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An Overview of Biomass Pyrolysis

Ayhan Demirbas & Gönenç Arin

To cite this article: Ayhan Demirbas & Gönenç Arin (2002) An Overview of Biomass Pyrolysis,
Energy Sources, 24:5, 471-482, DOI: 10.1080/00908310252889979

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Energy Sources, 24:471–482, 2002
Copyright © 2002 Taylor & Francis
0090-8312 /02 $12.00 C .00

An Overview of Biomass Pyrolysis

AYHAN DEMÇIRBAŞ
P. K. 216
Trabzon, Turkey

GÖNENÇ ARIN
Gazi University
Department of Chemical Engineering
Ankara, Turkey

The pyrolysis is degradation of biomass by heat in the absence of oxygen, which

results in the production of charcoal, liquid, and gaseous products. The pyrolysis
process can be divided into three subclasses: conventional pyrolysis, fast pyrolysis,
and  ash pyrolysis. The hemicelluloses break down Ž rst at temperatures of 470 to
530 K, cellulose follows in the temperature range 510 to 620 K, and lignin is the last
component to pyrolyze 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. For a high
char production, a low temperature, low heating rate process would be chosen. If
the purpose was to maximize the yield of fuel gas resulting from pyrolysis, a high
temperature, low heating rate, long gas residence time process would be preferred.

Keywords pyrolysis, thermal degradation, biomass, fast pyrolysis,  ash pyrolysis

Wood, woody, and other forms of biomass are some of the main renewable solid en-
ergy resources available and provide the only source of liquid, gaseous, and solid fuels
(Bridgwater et al., 1999). Biomass potential includes wood and animal and plant wastes.
Biomass is the only organic petroleum substitute that is renewable. The term “biomass”
refers to forestry, purpose-grow n agricultural crops, trees and plants, and organic, agricul-
tural, agro-industrial, and domestic wastes (municipal and solid waste) (Garg and Datta,
1998). Biomass is the name given to the plant matter that is created by photosynthesis,
in which the sun’s energy converts water and CO2 into organic matter. Thus biomass
materials are directly or indirectly a result of plant growth. These include Ž rewood plan-
tations, agricultural residues, forestry residues, animal wastes, etc. Fossil fuels can also
be termed biomass, since they are the fossilized remains of plants that grew some mil-
lions of years ago. Biomass contributes to about 12% of today’s world primary energy
supply, while in many developing countries its contribution ranges from 40% to 50%.
The demand for energy is increasing at an exponential rate due to the exponential
growth of world population. This, combined with the widespread depletion of fossil fuels

Received 18 May 2001; accepted 9 July 2001.

Address correspondence to Prof. Ayhan Demirbaş, P. K. 216, TR-61035 Trabzon, Turkey.
E-mail: [email protected]

471
472 A. Demirbaş and G. Arõ n

and gradually emerging consciousness about environmental degradation, suggests that

the energy supply in the future has to come from renewable sources of energy. Statistics
show that total renewable energy now accounts for nearly 18% of global primary energy
supply, but out of this traditional biomass only about 30% account for over 55% by
large hydro. Solar, wind, modern biomass, geothermal, small hydro (below 10 MW), and
ocean energy all together account for only 12% of total renewable energy. The new and
renewable account for only 2% of world primary energy supplies. Biomass contributes to
about 12% of today’s world primary energy supply, while in many developing countries
its contribution ranges from 40% to 50% (Garg and Datta, 1998). Renewable energy
consumption was 8% of the total US energy consumption in 1997 (Table 1). Hydropower
and biomass continued to dominate the renewable energy market, most of the year-to-
year drop was due to a decrease in biomass energy consumption due to a warmer than
expected heating season.
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.
World production of biomass is estimated at 146 billion metric tons a year, mostly wild
plant growth. Some farm crops and trees can produce up to 20 metric tons per acre of
biomass a year. Types of algae and grasses may produce 50 metric tons per year (Cuff
and Young, 1980).
Energy can be obtained from biomass in 5 ways:
1. Production of crops that yield starch, such as sorghum; sugar, such as sugar cane;
cellulose, such as Eucalyptus trees; and oil, such as sun ower, Euphorbia, etc.
2. Solid waste that can be burned.
3. Anaerobic digesters that produce bio-gas that can be used to generate heat/elec-
tricity.
4. LandŽ ll. This is a very ancient technique whereby all the municipal waste and
refuse is accumulated in large ditches, valleys, or specially excavated holes in
the land and the bacteria and decomposing waste produces methane. The gas is
then tapped and used either in houses or in power stations. LandŽ ll gas is not
only used for electricity generation, but also for Ž ring brick kilns and to produce
steam in industry.

