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Pyrolysis Mechanisms of Biomass

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A. Demirbas
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Sila Science, Trabzon, Turkey

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Pyrolysis Mechanisms of Biomass Materials

A. DEMIRBAS1
1
Sila Science, Trabzon, Turkey

Abstract Pyrolysis is degradation of biomass by heat in the absence of oxygen which

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results in the production of liquid, gaseous, and solid products. Conversion of biomass
materials composed predominantly of holocellulose and lignin using pyrolysis type
reactions represents a promising option for the production of fuels and chemicals. The
hemicelluloses degrade first at temperatures of 470 to 530 K and cellulose follows
in the temperature range of 510 to 620 K, with lignin being the last component to
pyrolyse at temperatures of 550 to 770 K. If the purpose is to maximize the yield of
liquid products resulting from biomass pyrolysis, a low temperature, high heating rate,
short gas residence time process would be required. If the purpose were to maximize
the yield of fuel gas resulting from pyrolysis, a high temperature, low heating rate,
long gas residence time process would be preferred. For a high char production, a low
temperature, low heating rate process would be chosen. Pyrolysis of lignocellulosic
biomass materials has been found to be a promising method for producing pyrolytic
oils also known as bio-oil.

Keywords biomass, pyrolysis, pyrolysis mechanism, thermal degradation

Introduction
The term biomass (Greek, bio, life C maza or mass) refers to wood, short-rotation
woody crops, agricultural wastes, short-rotation herbaceous species, wood wastes, bagasse,
industrial residues, waste paper, municipal solid waste, sawdust, bio-solids, grass, waste
from food processing, aquatic plants and algae animal wastes, and a host of other
materials. Biomass is the name given to all of the earths living matter. Biomass, as the
solar energy stored in chemical form in plant and animal materials, is among the most
precious and versatile resources on earth. It is a rather simple term for all organic materials
that originates from plants, trees, crops, and algae. The components of biomass include
cellulose, hemicelluloses, lignin, extractives, lipids, proteins, simple sugars, starches,
water, hydrocarbons, ash, and other compounds. Two larger carbohydrate categories that
have significant value are cellulose and hemicelluloses (holocellulose). The lignin fraction
consists of non-sugar type molecules.
Wood, woody, and other forms of biomass are some of the main renewable solid
energy resources available, and they provide the only source of liquid, gaseous, and solid
fuels (Bridgwater et al., 1999). Biomass is the only combustible renewable energy source
that yields liquid, gaseous, and solid fuels (Bridgwater and Peacocke, 2000) and has
been described as the renewable energy source with the highest potential to contribute to
the energy needs of modern society (Bridgwater, 2003). One technique used to convert
biomass into valuable liquid derivatives, also known as bio-oil, is pyrolysis. The resulting

Address correspondence to Professor Ayhan Demirbas, P. K. 216, TR-61035 Trabzon, Turkey.

E-mail: ayhandemirbas@hotmail.com

1186
 Pyrolysis Mechanisms of Biomass Materials 1187

bio-oil can then be used as fuel or for the production of chemicals and other bio-based
products (Maher and Bressler, 2007). Pyrolysis of lignocellulosic biomass materials has
been found to be a promising method for producing pyrolytic oils also known as bio-oil
(Demirbas, 2000a). Biomass is the only organic petroleum substitute which is renewable
(Garg and Datta, 1998; Demirbas, 2004).
Depending on the operation conditions, pyrolysis processes can be divided into
three subclasses: conventional pyrolysis, fast pyrolysis, and flash pyrolysis. Yields of
products obtained from biomass pyrolysis depend mainly on the chemical composition
of the feedstock and the operating temperature (Ceylan and B-son Bredenberg, 1982).
In the absence of oxygen, the thermal stability is in the order: lignin, cellulose, and
hemicelluloses (Demirbas, 2000a).
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Pyrolysis of Biomass Materials

