after the chemi-mechanical treat-
ment. The mechanical treatment of the fibers resulted in
defibrillation of nanofibers from the cell walls and the
TEM image of the nanofibers shows the separation of these
nanofibers from the micro-sized fibers.
Alemdar and Sain [508] extracted MFC from wheat
straw and soy hulls via mechanical treatment involving
cryocrushing followed by disintegration and fibrillation.
These authors found that almost 60% of the nanofibers
had a diameter within a range of 30–40 nm and lengths
of several thousand nanometers. Cryocrushing is an alter-
native method for producing nanofibers in which fibers are
frozen using liquid nitrogen and high shear forces are then
applied. When high impact forces are applied to the frozen
fibers, ice crystals exert pressure on the cell walls, caus-
ing them to rupture and thereby liberating microfibrils.
The cryocrushed fibers may then be dispersed uniformly
into water suspension using a disintegrator before high-
pressure fibrillation.
A blend containing 10% cellulose nanofibers obtained
from various sources, such as flax bast fibers, hemp fibers,
1583
kraft pulp or rutabaga and 90% poly(vinyl alcohol) was
used for making nanofiber reinforced composite material
by a solution casting procedure [509]. Both tensile strength
and Young’s modulus were improved compared to neat
PVOH film, with a pronounced four- to five-fold increase
in Young’s modulus observed.
Similarly, Wang and Sain [510,511] reported that soy-
bean stock-based nanofiber-reinforced PVOH films (up to
10% nanofiber content) demonstrated a two-fold increase
in tensile strength when compared with films without
filler. With a higher loading of MFC, the relative enhance-
ment of mechanical properties was even more remarkable.
They also applied solid phase melt-mixing followed by
compression molding to produce MFC-reinforced compos-
ites. In their study nanofiber was directly incorporated (up
to 5 wt%) into PE and PP matrix using a Brabender mixer and
an ethylene-acrylic oligomer emulsion was used as a dis-
persant. This work demonstrated that coating MFC fibers
with the dispersant improved the cellulose dispersion in
these polymers. As a consequence, the mechanical proper-
ties of PP and PE nanocomposites were slightly improved
when compared to pure matrices; however, this enhance-
ment was not considered significant.
Sain and Bhatnagar [512] invented a method to obtain
MFC from renewable feedstocks such as natural fibers and
root crops via cryocrushing of the pre-treated pulp with
liquid nitrogen. The pulp was hydrolyzed at a moderate
temperature of 50–90 ◦ C and then both acidic and alkali
extractions were performed.
Taniguchi [513] utilized natural cellulose fibers derived
from different sources (such as cotton, hemp, wood pulp,
seaweed, cereals, sea squirts, bacteria, etc.) for the produc-
tion of MFC by fibrillating raw materials between rotating
twin disks while adding shear stress in the vertical direc-
tion of fiber long axes. Joseph et al. [514–516] investigated
the effect of microfibrilation of oil palm fiber on the
dynamic mechanical properties of oil palm fiber reinforced
rubber composites.
As technology improves for biocomposites reinforced
with natural fibers to provide enhanced material and prod-
uct characteristics, the products will become more diverse
and enter markets that as of yet are unexplored. Today nat-
ural fiber reinforced biocomposites are found extensively
in automotive sectors [517–521].
By the time, biocomposite materials and associated
design methods are sufficiently mature to allow their
widespread use, issues related to construction materials.
The development of methods, systems and standards could
see biocomposite materials at a distinct advantage over
traditional materials. There is a significant research effort
underway to develop biocomposite materials and explore
their use as construction materials, especially for load bear-
ing applications.
Burgueno et al. manufactured cellular beams and
plates as load bearing structural components from hemp,
jute and flax fibers with unsaturated polyester resin
[522–525] for housing panel applications. The material
and structural performance was experimentally assessed
and compared with results from short-fiber compos-
ite micro-mechanics models and sandwich analyses. It
was demonstrated that cellular biocomposite components
1584 O. Faruk et al. / Progress in Polymer Science 37 (2012) 1552–1596
Fig. 24. SEM images of the wheat straw microfibers (a), and TEM image (magnification 15,000×) of the wheat straw nanofibers (b).
Adopted from [507]. Copyright 2008. By permission from Elsevier Ltd.
can be used for load-bearing components by improving
their structural efficiency through cellular material
arrangements. Furthermore, it was verified that they
could compete with components made from conventional
materials. This research should continue in conjunction
with development of conventional composite materials in
order to provide a solution in the future to allow wider
use of the bio composite materials by civil engineering
applications.
In the future, these biocomposites will see increased
use in structural applications. Various other applications
depend on their further improvements. But there are still
a number of problems that have to be solved before
biocomposites become fully competitive with synthetic
fiber composites. Biocomposites are sustainable and could
be fully recyclable, but could be more expensive if fully
bio-based and biodegradable and they are extremely sen-
sitive to moisture and temperature. If a proper matrix
is used, biocomposites could be 100% biodegradable, but
their biodegradation can difficult to control. Biocomposites
exhibit good specific properties, but there is high variabil-
ity in their properties. Biocomposites showed non-linear
mechanical behavior, poor long-term performance and low
impact strength. Many of these weaknesses can and will be
overcome with the development of more advanced pro-
cessing of natural fibers and their composites. However
fully environmental superiority of biocomposites com-
pared to synthetic fiber composites is still questionable
because of their relatively excessive processing require-
ments, which in turn consume more energy. Therefore,
careful life-cycle assessment of biocomposites is essen-
tial in order to retain the main advantage in the process
of developing high performance biocomposites. New mar-
kets will develop when these biocomposite products are
more durable, dimensionally stable, moisture proof, and
fire resistant.
Nanotechnology shows numerous opportunities
for improving biocomposite products by providing
nanotechnology-based coatings to increase water uptake,
reduce biodegradation and volatile organic compounds
and even flame resistance. The use of nanocrystalline
cellulose is being explored for a variety of uses since it is
stronger than steel and stiffer than aluminum. Nanocrys-
talline cellulose reinforced composites could soon provide
advanced performance, durability, value, service-life, and
utility while at the same time being a fully sustainable
technology.
8. Conclusions
Biocomposites reinforced with natural fibers and/or
biopolymers have developed significantly over the past
years because of their significant processing advantages,
biodegradability, low cost, low relative density, high spe-
cific strength and renewable nature. These composites are
predestined to find more and more application in the near
future, especially in Europe, where pressure from both
legislation and the public is rising. Interfacial adhesion
between natural fibers and matrix will remain the key issue
in terms of overall performance, since it dictates the final
properties of the composites. Many studies are examined,
reviewed and highlighted in this review paper regarding
the importance of the interface, the influence of various
types of surface modifications, different types of matrices
used for the composites, as well as fabrication methods,
and the performance of composites.
Further research is required to overcome obstacles
such as moisture absorption, inadequate toughness, and
reduced long-term stability for outdoor applications. In
particular, different weathering conditions, such as tem-
perature, humidity, and UV radiation all affect the service
life of the product. The major detrimental effect of
hygrothermal and UV exposure are property deterioration,
discoloring and deformation.
Significant research is currently underway around the
world to address and overcome the obstacles mentioned
above. This effort to develop biocomposite materials with
improved performance for global applications is an ongo-
ing process.
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