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Materials Today: Proceedings 5 (2018) 2518–2526 www.materialstoday.com/proceedings

ICAMA 2016

Green Composites: A Review

Sharath Shekar H Sa, M. Ramachandra a*
a
Department of Mechanical Engineering, B.M.S.C.E, India

Abstract

Due to dwindling reserves of petroleum sources and their non-biodegradability, researchers are looking into alternatives for
synthetic fiber and resin system. Some of the techniques used to improve the performance of natural composites are successful,
they are still below the performance of synthetic fiber. In this paper we are going to look into some of the commercially used
natural fibers, natural resins, their mechanical properties and some of the techniques used for fiber strengthening. Chemical
treatment and mechanical loading methods are used to improve the strength of the natural fibers. The main advantage of using
natural fiber and resin system is it is cheaper than synthetic composites, bio-degradable, abundantly available. Natural Fiber-
reinforced polymer matrix composites have gained commercial success in the semi structural and structural applications such as
aircraft, automobiles, sporting goods, electronics, and appliances are quite dependent on natural fiber-reinforced plastics. By
using long, aligned natural fibers in conjunction with naturally derived resins, 100% bio-based composites with improved
mechanical properties can be achieved and can potentially be employed for more structural purposes

© 2017 Elsevier Ltd. All rights reserved.

Selection and Peer-review under responsibility of International Conference on Advanced Materials and Applications (ICAMA
2016).

Keywords: Green composites, Natural fibres, natural resin, bio degradable composites;

1. Introduction

When two are more physically and chemically different materials are combined with a distinct interface between the
materials to form a single substance it can be called as composite. The different materials are generally
differentiated as matrix phase and dispersed phase (reinforcement). The reinforcement is the load bearing member
whereas the matrix bonds the reinforcing material together and distributes the load among them. Both matrix and
reinforcement material have different properties, but when combined together gives a material with superior
properties than the parent materials [1].

* Sharath Shekar H S. Tel.:+91-9481354520;

E-mail address: shekarsharath16@gmail.com

2214-7853 © 2017 Elsevier Ltd. All rights reserved.

Selection and Peer-review under responsibility of International Conference on Advanced Materials and Applications (ICAMA 2016).
 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526 2519

Composites are of different types. They can be majorly classified on the basis of matrix as
a) Metal matrix composites
b) Ceramics matrix composites
c) Polymer matrix composites

Among the above mentioned the polymer matrix composites is of greater interest to researchers due to its light
weight, high stiffness, high strength and ease of fabrication. In polymer matrix composites the matrix is a polymer
substance, generally hydro-carbon based. The reinforcement material will be synthetic fibres, generally glass or
carbon fibres. These polymers are replacing the metals in most of the engineering fields like automobile, aerospace,
sports equipment and so on [2].

The synthetic polymer composites are basically petroleum based products. With growing awareness of
petrochemical resources and its limited reserves and to reduce the carbon footprint researchers are looking for
alternatives to replace the petroleum based composites [3]. Some of the major problems associated with the
synthetic polymers are

a) Generation of huge plastic waste and its disposal as it is non-biodegradable.

b) The fabrication of composites and also synthetic fibres is an energy intensive process as it requires a lot of heat
and pressure
c) The fact that the recycling methods for polymer composites are very underdeveloped
d) Limited reserves of petroleum[4]

Due to above mentioned reasons now researchers are looking at polymers synthesised by sustainable and eco-
friendly raw materials that are generally more abundant. This led to use of natural fibres and matrices for fabrication
of polymer composites. Researches show that the energy involved in production of natural fibres is more than half
of the energy needed for the synthesis of synthetic fibres. The advantages of natural fibres include light in weight,
non-abrasive, non-irritating, combustible, non-toxic, and biodegradable to mention few [5].

The use of natural fibres as reinforcement material can be dated back to nearly 10,000 years back. The use of plant
fibres as reinforcement material can be seen in construction of bricks during the time of Pharaoh. Henry ford made
an entire automobile body out of hemp fibre [7].Natural fibres have good acoustic and thermal insulation properties.
Natural fibres can be used for construction of structural panels and sandwich beams for housing projects. The scope
of natural fibres as construction materials is enormous due to their high performance in terms of durability,
maintenance and cost effectiveness.

2. Green composites.

The polymer composites made of natural fibres and bio-polymers is called as Green composites. Some of the natural
fibres are coir, flax, sisal, hemp etc. Examples of bio-polymers are starch, Poly lactic acid (PLA), CNSL, furan etc.