Table 1
US energy consumption by source (1997)

% of total energy % of renewable energy

Petroleum 38
Natural gas 24
Coal 23
Nuclear electric 7
Renewable energy 8
Hydroelectric 55
Biomass 38
Geothermal 5
Solar 1
Wind < 0.5
Source: Energy Information Administration (EIE), Annual Energy Review 1997.
 An Overview of Biomass Pyrolysis 473

Figure 1. A graph representation of the relative importance of petroleum, coal, and biomass as
industrial feedstocks for the 250 year period from 1825 to 2075.

5. Bio-fuel or bio-oil production, which includes ethanol, methanol, bio-diesel, and

their derivatives. Many countries nowadays have alcohol production plants and
utilize the alcohol directly in cars or partially mixed with petrol to upgrade the
octane level, or it may be used in power stations to generate electricity.
Ethanol is blended with gasoline in the ratio of 1:9 to produce the fuel gasohol.
Ethanol can also be used in fuel cells. The production of bio-diesel has also gone up
from 11,000 tons in 1991 to 1,286,000 tons in 1997. The raw materials are oils from
84% rapeseed, 13% sun ower, 1% soybean, 1% palm, and 1% others (Demirbaş, 2000a).
Cost of purpose-grow n biomass is still a major issue. The aims are to increase use
of residues while reducing costs (increasing yields) of biomass production, improve con-
version efŽ ciencies, and improve economics (competitiveness with fossil fuels). Figure 1
shows a graph representation of the relative importance of petroleum, coal, and biomass
as industrial feedstocks for the 250 year period from 1825 to 2075 (Gohean, 1981). The
importance of biomass as a chemical feedstock will increase and it will be a promising
source of raw materials in the future.

Pyrolysis Principles
Pyrolysis is thermal degradation of biomass by heat in the absence of oxygen, which
results in the production of charcoal (solid), bio-oil (liquid), and fuel gas products. The
474 A. Demirbaş and G. Arõ n

pyrolysis of biomass has been studied with the Ž nal objective of recovering a bio-fuel
with medium-low caloriŽ c power (Desrosiers and Lin, 1984; Hofmann and Antal, 1984;
Solantausta et al., 1993; Frederick et al., 1994; Raveendran and Ganesh, 1996; Font et al.,
1999; Odden and Barth, 2000). The main pyrolysis reaction is

Biomass ! Charcoal C Volatile matter

Depending on the operating conditions, the pyrolysis process can be divided into
3 subclasses: conventional pyrolysis (carbonization), fast pyrolysis, and  ash pyrolysis.
The range of the main operating parameters for pyrolysis processes are given in Table 2
(Maschio et al., 1992). At present, the preferred technology is fast or  ash pyrolysis at
high temperatures with very short residence times (Elliot et al., 1991).
Conventional pyrolysis is deŽ ned as the pyrolysis that occurs under a slow heating
rate. This condition permits the production of solid, liquid, and gaseous pyrolysis products
in signiŽ cant portions. The Ž rst stage of biomass decomposition, which occurred between
395 and 475 K, can be called prepyrolysis. During this stage, some internal rearrangement
such as water elimination, bond breakage, appearance of free radicals, and formation
of carbonyl, carboxyl, and hydroperoxid e groups takes place (ShaŽ zadeh, 1982). The
second stage of the solid decomposition corresponds to the main pyrolysis process. It
proceeds with a high rate and leads to the formation of the pyrolysis products. During
the third stage, the char decomposes at a very slow rate and carbon-rich residual solid
forms.
If the aim is the production of mainly liquid and/or gaseous products, a fast pyrolysis
is recommended. The products produced by fast pyrolysis are considered a marginal
product, as its yield does not exceed 17 wt%. The achievement of fast heating rates
requires high operating temperatures, very short contact times, and very Ž ne particles.
The qualitative and quantitative composition of the most volatile part of pyrolytic
oil from  ash pyrolysis was described (Beaumont, 1985). Flash pyrolysis differs strongly
from that of conventional pyrolysis performed slowly with massive pieces of wood.
Hydropyrolysis (pyrolysis in a hydrogen atmosphere) is also considered to have a
potential application in the conversion of biomass to liquids enriched in hydrocarbons
(Barth, 1999; Rocha et al., 1997).
Biomass is a mixture of structural constituents (hemicelluloses, cellulose, and lignin)
and minor amounts of extractives that each pyrolyze at different rates and by different
mechanisms and pathways. It is believed that as the reaction progresses the carbon be-
comes less reactive and forms stable chemical structures, and consequently the activation
energy increases as the conversion level of biomass increases (Tran and Charanjit, 1978).