Pyrolysis is the thermal decomposition of materials in the absence of oxygen or when
significantly less oxygen is present than required for complete combustion. Pyrolysis is
the basic thermochemical process for converting biomass to a more useful fuel. Biomass
is heated in the absence of oxygen, or partially combusted in a limited oxygen supply,
to produce a hydrocarbon-rich gas mixture, an oil-like liquid, and a carbon-rich solid
residue.
Pyrolysis dates back to at least ancient Egyptian times, when tar for caulking boats
and certain embalming agents were made by pyrolysis. In the 1980s, researchers found
that the pyrolysis liquid yield could be increased using fast pyrolysis where a biomass
feedstock is heated at a rapid rate and the vapors produced are also condensed rapidly
(Mohan et al., 2006).
In wood derived pyrolysis oil, specific oxygenated compounds are present in
relatively large amounts (Rowell and Hokanson, 1979; Phillips et al., 1990; Mohan
et al., 2006). A current comprehensive review focuses on the recent developments in the
wood/biomass pyrolysis and reports the characteristics of the resulting bio-oils, which
are the main products of fast wood pyrolysis (Mohan et al., 2006). Sufficient hydrogen
added to the synthesis gas to convert all of the biomass carbon into methanol carbon
would more than double the methanol produced from the same biomass base (Phillips
et al., 1990).
Rapid heating and rapid quenching produced the intermediate pyrolysis liquid prod-
ucts, which condense before further reactions break down higher molecular-weight species
into gaseous products. High reaction rates minimize char formation. Under some con-
ditions, no char is formed (Demirbas, 2005). At higher fast pyrolysis temperatures, the
major product is gas. Many researchers have attempted to exploit the complex degradation
mechanisms by conducting pyrolysis in unusual environments (Mohan et al., 2006). The
main pyrolysis variants are listed in Table 1.
Pyrolysis is the simplest and almost certainly the oldest method of processing one
fuel in order to produce a better one. Pyrolysis can also be carried out in the presence
of a small quantity of oxygen (gasification), water (steam gasification), or hydrogen
(hydrogenation). One of the most useful products is methane, which is a suitable fuel
for electricity generation using high-efficiency gas turbines.
Cellulose and hemicelluloses form mainly volatile products on heating due to the
thermal cleavage of the sugar units. The lignin forms mainly char since it is not readily
cleaved to lower molecular weight fragments. The progressive increase in the pyrolysis
temperature of the wood led to the release of the volatiles thus forming a solid residue that
 1188 A. Demirbas

Table 1
Pyrolysis methods and their variants

Residence Temperature, Heating

Method time K rate Products

Carbonation Days 675 Very low Charcoal

Conventional 530 min 875 Low Oil, gas, char
Fast 0.55 s 925 Very high Bio-oil
Flash-liquida <1 s <925 High Bio-oil
Flash-gasb <1 s <925 High Chemicals, gas
Hydro-pyrolysisc <10 s <775 High Bio-oil
Methano-pyrolysisd <10 s >975 High Chemicals
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Ultra pyrolysise <0.5 s 1,275 Very high Chemicals, gas

Vacuum pyrolysis 230 s 675 Medium Bio-oil
a Flash-liquid: Liquid obtained from flash pyrolysis accomplished in a time of <1 s.
b Flash-gas: Gaseous material obtained from flash pyrolysis within a time of <1 s.
c Hydropyrolysis: Pyrolysis with water.
d Methanopyrolysis: Pyrolysis with methanol.
e Ultra pyrolysis: Pyrolyses with very high degradation rate.

is different chemically from the original starting material (Demirbas, 2000b). Cellulose
and hemicelluloses initially break into compounds of lower molecular weight. This forms
an activated cellulose which decomposes by two competitive reactions: one forming
volatiles (anhydrosugars) and the other char and gases. The thermal degradation of the
activated cellulose and hemicelluloses to form volatiles and char can be divided into
categories depending on the reaction temperature. Within a fire all of these reactions take
place concurrently and consecutively. Gaseous emissions are predominantly a product of
pyrolitic cracking of the fuel. If flames are present, fire temperatures are high, and more
oxygen is available from thermally induced convection.
The biomass pyrolysis is attractive because solid biomass and wastes can be readily
converted into liquid products. These liquids, as crude bio-oil or slurry of charcoal of
water or oil, have advantages in transport, storage, combustion, retrofitting, and flexibility
in production and marketing.
The pyrolysis of biomass is a thermal treatment that results in the production of
charcoal, liquid, and gaseous products. Among the liquid products, methanol is one of
the most valuable products. The liquid fraction of the pyrolysis products consists of two
phases: an aqueous phase containing a wide variety of organo-oxygen compounds of
low molecular weight and a non-aqueous phase containing insoluble organics of high
molecular weight. This phase is called tar and is the product of greatest interest. The
ratios of acetic acid, methanol, and acetone of the aqueous phase were higher than those
of the non-aqueous phase. The point where the cost of producing energy from fossil
fuels exceeds the cost of biomass fuels has been reached. With a few exceptions, energy
from fossil fuels will cost more money than the same amount of energy supplied through
biomass conversion (Demirbas, 2007).
The kinematic viscosity of bio-oil varies from as low as 11 mm2 /s to as high as
115 mm2 /s at 313 K depending on the nature of the feedstock, temperature of pyrolysis
process, thermal degradation degree and catalytic cracking, the water content of the
 Pyrolysis Mechanisms of Biomass Materials 1189

