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Universitatea Tehnică „Gheorghe Asachi” din Iaşi
Tomul LV (LIX), Fasc. 2, 2009
Secţia
CHIMIE ŞI INGINERIE CHIMICĂ
1.Introduction
The use of composite materials started many centuries ago with vegetal
fibers. In ancient Egypt, 3 000 years ago, clay was reinforced by straw to build
walls and houses. During the 1960s, the rise of composite materials began when
glass fibers in combination with resins was produced on a large scale. In the last
decade there has been a renewed interest in the natural fiber as substitutes for
synthetic fibers, motivated by potential advantages of weight saving, lower raw
material price, and the ecological advantages of using resources which are
renewable.
86 Dan Gavrilescu, Bogdan Marian Tofănică, Adrian Cătălin Puiţel and Puiu Petrea
fibers, they resist in alkaline solutions. Vegetable fibers resist at the action of
most organic acids but they are destroyed by strong mineral acids.
Vegetal fibers are divided in wood fibers and nonwood (annual) plant
fibers. Both these fibers are widely used for industrial applications: textile
industry, paper manufacturing, packaging, composite materials. A widely
accepted classification of vegetal fibers is presented in Figure 3, [3].
There are four major types of nonwood fibers: seed fibers, which are
the soft hairs that surround the seeds of certain plants; bast fibers, the tough
fibers that grow between the bark and stem of many dicotyledonous plants;
vascular fibers, the tough fibers found in the leaves and stems of
monocotyledons; and grass-stem fibers. Other fiber types, of limited utility,
include strips of leaf skins, such as raffia; the fiber of fruit cases, such as coir;
and palm fibers. Wood fibers originate from softwood or hardwood species.
Fiber reinforced composites use both annual plant fibers and fibers
isolated from wood. Nonwood fiber component may be sisal, hemp, coconut,
cotton, kenaf, flax, jute, abaca, banana leaf fibers, bamboo, wheat straw or other
fibrous material.
Pulping is the process of converting wood and nonwood vegetal
materials to separate vegetal fibers. Pulping processes differ from purely
mechanical, in which the wood is ground into fibers by disk refiners or
grindstones, to chemical, in which the fibers are separated by chemically
degrading and dissolving of lignin that binds fibers them together. The common
commercial pulps can be grouped into two large classes: mechanical pulps and
chemical pulps. Mechanical pulping process use grinding for logs and disc
refiners for chips. In these processes, mechanical shear forces are used to break
the fibers. In mechanical pulps, majority of the lignin remains within the fibers
and for this reason these fibers are stiffer [4].
Chemical pulp manufacturing is a process where vegetable material is
cooked in association with appropriate chemicals aiming to dissolve lignin. The
Bul. Inst. Polit. Iasi, t. LV (LIX), f. 2, 2009 89
main commercial chemical pulping techniques comprise sulfate (or kraft), and
sulfite. The dissolution of lignin during pulping is characteristic for each
pulping process, which is reflected in residual lignin content, carbohydrate yield
and composition.
Table 2
Fiber dimensions of representative wood species
Wood species Fiber dimensions, mm
Fiber length Fiber width
Softwoods 2-4 0.02-0.04
Hardwoods 0.7-1.7 0.15-0.04
90 Dan Gavrilescu, Bogdan Marian Tofănică, Adrian Cătălin Puiţel and Puiu Petrea
Table 4.
Annual dry matter and pulp yields of various fiber plants.
Dry Matter yield Pulp yield
Plant species
(t/ha) (t/ha)
Wheat straw 2.5 1.1
Rye straw 2.2 1.1
Rice straw 3 1.2
Common reed 9 4.3
Reed canary grass 6 3
Hemp 12 6.7
Bamboo 4 1.6
Miscantus 12 4.2
Bagasse 9 4.2
Kenaf 15 6.5
Softwood (coniferous) 1.5 0.7
Hardwood (birch) 3.4 1.7
plants contain more pentosans (over 20%), holocellulose (over 70%) and less
lignin (about 15%) as compared with hardwoods. The low lignin content in
grasses and other annual plants lowers the requirement of chemicals for cooking
of these plants and for bleaching of pulps. Inorganic compounds are absolutely
necessary for plants growth and development but they are not wanted in pulping
and papermaking [17], ..., [19].
Carbohydrate portion of majority of plants is composed of cellulose and
hemicellulose polymers with minor amounts of other sugar polymers such as
starch and pectins. The combination of cellulose and hemicelluloses are called
holocellulose and usually accounts for 65–70 percent of the plant dry weight.