Table 2
Range of the main operating parameters for pyrolysis processes

Conventional
pyrolysis Fast pyrolysis Flash pyrolysis

Pyrolysis temperature (K) 550–950 850–1250 1050–1300

Heating rate (K/s) 0.1–1 10–200 > 1000
Particle size (mm) 5–50 <1 < 0.2
Solid residence time (s) 450–550 0.5–10 < 0.5
 An Overview of Biomass Pyrolysis 475

Lignin decomposes over a wider temperature range compared to cellulose and hemi-
celluloses, which rapidly degrade over narrower temperature ranges, hence the apparent
thermal stability of lignin during pyrolysis (Bridgwater et al., 1999). Thermal degrada-
tion properties of hemicelluloses, cellulose, and lignin can be summarized as follows
(Chum, 1991):

Thermal degradation of hemicelluloses > of cellulose > of lignin

The rate and extent of degradation of each of these components depends on the process
parameters of reactor type, temperature, and particle size heating rates and pressure.
Thermal depolymerization and degradation of biomass, cellulose, hemicelluloses,
and products were formed as well as a solid residue of charcoal. The mechanism of the
pyrolytic degradation of structural components of the biomass samples were separately
studied (Demirbaş, 2000b). If wood is completely pyrolyzed, resulting products are about
what would be expected by pyrolyzing the 3 major components separately. The hemi-
celluloses break down Ž rst, at temperatures of 470 to 530 K, and cellulose follows in
the temperature range 510 to 620 K, with lignin being the last component to pyrolyze at
temperatures of 550 to 770 K (Demirbaş and Küçük, 1993).
The pyrolysis of lignin has been studied widely (Demirbaş, 2000b). Its pyrolysis
products, of which guaiacol is that chie y obtained from coniferous wood, and guaiacol
and pyrogallol dimethyl ether show the aromatic nature of lignin from deciduous woods.
Lignin gives higher yields of charcoal and tar from wood, although lignin has a threefold
higher methoxyl content than wood. Cleavage of the aromatic C¡O bond in lignin led to
the formation of one-oxygen atom products, and the cleavage of the methyl C¡O bond
to form two-oxygen atom products is the Ž rst reaction to occur in the thermolysis of
4-alkylguaiacol at 600–650 K. Cleavage of the side chain C¡C bond occurs between the
aromatic ring and ®-carbon atom.

Technological Considerations

Technical Assessment of Pyrolysis

The biomass distillation industry used pyrolytic reactors in a process called destructive
distillation. The operation was carried out in a fractionating column (a tall still) under
a high temperature (from 750 to 1350 K). Charcoal was the main fuel product, and
methanol production was about 1 to 2% of volume or 6 gallons per ton. The synthetic
process developed in 1927 (< biblio >) replaced this traditional method. The synthetic
process utilizes a pyrolytic reactor operating as a gasiŽ er by injecting air or pure oxygen
into the reactor core to completely burn the biomass to ash. The energy contained in
the biomass is released in the gasses formed. After puriŽ cation the syngas, hydrogen
and carbon monoxide in a 2 to 1 ratio, is altered by catalyst under high pressure and
temperature to form methanol. This method will produce 100 gallons of methanol per
ton of feed material (Rowell and Hokanson, 1979).
There are 3 main methods of achieving fast pyrolysis: (1) ablative pyrolysis, in which
biomass is pressed against a heated surface and rapidly moved during which the biomass
melts at the heated surface and leaves oil Ž lm behind which evaporates; (2)  uid bed and
circulating  uid bed pyrolysis, which transfer heat from a heat source to the biomass by a
mixture of conversion and conduction; and (3) vacuum pyrolysis, which has slow heating
rates but removes pyrolysis products as rapidly as in the preliquid product (Bridgwater
et al., 1999).
476 A. Demirbaş and G. Arõ n