2.1. Natural Fibres

Natural fibres can be broadly classified into cellulose based; protein based and mineral based [6].
Fig.1 shows classification of natural fibres
2520 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526

Fig. 1: Classification of natural fibres. [Courtesy: University of arts, London]

The cellulose based fibres can be further classified according to their origin into: leaf, bast, seed, stalk and grass.
Fibres from bast, stem and leaf are naturally organised into bundles and are therefore called fibre bundles whereas
fibres from seed are single cells and are referred to as fibres [7].Natural fibres are mainly made of three principal
components; cellulose, lignin and hemicellulose. Cellulose is the major component which is responsible for the
inherent strength and stability of the natural fibre whereas hemicellulose contributes to the structure of the natural
fibre. Generally in rural areas the natural fibres are used extensively for non-structural application such as rope, bag,
broom and furniture. The fibres are also used for roofing and insulation. The fibres are coarse in texture and have
white to dark brown colour [8].

Some of the extensively used fibres are mentioned below:

2.1.1 Bamboo
Bamboo is the fast growing grass found in monsoon climates. Having high inherent strength and temperature
stability, especially coupled with coupling agents, bamboo fibres are used to make furniture, automobile interiors
and surf board.
2.1.2 Coir
Coir fibre is extracted from the husk and outer shell of the coconut and as a result considered as a seed derived
fibre. Coir is relatively water resistant and resistant to salt water damage. If the fibre is harvested when the coconut
is green, produces a smooth, fine pliable white fibre, whereas if extracted when fully matured produces brown strong
but less flexible fibre.
2.1.3 Flax
Flax is one of the oldest fibre crop in the world. Flax fibres can be easily woven into different types of fabric,
which are then used to create composites with different properties. Flax is economical eco-friendly and as per some
studies can rival to synthetic fibres.
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2.1.4 Hemp
Hemp is an extract from cannabis family of plant. Hemp fibres are mainly used in textile manufacturing as well as
paper industry. In early centuries hemp fibres were used to manufacture all the ships canvas sails, rigging, nets and
caulk because of its strength and resistance to salt water [9].
2.1.5 Jute
Jute is one of the cheapest fibres produced in high volume in India, Bangladesh and china. The specific modulus
of jute fibre approaches that of the glass fibre and it remains stable up to a temperature of 200oC without any damage
to its properties.
2.1.6 Bagasse
Bagasse fibre is obtained from the remains of squeezed sugarcane and has been used as a combustible material by
sugarcane industry, in pulp by paper industry [10].

Tabel 1: Physical properties of some plant fibers.[courtesy: 12]

Types of fibres Fibres Density(g/cm3) Elongation (%) Tensile strength (MPa) Young modulus
(GPa)
Stem fibres Bamboo 0.6-0.91 1.4 193-600 20.6-46.0
Flax 1.5 1.2-3.2 345-2000 15-80
Hemp 1.48 1.6 550-900 26-80
Jute 1.3 1.16-1.5 393-800 13-55
Kenaf 1.45 1.6 157-930 22.1-60
Ramie 1.5 1.2-3.8 400-938 61.4-128
Leaf fibres Banana 0.72.0.88 2.0-3.34 161.8-789.3 7.6-9.4
Pineapple 1.07 2.2 126.6 4.4
Sisal 1.5 3.0-7.0 468-700 9.4-22
Fruit fibres Coir 1.2 17-47 175 4.0-6.0
Oil palm 0.7-1.55 4-18 50-400 0.57-9.0
Wood fibres Softwood
Kraft (spruce) 1.5 - 1000 18-40
Hardwood
Kraft (brich) 1.2 - - 37.9

Synthetic fibres E-glass 2.5 2.5 2000-3500 70

S-glass 2.5 2.8 4570 86
Aramide 1.4 3.3-3.7 3000-3150 63.0-67.0

2.2 Fibre Extraction Process

Decortication and retting techniques are usually employed to separate fibres bundles from the leaf and bast of
fibre plants. A decorticator is a machine used to strip fibre bundles from the stem or leaf. Leaves are crushed and
beaten by a rotating wheel set with blunt knives so that only the fibres remain. The other parts of the leaf are washed
away by water. Decorticated fibres are then washed before drying on the sun or using hot air. The dry fibres are
combed and sorted into various grades

Retting is defined as ‘the subjection of crop or deseeded straw to chemical or biological treatment to make the
fibre bundles more easily separable from the woody part of the stem to facilitate the removal of fibre bundles. There
are two traditional types of retting namely dew and water retting. Dew retting entails leaving the plant stem in the
field to rot. In this process retting is constantly monitored to ensure that bast fibres separate from the core without
much deterioration in quality. Dew retting is the most popular in Europe although it is heavily dependent on the
geographical location, produces coarser and lower quality fibres than those produced using water retting technique.
Water retting entails the soaking of stems in water (ponds or tanks and slow moving rivers).
2522 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526

Water retting may require large amount of clean water and therefore expensive but results in high quality fibres
and produces environmentally unacceptable fermentation waste.