These polymers are made up of simple sugars, mainly, D-glucose, D-mannose,
D-galactose, D-xylose, L-arabinose, D-glucuronic acid, and lesser amounts of
other sugars such as L-rhamnose and D-fructose. These polymers are rich in
hydroxyl groups, which are responsible for moisture sorption through hydrogen
bonding [20].
Cellulose is the most abundant biopolymers in the nature since is the
main structural component of the vegetal cells and is the main structural
component that provides strength and stability to the plant cell walls and the
fiber. From the structural point of view, cellulose is a linear polymer, whose
basic unit is D-glucose that connects by means of a glycosidic bond in the
configuration β-(1-4) forming a cellobiose unit that is repeated exactly in the
polymeric chain. A number of cellulose macromolecules form cellulose
microfibrils. Cellulose macromolecules have a tendency to form intra crystalline
regions. Most plant-derived cellulose is highly crystalline and may contain as
much as 80% crystalline regions.
Table 5.
Chemical composition of common plant species [16].
Chemical composition (%)
Plant species
Cellulose Lignin Pentosans Inorganic Silica
Cotton 85-96 0.7-1.6 1-3 0.8-2 -
Wheat straw 29-51 16-21 26-32 4.5-9 3-7
Rye straw 33-50 16-19 27-30 2-5 0.5-4
Rice straw 28-48 12-16 23-28 15-20 9-14
Common reed 44-46 22-24 20 3 2
Jute 41-48 21-24 18-22 0.8 -
Hemp 57-77 9-13 14-17 0.8 -
Bamboo 26-43 21-31 15-26 1.7-5 0.7
Bagasse 32-48 19-24 27-32 1.5-5 0.7-3.5
Kenaf 44-57 15-19 22-23 2-5 -
Softwoods 40-45 26-34 7-14 <1 -
Hardwoods 38-49 23-30 19-26 <1 -
The remaining portion has a lower packing density and is referred to as
amorphous cellulose [21]. Table 5 shows the average cellulose contents for a
Bul. Inst. Polit. Iasi, t. LV (LIX), f. 2, 2009 93
wide variety of plant types. On a dry weight basis, most plants consist of
approximately 45-50% cellulose. Cellulose content can vary from almost 90%
for cotton, to about 30% for rice straw or bamboo. The amount of cellulose in a
plant influences the properties of fibers, economics of fiber production and the
utility of the fibers for various applications. Fibers having higher cellulose
content would be preferable for composites, textile, paper and other fibrous
applications [22].
Hemicelluloses are heterogeneous polysaccharides constituted by
monosaccharides units including pentoses (xylose and arabinose), hexoses
(glucose, manose and galactose) and uronic acids, connected by glycosidic
bonds, forming graft and generally amorphous structures. Some hemicelluloses
are associated to the cellulose fraction, whereas others are associate to the
lignin. They first act like support for cellulose microfibrills in the cell wall, and
are of smaller molecular mass, more accessible, more degradable and easier to
dissolve than the cellulose [16]. Mechanically, hemicelluloses contribute little
to the stiffness and strength of fibers or individual cells. Hemicelluloses are
easily hydrolyzed into sugars and therefore fibers containing a higher proportion
of hemicelluloses would be preferable for producing sugars, chemicals and
eventually for car-fuels such as ethanol [21]. Pentosans represent the fraction of
the hemicelluloses consisting of monosaccharides containing five carbon,
mainly D-xylose and L-arabinose. Identification of this fraction in a plant
material indicates its potential utilization for producing furan-type chemicals
[20].
Lignin is an aromatic polymer formed by condensation of some
phenolic precursors. Lignin is an amorphous and highly branched aromatic
polymer. The function of lignin in plants is as an encrusting agent of the
cellulose/hemicelluloses matrix. It is often referred to be the plant cell wall
adhesive. Lignin provides plant tissue and individual fibers with compressive
strength and stiffens the cell wall of the fibers to protect the carbohydrates from
chemical and physical damage. Lignin is also associated with the
hemicelluloses, forming lignin-carbohydrate complexes that are resistant to
hydrolysis even under pulping conditions [23].
Extractives are a group of plant chemicals formed by lipophilic
compounds (mainly consisting of fats, fatty acids, fatty alcohols, terpenes, resin
acids, rosin, waxes, etc.) and phenolic compounds (phenols, steroids, etc.).