bio-oil, the amount of light ends that have collected, and the pyrolysis process used.
The bio-oils have water contents of typically 1530 wt% of the oil mass, which cannot
be removed by conventional methods like distillation. Phase separation may partially
occur above certain water contents. The water content of bio-oils contributes to their low
energy density, lowers the flame temperature of the oils, leads to ignition difficulties,
and, when preheating the oil, can lead to premature evaporation of the oil and resultant
injection difficulties. The higher heating value (HHV) of pyrolysis oils is below 26 MJ/kg
(compared to 4245 MJ/kg for conventional petroleum fuel oils). In contrast to petroleum
oils, which are nonpolar and in which water is insoluble, bio-oils are highly polar and
can readily absorb over 35% water (Demirbas, 2007).
The bio-oil from wood is typically a liquid, almost black through dark red brown.
The density of the liquid is about 1,200 kg/m3 , which is higher than that of fuel oil and
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significantly higher than that of the original biomass. The bio-oils have water contents of
typically 1433 wt%, which cannot be removed by conventional methods like distillation.
Phase separation may occur above certain water contents. The HHV is below 27 MJ/kg
(compared to 4346 MJ/kg for conventional fuel oils).
The bio-oil formed at 725 K contained high concentrations of compounds
such as acetic acid, 1-hydroxy-2-butanone, 1-hydroxy-2-propanone, methanol, 2,6-
dimethoxyphenol, 4-methyl-2,6-dimetoxyphenol, and 2-cyclopenten-1-one, etc. A sig-
nificant characteristic of the bio-oils was the high percentage of alkylated compounds
especially methyl derivatives. As the temperature increased, some of these compounds
were transformed via hydrolysis (Kuhlmann et al., 1994). The formation of unsaturated
compounds from biomass materials generally involves a variety of reaction pathways such
as dehydration, cyclization, Diels-Alder cycloaddition reactions, and ring rearrangement.
For example, 2,5-hexandione can undergo cyclization under hydrothermal conditions to
produce 3-methyl-2-cyclopenten-1-one with very high selectivity of up to 81% (An et al.,
1997).

Reaction Mechanisms of Biomass Prolysis

Pyrolysis mechanisms of biomass have been studied by many investigators (Domburg
et al., 1974; Adjaye et al., 1992; Demirbas, 2000a). According to the proposed mecha-
nism, the heat variations associated with the thermal degradation reactions may affect the
pyrolysis route. Experimental runs indicate several endothermic and/or exothermic peaks
for biomass pyrolysis (Stamm and Harris, 1953; Shafizadeh et al., 1976). According to
several researchers, cellulose pyrolysis is endothermic (Brown et al., 1952; Roberts and
Clough, 1963; Demirbas and Kucuk, 1994), but lignin pyrolysis is exothermic (Demirbas
et al., 1996).
The general changes that occur during pyrolysis are enumerated below (Babu and
Chaurasia, 2003; Mohan et al., 2006):

1. Heat transfer from a heat source increases the temperature inside the fuel.
2. The initiation of primary pyrolysis reactions at this higher temperature releases
volatiles and forms char.
3. The flow of hot volatiles toward cooler solids results in heat transfer between hot
volatiles and cooler unpyrolyzed fuel.
4. Condensation of some of the volatiles in the cooler parts of the fuel, followed by
secondary reactions, can produce tar.
 1190 A. Demirbas

5. Autocatalytic secondary pyrolysis reactions proceed while primary pyrolytic re-

actions simultaneously occur in competition.
6. Further thermal decomposition, reforming, water gas shift reactions, radicals
recombination, and dehydrations can also occur, which are a function of the
processs residence time/temperature/pressure profile.

