ARTICLE

pubs.acs.org/EF

CO2 Gasification Kinetics of Biomass Char Derived from

High-Temperature Rapid Pyrolysis
Shuai Yuan, Xue-li Chen,* Jun Li, and Fu-chen Wang
Key Laboratory of Coal Gasification of Ministry of Education, East China University of Science and Technology, Shanghai 200237,
People’s Republic of China

ABSTRACT: The char of three typical biomasses, rice straw char (RS char), chinar leaves char (CL char), and pine sawdust char
(PS char), was prepared in a high-frequency furnace, which could efficiently reduce secondary reactions under rapid pyrolysis
conditions at 800
1200 °C. The rapid pyrolysis char produced was isothermally gasified in a thermogravimetric analyzer (TGA)
under a CO2 atmosphere. Effects of biomass type and pyrolysis temperature on intrinsic carbon structures and morphologic
structures of char and further on gasification characteristics of char were investigated using a Raman spectrum analyzer, scanning
electron microscopy (SEM), and a surface area and pore size distribution analyzer. Gasification kinetic models were also
contrastively discussed under different conditions. Results show that gasification rates decrease with the increasing pyrolysis
temperature. Under the morphologic characteristic reserved conditions, morphologic structures present obvious effects on
gasification rates. Gasification reactivity of the three biomass chars is in the order of CL char > RS char > PS char. Melting and
shrinkage happen during rapid pyrolysis of PS, and the disappearance of the pore and decrease of the specific surface area of PS char
lead to the low specific surface area and gasification rates of PS char. Unobvious melting happens to RS char and CL char, and the
initial physical structures can be almost reserved, while CL char presents larger porosity and specific surface area, which make its
gasification rates higher than those of RS char. In most conditions, the random pore model (RPM) performs well to describe
gasification rates of biomass char studied in this work. However, for gasification of PS char at high temperatures, during which high
gasification rates can be maintained in high conversion ranges, the modified random pore model (M-RPM) performs better. For
gasification of RS char and CL char at low temperatures, during which gasification rates present a sharp decrease and trailing in
medium
high conversion ranges, the shifted M-RPM performs better.

1. INTRODUCTION literature. Rapid pyrolysis char of sawdust was prepared in a

Extensive attention has been attracted by biomass energy for
its advantages, including renewability, low pollution, wide dis-
tribution, etc. Efficient and clean use of biomass has become an
important research field. Pyrolysis, combustion, and gasification
are the main methods of biomass thermal conversions for
productions of gas, liquid, and solid products. Pyrolysis is not
only a biomass thermal conversion method but also an important
process of combustion and gasification.
Many studies focus on bio-oil production through med-
ium
low temperature rapid pyrolysis.1
10 However, some re-
searchers have found that high-quality syngas can be directly
produced through high-temperature rapid pyrolysis of biomass,
with the carbon conversions being high and the liquid yields
being low;11
15 therefore, it may also be an available method for
biomass use. Although carbon retained in char might be low after
rapid pyrolysis of biomass at high temperatures, this part of
carbon should also be used to increase the efficiency of biomass.
Gasification or co-gasification with coal might be good use
methods for this part of char. Therefore, research on gasification
characteristics of biomass char derived from rapid pyrolysis has
important significance.
Presently, gasification characteristics of char derived from
rapid pyrolysis at high temperatures have not been fully under-
stood. Pyrolysis conditions have important effects on gasification
characteristics, and high-temperature rapid pyrolysis char was
mostly prepared by the drop-tube furnace in the present
drop-tube furnace at 1000 and 1400 °C by Fermoso and
co-workers, and effects of the pyrolysis temperature, pressure,
and CO2 concentration on gasification characteristics were
investigated.16 Rapid pyrolysis of sawdust and bagasse was
carried out in a drop-tube furnace by Cetin and co-workers,
and effects of the pyrolysis temperature, heating rates, and
pressure on char structures and further on gasification character-
istics were investigated.17,18 A similar reactor was used by Biagini
and co-workers to prepare rapid pyrolsis char, and correlations
between gasification/combustion characteristics and char struc-
tures were discussed. However, the pyrolysis temperatures were
relatively low (400
800 °C).19 A fluidized-bed reactor20 and
wire-mesh reactor17,18 were also used to prepare rapid pyrolysis
char, while the pyrolysis temperatures were lower than 900 and
950 °C, respectively. Moreover, during pyrolysis in a drop-tube
furnace and fluidized-bed reactor, fuel samples were continu-
ously fed into the reactor; thus, there are gas-phase products that
remained in the reactors. Char derived from the later fed fuel
samples may react with CO2 and H2O in gas-phase products in
the reactor (called self-gasification).19 Diversities of gas velocity
and residence time may lead to the differences of char properties
and gasification characteristics.
Received: January 10, 2011
Revised: March 30, 2011
Published: March 30, 2011