These chemicals exist as monomers, dimers and polymers. One of the main
functions of extractives compounds is the protection of plants against the
pathogens. The low degradability of many of these compounds contributes to
this aim, but also creates problems in some industrial uses of the vegetal
biomass, resulting in the formation of deposits, called pitch, during the
manufacture of paper pulp, [24].
The inorganic content of a plant usually refers to ash content, which is
an approximate measure of the mineral salts and other inorganic matter in the
94 Dan Gavrilescu, Bogdan Marian Tofănică, Adrian Cătălin Puiţel and Puiu Petrea
There are several physical properties that are important to know about
each non-wood plant fiber before that fiber can be used to reach its highest
potential. Fiber dimensions, strength and variability are the most important
properties. Major differences in fiber structure: fiber length and width, fiber
density, cell wall thickness, determine differences in physical properties.
Fiber length and width are very important for comparing different
species of agro-fibers. A high aspect ratio (length/width ratio) is essential in
fiber reinforced composites as it give an indication of possible strength
properties of the final product. In many cases, there is a wide variation in both
length and width of different fibers, [25]. The length and width of common
annual plant fibers and wood fibers are shown in Table 6.
Table 6
Length and width of selected annual plant fibers and wood fibers [16].
Ratio
Plant Fiber length (µm) Fiber width (µm)
length/
species
Average Range Average Range width
20000-
Cotton
30000 50000 20 12-30 1500:1
Wheat
straw 1400 400-3200 15 8-34 110:1
Rye straw 1400 600-3200 13 7-24 110:1
Rice straw 1400 400-3400 8 4-16 175:1
Common
reed 2000 1000-3000 16 10-20 75:1
Jute 2000 500-5000 20 10-25 100:1
5000-
Hemp
25000 55000 25 10-55 1000:1
1300- 135-
Bamboo
4000 500 - 9000 6-30 3-55 175:1
Bagasse 1700 800-2800 20 10-34 85:1
Kenaf 5000 2000-6000 21 14-33 135:1
Softwoods 3000 2700-3600 32 30-43 100:1
Hardwoods 1250 1000-1800 25 20-50 50:1
Bul. Inst. Polit. Iasi, t. LV (LIX), f. 2, 2009 95
Common fibers used in composites and their basic physical properties are presented in
Table 7. Vegetal fibers show low density but their mechanical properties are at the same
level as carbon or aramid fibers
Table 7
Common fibers used in composites and their basic properties [26]
Fiber Density, Elongation Tensile strength Young’s
(g/cm3) (%) (MPa) Modulus
(GPa)
Cotton 1.55 7.0-8.0 300-600 5.5-12.6
Jute 1.3 1.5-1.8 400-800 26.5
Flax 1.5 2.7-3.2 345-1035 69.3
Hemp 1.48 1.6 690 70
Ramie 1.5 3.6-3.8 100-938 61.4-128
Softwood kraft 1.5 - 1000 40
Viscose (cord) 1.52 11.4 593 11
Glass 2.5 2.5 2000-3500 70
Aramid 1.4 3.3-3.7 3000-3150 63-67
Carbon 1.4 1.4-1.8 4000 230-240
There are many advantages of vegetal fibers when are used as a composites
component:
- Low specific weight, which results in a higher specific strength and stiffness
than glass fibers;
- It is a renewable resource, the production requires little energy, CO2 is
sequestered while oxygen is given back to the environment;
- Producible with low investment at low cost, this makes the material an
interesting product for low-wage countries;
- Friendly processing - less problem regarding health and safety of workers, no
wear of tooling, no skin irritation;
- Thermal recycling is possible, where fibers glass causes problems in
combustion furnaces;
- Strong and flexible, good thermal and acoustic insulating properties;
- Good price-performance ratio
The primary advantages of using vegetal fibers as reinforcements in
composites can be divided as properties advantages and environmental and
socio-economic advantages. These advantages are listed in Table 8 [27]. It is
well known that specific gravity of vegetal fibers based composites is much
lower than the mineral filled composites. The density of natural fibers is in the
range of 1.25-1.5 g/cc compared with 2.54 g/cc for glass fibers and 1.8–2.1 g/cc
for carbon fibers. Specific gravity of a 50% (by weight) kenaf-polypropilene
composite is about 1.07, while that of a 40% (by weight) glass–polypropylene
composite is 1.23.