2.3 Pre-treatment
Pre-treatment of natural fibres using chemical methods (for instance, use of coupling agent such as silane
compound enhances the adhesion at the fibre-matrix interface and reduces moisture sorption of natural fibres. The
chemical treatment of fibres also helps in improving mechanical properties under both controlled and environmental
aging conditions [11].
2.3.1 Physical modification
Physical modification has always been done by using some instruments to change the structural and surface
properties of the fibres with the aims of increasing the strength of fibres. The hydrophobicity of the fibres thereby
influences the mechanical bonding with the matrix. The traditional methods involve thermo treatment, calendaring,
and stretching. Thermo treatment is the useful way to modify the natural fibres in the traditional method. When
fibres are subjected to heat treatment much above the glass transition temperature of lignin, it is postulated that
lignin will be softened and migrate to the fibre surface. According to the report by Cunha et al, Kraft lignin is having
a glass transition temperature at 142 °C. Lignin begins to degrade at around 214°C, hence heating the fibres to 200
°C would be expected to cause some softening. Surface modification by discharge treatment, such as low-
temperature plasma, sputtering, and corona discharge, is of great interest in relation to the improvement in functional
properties of natural fibres. The sputter etching brings about mainly physical changes, such as surface roughness,
and this leads to increase in adhesion. Longer treatment time, leading to rougher surface, results in better surface
wettability and dye ability. It has been found that the plasma treatment can reduce the strength of fibres. Baltazar-y-
Jimenez et al found that the strength of fibres (hemp, flax and sisal) decreases significantly with the increase the time
of plasma treatment [12].
2.3.2 Chemical modification
Chemical modification utilizes chemical agents to modify the surface of fibres or the whole fibres throughout.
The modification can be classed in five methods: mercerization, oxidation, crosslink, grafting and coupling agent
treatment
Mercerization is an old method of cellulose fibre modification which is an alkaline treatment of cellulose fibres.
The process was devised in 1844 by John Mercer of Great Harwood, Lancashire, England, who treated cotton fibres
with sodium hydroxide. This treatment caused the fibres to swell; about 25% of hydrogen bonds are broken during
the swelling process, in the post-treatment (drying). These bonds will re-bond and the following effects of the re-
bond have been reported in the literature: (i) decreasing the spiral angle of the micro-fibrils and increasing the
molecular direction; (ii) producing fibre fibrillation, i.e., axial splitting of the elementary fibres (or microfibers) that
constitute the elementary fibre. This process leads to a decrease in fibre diameter, increasing the aspect ratio and the
effective surface area available for wetting by a matrix in a composite. There is also an increase in fibre density as a
consequence of the collapse of its cellular structure; (iii) changing the fine structure of the native cellulose I to
cellulose II. These changes may result in improvement in fibre strength and hence stronger composite materials.
Oxidation modification can be done under mild condition, in this case carboxyl groups, aldehyde group and
ketone group can be introduced in the cellulose chains by the selective oxidation of primary or secondary hydroxyl
group in the cellulose chains. In 1938, Yackel and Kenyon firstly employed NO2 as oxidant to oxidise cellulose
selectively [12].
2.4 Biopolymers
Polymers from renewable resources can be classified into three major groups: natural polymers such as starch and
cellulose; synthetic polymers from natural monomers such as poly-lactic acid (PLA); polymers from microbial
fermentation such as poly-hydroxy-butyrate (PHB). Polylactic acid is one of the most promising biodegradable
polymers, which can be derived from natural feedstock such as corn starch but can also be derived from rice,
 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526 2523