Choice of Reactor Type

The main part of a pyrolysis plant is the reactor. The most common pyrolysis systems
employ the following types of reactor: rotary kiln, moving-bed with cocurrent or coun-
tercurrent  ow (in conventional pyrolysis), entrained bed,  uidized bed, multiple hearth,
or Ž xed-bed tubular reactor. Pyrolysis has received considerable creativity and innovation
in devising reactor systems that provide the essential ingredients of high heating rates,
moderate temperatures, and short vapor product residence times for liquids (Bridgwater
et al., 1999). The choice of the reactor type and heating systems affects the Ž nal product
distribution (Jones, 1987). If the raw material is available as powder or Ž ne particles,
then a fast pyrolysis in an entrained- or  uidized-bed reactor is recommended.
Pyrolysis can be used for the production of bio-oil if  ash pyrolysis processes are
used and it is currently at the pilot stage (Ramage and Scurlock, 1996). The conversion
of biomass to crude oil can have an efŽ ciency of up to 70% for  ash pyrolysis processes.
The so-called bio-crude can be used in engines and turbines. Its use as feedstock for
reŽ neries is also being considered. Some problems in the conversion process and use
of the oil need to be overcome; these include poor thermal stability and corrosivity of
the oil. Upgrading by lowering the oxygen content and removing alkalis by means of
hydrogenation and catalytic cracking of the oil may be required for certain applications
(Garg and Datta, 1998).

Figure 2. SimpliŽ ed experimental setting for biomass pyrolysis. (1) Biomass feeder, (2) pyrolysis
chamber, (3) electric furnace, (4) packing material, (5) condenser, (6) cold trap, (7) gas volume
measure, (8) tight gas tank, (9) sweeping gas stream, and (10) peristaltic pump.
 An Overview of Biomass Pyrolysis 477

Experimental Considerations
Pyrolysis is conceptually simple to perform. A simple experimental setting for biomass
pyrolysis is depicted in Figure 2. A thermogravimeter is used to obtain the effect of
heating rate on the pyrolysis rate in experimental runs. It is interesting to determine how
the heating rate affects the pyrolysis rate. Figure 3 shows typical thermograms (TGs)
obtained under varied heating rates from pyrolysis of beech wood powder.
The most interesting temperature range for the production of the pyrolysis products
is between 625 and 775 K. The charcoal yield decreases as the temperature increases.
The production of the liquid products has a maximum at temperatures between 625
and 725 K. At higher temperatures, the rather large molecules present in the liquid and
residual solid are broken down to produce smaller molecules, which enrich the gaseous
fraction (Maschio et al., 1992). The results of pyrolysis of solid waste and analysis of
the gas content are given in Table 3.
Pyrolysis of biomass has been studied as a zonal process, with zone A (easily de-
grading zone) occurring at temperatures up to 473 K. The surface of the biomass particle
becomes dehydrated at this temperature, and water vapor, carbon dioxide, formic acid,
acetic acid, and glyoxal are given off. When temperatures of 473 to 533 K are attained,
the wood is said to be in zone B and is evolving water vapor, carbon dioxide, formic acid,
acetic acid, glyoxal, and some carbon monoxide. The reactions up to this point are mostly

Figure 3. Effect of heating rate on pyrolysis rate: Thermograms from pyrolysis of beech wood
powder (Particle size: 250–400 mesh).
 Table 3
Results of pyrolysis of solid waste and analysis of the gas content

Temperature Char Liquid Gas CO2 O2 HC CO Others

(K) (wt%) (wt%) (wt%) (vol%) (vol%) (vol%) (vol%) (vol%)

478
507 97.0 0.0 3.0 22.1 0.6 32.5 13.8 31.0
584 76.2 15.9 7.9 18.9 3.9 32.9 18.2 26.1
655 62.9 25.4 11.7 34.5 0.4 21.4 10.6 33.1
683 49.0 35.0 16.0 45.1 4.6 20.9 9.4 19.7

Source: Küçük and Demirbaş (1997).

 An Overview of Biomass Pyrolysis 479

endothermic, the products are largely noncondensable, and the wood is becoming charred.
Pyrolysis actually begins between 535 and 775 K, which is called zone C. The reactions
are exothermic and unless heat is dissipated the temperature will rise rapidly. Combustible
gases such as carbon monoxide from cleaving of carbonyl group, methane, formaldehyde,
formic acid, acetic acid, methanol, and hydrogen are being liberated and charcoal is being
formed. The primary products are beginning to react with each other before they can
escape the reaction zone (Goldstein, 1991). If the temperature continues to rise above
775 K, a layer of charcoal will be formed that is the site of vigorous secondary reactions
and is classiŽ ed as zone D. Carbonization is said to be complete at temperatures of 675
to 875 K (Chum, 1991).
The liquid fraction of the pyrolysis products consists of 2 phases: an aqueous phase
containing a wide variety of organo-oxyge n compounds of low molecular weight and a
nonaqueous phase containing insoluble organics (mainly aromatics) of high molecular
weight. This phase is called bio-oil or tar and is the product of greatest interest. The ratios
of acetic acid, methanol, and acetone in the aqueous phase were higher than those in the
nonaqueous phase. Table 4 shows the chemical analysis of organic substances contained
in the liquid fractions of pyrolysis products from deciduous woods at 725 K.
If the purpose was 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. For a high char production, a low temperature, low heating rate process
would be chosen. If the purpose was to maximize the yield of fuel gas resulting from
pyrolysis, a high temperature, low heating rate, long gas residence time process would
be preferred.