The mechanism of pyrolysis reactions of structural components of biomass (hemi-

celluloses, cellulose, and lignin) was extensively discussed in an earlier study (Demirbas,
2000a).
A process has been investigated for the saccharification of wood, involving prehy-
drolysis, lignocellulose pyrolysis, and tar hydrolysis. In this process, ground wood was
first prehydrolyzed to remove the more readily hydrolyzable hemicelluloses. The residual
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lignocellulose was then pyrolyzed rapidly to provide a tar containing levoglucosan and
its condensation products. The destructive reaction of cellulose is started at temperatures
lower than 325 K and is characterized by a decreasing polymerization degree. Thermal
degradation of cellulose proceeds through two types of reaction: a gradual degradation,
decomposition, and charring on heating at lower temperatures, and a rapid volatilization
accompanied by the formation of levoglucosan on pyrolysis at higher temperatures. The
glucose chains in cellulose are first cleaved to glucose and from this, in a second stage,
glucosan is formed by the splitting off of one molecule of water. Since cellulose and
levoglucosan have the same elementary formula, C6 H10 O5 , a yield of 100% of the latter
might be expected. The initial degradation reactions include depolymerization, hydrolysis,
oxidation, dehydration, and decarboxylation (Shafizadeh and Stevenson, 1982).
The hemicelluloses reacted more readily than cellulose during heating (Roni et al.,
2002). The thermal degradation of hemicelluloses begins above 373 K during heating for
48 h; hemicelluloses and lignin are depolymerized by steaming at a high temperature for
a short time (Shafizadeh et al., 1976).
Lignin is broken down by extensive cleavage of b-aryl ether linkages during steaming
of wood under 488 K (March, 1977). It has been found that on analysis of the methoxyl
groups after isothermal heating of dry distilled wood, lignin decomposition begins at about
550 K with a maximum rate occurring between 625 K and 725 K and the completion of
the reaction occurs at 725 K and 775 K (Sandermann and Augustin, 1963).
The formation of char from lignin under mild reaction conditions is a result of
the breaking of the relatively weak bonds, like the alkyl-aryl ether bond(s), and the
consequent formation of more resistant condensed structures, as has already been noted
(Domburg et al., 1974). One additional parameter, which may also have an effect on the
char formation, is the moisture content of the kraft lignin used.
Water is formed by dehydration. In the pyrolysis reactions, methanol arises from
the breakdown of methyl esters and/or ethers from decomposition of pectin-like plant
materials (Goldstein, 1981). Methanol also arises from methoxyl groups of uronic acid
(Demirbas and Gll, 1998). Acetic acid is formed in the thermal decomposition of all
three main components of wood. When the yield of acetic acid originating from the
cellulose, hemicelluloses, and lignin is taken into account, the total is considerably less
than the yield from the wood itself (Wenzl et al., 1970). Acetic acid comes from the
elimination of acetyl groups originally linked to the xylose unit.
If wood is completely pyrolyzed, resulting products are about what would be expected
by pyrolyzing the three major components separately. The hemicelluloses would break
down first, at temperatures of 470 K to 530 K. Cellulose follows in the temperature
range 510 K to 620 K, with lignin being the last component to pyrolyze at temper-
 Pyrolysis Mechanisms of Biomass Materials 1191

atures of 550 K to 770 K. A wide spectrum of organic substances was contained in

the pyrolytic liquid fractions given in the literature (Beaumont, 1985). Degradation
of xylan yields eight main products: water, methanol, formic, acetic and propionic
acids, 1-hydroxy-2-propanone, 1-hydroxy-2-butanone, and 2-furfuraldeyde. The methoxy
phenol concentration decreased with increasing temperature, while phenols and alkylated
phenols increased. The formation of both methoxy phenol and acetic acid was possible as
a result of the Diels-Alder cycloaddition of a conjugated diene and unsaturated furanone
or butyrolactone.
Timell (1967) described the chemical structure of the xylan as the 4-methyl-3-
acetylglucoronoxylan. It has been reported that the first runs in the pyrolysis of the
pyroligneous acid consist of about 50% methanol, 18% acetone, 7% esters, 6% aldehydes,
0.5% ethyl alcohol, 18.5% water, and small amounts of furfural (Demirbas, 2000a).
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Pyroligneous acids disappear in high-temperature pyrolysis.

The composition of the water soluble products was not ascertained but it has been
reported to be composed of hydrolysis and oxidation products of glucose such as acetic
acid, acetone, simple alcohols, aldehydes, sugars, etc. (Sasaki et al., 1998).

Conclusion
Bio-oil from biomass pyrolysis mainly consisted of aromatic, aliphatic, and naphthenic
hydrocarbons and oxygenated compounds such as phenols, furans, alcohols, acids, ethers,
aldehydes, and ketones.
The organic compounds from biomass pyrolysis are the following main groups:

1. A gas fraction containing: CO, CO2 , some hydrocarbons, and H2 .

2. A condensable fraction containing: H2 O and low molecular weight organic com-
pounds (aldehydes, acids, ketones, and alcohols).
3. A tar fraction containing: higher molecular weight sugar residues, furan deriva-
tives, phenolic compounds and airborne particles of tar, and charred material
which form the smoke.

The kinematic viscosity of bio-oil varies from as low as 11 mm2 /s to as high as

115 mm2 /s at 313 K depending on nature of the feedstock, temperature of pyrolysis
process, thermal degradation degree and catalytic cracking, the water content of the bio-
oil, the amount of light ends that have collected, and the pyrolysis process used. The
bio-oil viscosity and chemical composition were found to change substantially over time
probably due to polymerization of some components. Upon storage, the concentration of
aromatic hydrocarbons and phenols decreased while the concentration of aldehydes and
ketones increased (Adjaye et al., 1992).

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