potatoes, sugar beet and other agricultural waste. PLA synthesis involves conversion of the raw material feedstock
into dextrose, which then undergoes conversion into lactic acid or lactide via a fermentation process in the presence
of a catalyst. The lactide undergoes further processing in order to purify the monomer and this is followed by
conversion of the purified monomer in into a polymeric form of PLA through polymerisation in the presence of a
suitable catalyst.
2.4.1 Poly-L-lactic acid
Poly-L-lactic acid has received much attention, this biodegradable polymer is widely available and has a
relatively high melting point (160°C) allowing processing conditions similar to those employed for polypropylene.
PLLA also has relatively high mechanical properties. In tests with 70% kenaf fibre in PLLA the strength at failure
was three times higher than in PLLA. This showed a strong anisotropic effect, however further tests using a laminate
with fibre oriented in four principal directions (0°, 45°, 90° and 135°) showed a great improvement.
2.4.2 Starch
Starch is a complex polymer comprising a mixture of amylose and amylo-pectin polysaccharides. The properties
of starch will vary according to the amylose/Amylo-pectin ratio and hence according to the plant source. A major
source of starch is corn but it can also be extracted from potato, wheat and rice. The polymer is crystalline due to the
presence of the amylo-pectin component. The two main disadvantages of starch are its water-solubility and poor
mechanical properties. Hence, this polymer is suited to applications where long term durability is not needed and
where rapid degradation is advantageous. It is often processed as foam where it provides an alternative to
polystyrene for use in the manufacture in food trays, moulded shaped parts or as loose packing filler.
2.4.3 Polyesters
This group includes poly-hydroxyalkanoates and poly (alkylene dicarboxylates) and are produced synthetically by
condensation reactions between dicarboxylic acids and diols. PLA in particular shows potential as a structural
material since it can be polymerized to a high molecular weight and is hydrophobic, yet vapour permeable. The latter
properties render the polymer sufficient lifetime to maintain mechanical competence without rapid hydrolysis, whilst
maintaining good composting capability, provided always that industrial, not domestic, composting techniques are
employed. Current uses for this polymer group centre on medical applications such as implants, sutures, drug
delivery systems and grafts.
2.4.4 Cellulose acetate
Cellulose acetate is a modified polysaccharide which can be prepared from a reaction between acid anhydride and
cellulosic products derived from cotton linters, wood pulp, recycled paper or sugar cane. The manufacturing process
for cellulose acetate was first patented at the end of the nineteenth century and the polymer found use in filaments,
films and lacquers since that time. This biodegradable polymer exhibits good toughness and a high degree of
transparency.
2.4.5 Furfural alcohol and furan resins
The pre-cursor to furfural alcohol and furan-based resins is furfural, a compound which is extracted from
naturally occurring agricultural residues. Residues may derive from sugar cane bargasse as well as corn cobs, wood
products or cereal by-products [13].
2.4.6 Bio based thermosetting resins
A large number of bio based thermosetting resins can be formed from vegetable oils – by grafting hydroxyl,
acrylate and maleate moieties or combinations of these onto the fatty acid triglyceride.
Other naturally derived resins can be formed from cashew nut shell liquid (CNSL) which is extracted from the
shell of cashew nuts as a by-product of the nut industry. The CNSL is rich in anarcardic acid, which is converted to
cardanol during the heated extraction process. Cardanol can be polymerised by free radical polymerisation, and
condensation polymerisation between phenolic units can occur in the presence of aldehydes.
2524 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526

2.4.7 Cashew nut shell liquid

Cashew nut shell liquid (CNSL) was originally a waste product of the cashew (Anacardium occidentale) nut
extraction process. A dark, viscous liquid obtained from a honeycomb-like structure in the cashew shell, it has
become a popular option for producing cheap, more eco-friendly resins [14]. In its raw form, CNSL consists of
mainly anacardic acid, with some cardanol and cardol –but once heated and distilled in order to decarboxylate the
anacardic acid, what remains is a technical grade CNSL consisting of mostly cardanol with a small amount of cardol
2.4.8 Cellulose
Cellulose is a structural compound found in plant matter and it can be obtained either in its basic form or
esterified from trees, cotton, sugarcane or even recycled paper. Examples of cellulose esters include cellulose acetate
(CA) and cellulose acetate butyrate (CAB). In order for cellulose acetate to be used as a resin, it is often plasticised
with an agent such as citrate plasticiser (CAP) to form an effective composite polymer matrix
2.4.9 Poly (butylene succinate)
Synthesised from 1,4-butanediol (BDO) and succinic acid, poly(butylene succinate) or PBS is a biodegradable
thermoplastic that is attracting a great deal of interest in the field of bio-composites. Due to its “wide temperature
window for thermoplastic processing”, PBS is suitable for extrusion, injection moulding, thermoforming and film
blowing.
2.5 Advantages of bio-polymer technology

(a) Reduction of petrol consumption

(b) Relative reduction of fossil fuel import dependence
I Reduction of greenhouse gas emission
(d) Reduction of discharge of polymer production-associated waste system
I Reduction of harmful solid waste deposition
(f) Increase in employment in agriculture sector (i.e. harvesting) [15].