Table 4
Chemical analysis of organic subtances contained in the liquid fractions of
 ash pyrolysis products from beech wood at 725 K (wt% dry basis)

Substance Substance

Acetic acid 16.78 Ethanal 0.54

1-hydroxy-2-propanone 7.01 2,3-butanedione 0.54
Methanol 4.11 2,3-pentanedione 0.54
1-hydroxy-2-butanone 3.47 Valeric acid 0.54
Furfural 2.09 Isovaleric acid 0.54
2,6-dimethoxyphenol 1.97 5-methyl-furfural 0.33
Levoglucosan 1.89 Valerolactone 0.33
®-angelilactone 1.81 Butyric acid 0.33
4-methyl-2,6-dimetoxyphenol 1.81 Isobutyric acid 0.33
1-hydroxy-2-propan e acetate 0.86 Propanone 0.33
Guaiacol 0.82 Acrylic acid 0.33
1-hydroxy-2-butanon e acetate 0.67 2-butanone 0.33
Crotonic acid 0.66 Methyl acetate 0.21
Formic acid 0.66 Methyl-furyl-cetone 0.16
Butyrolactone 0.66 Crotonolactone 0.16
Crotonic acid 0.66 2-methyl-cyclopentenone 0.16
Propionic acid 0.59 Cyclopentenone 0.16

Source: Beaumont (1985).

 Table 5
Comparison of kinetic data from literature

Frequency factor Activation energy Temperature range

Biomass (min¡1 ) (kJ/mole) (K) Researcher

Douglas Ž r sawdust 1:1 ´ 1011 105 368–525 Stamm (1956)

480
Wood 1:4 ´ 106 84.2 > 605 Barooah and Long (1976)
Douglas Ž r bark 1:3 ´ 1010 100–201 450–850 Tran and Charanjit (1978)
Missouri oak sawdust 1:5 ´ 108 106 595–665 Thurner and Mann (1981)
Sawdust 1:9 ´ 107 95.9 565–665 Koullas et al. (1998)
Hazelnut shell sawdust 4:7 ´ 1013 92–170 450–750 Demirbaş (1998)
 An Overview of Biomass Pyrolysis 481

Kinetics for Pyrolysis

Earlier kinetic studies have been conducted under a variety of experimental conditions,
resulting in con icting data with a wide range of kinetic parameters (Stamm, 1956; Ba-
rooah and Long, 1976; Tran and Charanjit, 1978; Thurner and Mann, 1981; Hofmann
and Antal, 1984; Desrosiers and Lin, 1984; Demirbaş, 1998; Koullas et al., 1998). Ther-
mogravimetric analysis (TGA) is the general approach applied to determine the weight
loss of pyrolyzed samples at various reaction temperatures. Comparison of kinetic data
from literature is given in Table 5.
The enthalpy of pyrolysis of Whatman CF-11 cellulose is a function of mass loss
from the sample and its heating rate. The pyrolysis process is always initially endothermic
and almost linear in mass loss. At high heating rates, this character is maintained through-
out the process. At low heating rates, the well-known exothermic char forming processes
begin at some point to compete with the basic endothermic nature of the process and
drive it back toward thermoneutrality. There is, however, no evidence of thermodynami-
cally different pathways being followed at high and low heating rates during the initial
stages of pyrolysis. This alone does not assure that a change of mechanism does not
occur, but there is also no other evidence to suggest such a change in mechanism with
heating rate.
On the one hand there are the results characterized by activation energies in excess
of 200 kJ/mol which come from careful work, normally performed in TG type systems.
On the other hand, there are a number of reports of mass loss kinetics governed by
activation energies of about 140 kJ/mol seen in studies conducted at higher heating
rates than are conveniently examined in the TGA. The evidence strongly suggests that a
transport limitation is the explanation for this apparent discrepancy, but there are some
inconsistencies associated with an explanation based on heat transfer limitations. This
has led to a search for other plausible sources of transport limitations.

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