96 Dan Gavrilescu, Bogdan Marian Tofănică, Adrian Cătălin Puiţel and Puiu Petrea
Table 8
The primary advantages of using vegetal fibers as reinforcements in composites
Property Advantages Environmental and Socio-Economic
Advantages
Wide variety of fibers It is a renewable resource
Low specific weight Producible with low investment at low
High specific strength and stiffness cost
Non abrasive The production requires little energy
Unlike brittle fibers, the vegetal fibers will Biodegradable
not fracture when processing over sharp Generates rural jobs
curvatures. Non-food agricultural/farm based
Good thermal and acoustic insulating economy
properties Reducing the "greenhouse effect”: CO2
is used while oxygen is given back to the
environment
Easily recyclable
that will be considered by the plastics industry when evaluating these natural
fibers. In addition, agro-based fibers are less brittle and softer than glass fibers
and are likely to result in composites that are easier to recycle than mineral
based fibers.
5. Environmental impact
Table 9
Nonrenewable energy requirements for production of different fibers [34]
Nonrenewable energy requirements, MJ/kg
Glass fiber matt Flax fiber matt China reed fiber
Raw materials, 1.7 Seed production, 0.05 Cultivation, 2.50
Mixture, 1.0 Fertilizers, 1.0 Transport plant, 0.40
Transport, 1.6 Transport, 0.9 Fiber extraction, 0.08
Melting, 21.5 Cultivation, 2.0 Fiber grinding, 0.40
Spinning, 5.9 Fiber separation, 2.7 Transport fiber, 0.26
Mat production, 23.0 Mat production, 2.9
Total: 54.7 Total: 9.55 Total: 3.64
As can be seen from Table 10, glass fiber production needs 5-10 times
more energy than vegetal fiber production and as a result the pollutant
emissions from glass fiber production are much higher than from natural fiber
production. Table 12 compares the environmental impacts for producing
different types of fibers.
When fiber reinforced composite materials reach the end of their utility,
vegetal fibers are composted naturally by micro-organisms and the carbon
dioxide absorbed during the growth of the plant is released back into the
atmosphere. When vegetal fibers are incorporated into a composite material
with petroleum-based polymers, incineration is a likely end-of-life possibility.
In this case, the petrochemical component adds to the total atmospheric
emissions, including carbon dioxide formerly locked up in underground fossil-
fuel deposits. The combustion value of the petrochemical matrix and natural
fiber components combined can total as much as a quarter of the original energy
used in production [36].
With the increasing consumer market new products have been
introduced in order to replace material such as metals, cement and some
synthetic polymers that are very heavy, corrosive and less environment friendly.
In the past 30 – 40 years fiber composites have been competing with materials
such as steel, aluminum and concrete in cars, aircraft, buildings, bridges, and
many everyday goods. It has such a wide range of application due to its
possibility to combine high strength and stiffness with low weight it is non-
corrosive and less expensive in cost when compared to other materials. They are
also cheaper because they reduce the cost over the product’s lifetime as they
have very low maintenance costs. The most important thing is that vegetal
fibers composites are more suitable with sustainability concepts.
Bul. Inst. Polit. Iasi, t. LV (LIX), f. 2, 2009 101
6. Conclusions
1. There are many types of vegetal fibers that are divided in nonwood
plant fibers and wood fibers. Both these fibers are widely used for industrial
applications: textile industry, paper manufacture, packaging, composite
materials. In composites, vegetal fibers are used as reinforcement materials.
2. When vegetal fibers are used as composites component the main
advantages are: vegetal fibers are renewable, fibers are strong and flexible and
give less problem regarding health and safety of workers, they have good
thermal and acoustic properties, vegetal fibers show good price-performance
ratio. At the same time, the disadvantages of vegetal fibers are: dimension
instability, high moisture absorption, susceptibility to rotting, restricted
processing temperature.
3. Most important limitations of using vegetal fibers in composite
materials are: dimension instability, high moisture absorption, susceptibility to
rotting, restricted processing temperature. Vegetal fibers are also affected by
environmental temperature and humidity of the medium
4. Production of vegetal fibers results in less severe environmental
impacts compared with production of petroleum-base fibers or glass fibers.
Cultivation of vegetal fibers needs solar energy, and fiber production and
separation use low fossil fuels consumption. Synthetic fibers production is a
high energy process depending on non-renewable energy. Substitution of
synthetic fiber by natural fibers improves environmental impacts of composites
Acknowledgements
This work was financial supported by CNCSIS-UEFISCSU - Program IDEI, grant code
308/2008 “INTEGRATED STUDIES ON THE OBTAINING, BEHAVIOUR AND
ENVIRONMENTAL IMPACT OF SOME CELLULOSIC COMPOSITES ON RECYCLABLE
MATERIALS BASIS – ECO-COMPOZ”
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