2.6 Factors affecting strength of composite

Composite properties depend on the properties of the constituent materials i.e. the fibres and resins used. The
strength and stiffness of the composites are directly a function of the reinforcing fiber properties which carry most of
the load and their volume content [16]. The resin helps to maintain the relative position of the fibres within the
composite and, more importantly, transfers the load from the bottom fibres to the intact fibres. To fabricate high
strength composites, all three factors namely fiber properties, resin properties as well as fiber/resin interface
characteristics are critical [17].
Modification to the fibre also improves resistance to moisture induced degradation of the interface and the
composite properties. In addition, factors like processing conditions/techniques have significant influence on the
mechanical properties of fibre reinforced composites.
Properties vary depending on the quality of the harvest, age and body of the plant from which they are extracted,
the extraction techniques and the environmental conditions of the site.

3. Advantages
Composite products have good mechanical properties per unit weight, are durable and their technologies allow
the manufacture of complex and large shapes. They can be formed on site into complicated shapes and can also be
easily cut to length on site. These include wood fibres, jute, sisal, coconut, bamboo and banana leaves. Such fibres
could be added alone or in hybrid composites, in partial substitution for industrial fibres.
These fibres are renewable, non-abrasive to process equipment, and can be incinerated at the end of their life
cycle for energy recovery as they possess a good deal of calorific value. Plant fibres have the advantage over fossil-
based fibres due to the low density and high specific stiffness, low cost and renewable.
 Sharath Shekar H S & Ramachandra M / Materials Today: Proceedings 5 (2018) 2518–2526 2525

Plant fibres are also known to be carbon neutral thus environmentally friendly. Lower specific density of the
cellulose-based fibres leads to weight savings in composite manufacture with direct advantages on transportation.
The higher fibre volume fractions of plant fibres compared to those of the fossil fuel based reinforcements will result
in significant material cost savings as plant fibres are cheaper than the matrices.
4. Disadvantages
The use of NFRP composites has been restricted due to certain characteristics of the natural fibres such as
moisture absorption tendency, poor wettability, poor adhesion with the synthetic counterparts and low thermal
stability during processing. The mechanical properties of natural fibre reinforced composites deteriorate over a
period of time as fibres, fibre-matrix interface region and matrix is typically affected by the moisture. The degree of
deterioration and reversibility of the properties of the natural fibre composites is largely dependent on the extent of
moisture absorption. Low thermal stability, in other terms the possibility of degradation at moderate temperature
(230-250 ° C).

5. Applications
Although lacking the inherent strength provided by synthetic fibre composites in most cases, many bio-
composites are still useful in non-load bearing capacities; with applications such as in sports equipment, housing for
electronics, internal and external vehicle panelling and furniture.
Flax is widely considered the strongest mechanically. It is easily manipulated and shows properties comparable to
glass fibre when woven in optimum arrangements. Hard but lightweight, flax bio-composites may be used in wide
range of products. Of the bio-resins mentioned, those containing cashew nut shell liquid are perhaps the most
applicable to varied conditions.
Sisal fibre reinforced CNSL (cashew nut shell liquid) resin composites have been tested and had a mean strength
of 24.5 MPa and Young’s modulus of 8.8 GPa. Bending tests confirmed that these composites have adequate
strength to be used in roofing applications.
Plant Fibre Technology (a spinout company from the BioComposites Centre) has produced a range of natural
based construction products. One of which is the Isonat® insulation fibre, made from hemp grown on UK farms and
from waste cotton fibres. Isonat® contains 15% polyester fibres to give loft and stability. Isonat® can be harmlessly
disposed of by composting or incineration. The ability of Isonat® to absorb and release humidity actively assists the
control of moisture in buildings without any loss in thermal performance, and without affecting on the durability of
the insulation.

6. Conclusion

It is worth mentioning that fibrous materials are commonly subjected to the following deformations: tension,
compression, bending, torsion, shear, abrasion, wear and flexingPineapple fibre exhibits the highest specific strength
and specific modulus followed by flax fibre and hemp fibre respectively. This implies that the weight of pineapple,
flax and hemp fibres will be more suitable in composite manufacture due to the savings on weight economies over
the rest of the fibres. More importantly, the same fibres exhibit high stiffness which means that they can be used as
replacement for glass, carbon and high performance synthetic fibres such as Kevlar fibres in end uses where
requirements for extreme stiffness is not a prerequisite.

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