r 2011 American Chemical Society 2314 dx.doi.org/10.1021/ef200051z | Energy Fuels 2011, 25, 2314–2321
Energy & Fuels ARTICLE

Table 1. Contents of Indigenous Elements in Fuel Samples

(ppm, dry basis)
K Na Ca Mg Si

RS 1584 101 603 196 3779

CL 688 59 1451 255 834
PS 51 15 1187 44 256

In addition, the random pore model (RPM) was found as the

most reliable model for describing biomass char gasification
characteristics. However, in some conditions, melting and plastic
deformations happen during pyrolysis of biomass,17,19,21 to-
gether with the catalysis effects of mineral matters, and gasifica-
tion characteristics may vary significantly. Therefore, whether
RPM could perform well on various biomass and pyrolysis
conditions is a worthy question to discuss.
In this study, a high-frequency furnace was used to carry out
rapid pyrolysis of biomass. The reactor could efficiently restrain
the secondary reactions between volatiles and char, and nascent
char without “self-gasification” conversion during pyrolysis could
be obtained. Particle morphological structures were reserved,
and effects of biomass type and pyrolysis temperature on
morphological structures and intrinsic carbon structures and
further on gasification characteristics were investigated. Applic-
ability of RPM was also discussed.

2. MATERIALS AND METHODS

2.1. Fuel Samples. Three typical agricultural and forestry wastes,
rice straw (RS), chinar leaves (CL), and pine sawdust (PS), were chosen
as the fuel samples. Compositions and particle sizes have been reported
in detail elsewhere.22 Contents of indigenous mineral elements (K, Na,
Ca, Mg, and Si) in biomass are listed in Table 1.
2.2. Experimental Setup. Rapid pyrolysis was carried out at
800
1200 °C and 1 atm. Morphological structures of char were
investigated by scanning electron microscopy (SEM, JSM-6360LV) at
15 kV. Intrinsic carbon structures of char were investigated by a Raman
spectrometer (IUVIA REFL). The contents of mineral elements in
biomass samples were detected by inductively coupled plasma
atomic
emission spectroscopy (ICP
AES, IRIS 1000). The contents of C in
char were analyzed in an elemental analyzer (Vario MACRO CHN/
CHNS). Surface areas and pore size distributions of the char were
analyzed by an automated surface area and pore size distribution
analyzer (Micromeritics ASAP-2020M). N2 adsorption isotherms at
77 K were measured for the relative pressure (P/P0) range from 0.01 to
0.99. Specific surface areas were obtained by the Brunauer

Emmett
Teller (BET) model, and the pore size distributions were
obtained by the Barrett
Joyner
Halenda (BJH) model. Gasification
experiments of char were carried out in a thermogravimetric analyzer
(TGA, CAHN D-110) at 1 atm. Biomass char was heated to the
gasification temperature in a N2 atmosphere, and then N2 (1 L/min)
was shifted to CO2 (1.2 L/min) for isothermal gasification. Pyrolysis
setup and operating conditions have been described in detail
elsewhere.22 The feeding time of the fuel sample was 1.5 min each time,
and the power supplier was shut down after 2 min when the injection of
fuel samples was finished. Because coking happened in some conditions
during pyrolysis of biomass, all of the char was crushed and char with a
particle size of 56
180 μm was gasified.
3. RESULTS AND DISCUSSION
3.1. Char Yields. Effects of the temperature on the yields of
char and char C during rapid pyrolysis of RS, CL, and PS are
2315
Figure 1. (a) Char yields (dry basis) and (b) char C yields during
biomass rapid pyrolysis at different temperatures.
shown in Figure 1. It can be found from Figure 1a that, as the
pyrolysis temperature increases, the char yields decrease gradu-
ally. Char yields from the three biomasses are in the order of
RS > CL > PS. Ash contents of the three biomasses express the
same order.22 During rapid pyrolysis of biomass under a high
temperature, char yields are low; thus, ash accounts for large
proportions of char. Therefore, ash contents in biomass may
affect their char yields to some extent.
The yields of char C were calculated by the following equation:
char C (%) = C in char (mg)/C in fuel (mg)  100%. The
equation denotes the proportion of carbon retained in char after
pyrolysis. It can be found from Figure 1b that the char C yields of
the three biomasses decrease with an increasing temperature. As
the temperature increases from 800 to 1200 °C, char C yields of
RS decrease from 28.4 to 16.0 wt % and char C yields of CL
decrease from 20.6 to 9.6 wt %. PS gives much lower char
C yields, which decrease from 6.8 wt % at 800 °C to 3.8 wt % at
1200 °C.
3.2. Effect of Char Structures on Gasification Character-
istics. Gasification rates of the biomass char produced at different
temperatures are shown in Figure 2. The gasification tempera-
ture ranges from 850 to 1050 °C. The gasification conversion
X and gasification rate r were calculated by the following func-
tions, respectively: X = (m0
mt)/(m0
mash) and r = dX/dt,
where m0 is the sample weight at the start of gasification, mt is the
sample weight at a gasification time of t, and mash is the weight of
ash remaining in char after being completely converted.
Gasification rates decrease with the increasing pyrolysis tem-
perature. The increase of the graphitization degree might be the
reason. Raman spectra of CL char derived from different
dx.doi.org/10.1021/ef200051z |Energy Fuels 2011, 25, 2314–2321
Energy & Fuels
Figure 2. Gasification rates of soybean cake char and fitting curves of RPM.
temperatures and Raman spectra of the three biomass chars
derived at 1000 °C are shown in panels a and b of Figure 3,
respectively. Two main peaks appear in the range of the Raman
shift between 800 and 2000 cm
1. The peak appearing at
approximate 1350 cm
1 is the D band, which is related to the
amorphous carbon structures. The peak appearing at approx-
imate 1580 cm
1 is the G band, which is related to the CdC
bonds of graphite crystals. The intensities of D and G bands can
be denoted by ID and IG, respectively. A valley appears between D
and G bands, and its intensity can be denoted by IV. Generally,
the G band becomes sharpened as the graphitization degree
increases. The uniformity of carbon structures can be reflected by
the IV/IG ratio, which decreases with the increasing uniformity of
carbon structures.23,24 It can be found from Figure 3a that both
ID and IG of CL char decrease with the increasing pyrolysis
temperature. IV/IG ratios of CL char at 800 °C, CL char at
1000 °C, and CL char at 1200 °C are 0.516, 0.512, and 0.494,
which decrease with the increasing pyrolysis temperature. It
proves that the uniformity of the biomass char increases with the
increasing pyrolysis temperature.
Under the same conditions, gasification rates of CL char are
found to be the highest, followed by those of the RS char, and
2316
ARTICLE
gasification rates of PS char are the lowest. IV/IG ratios of the
three biomass chars are 0.568 (RS char), 0.512 (CL char), and
0.550 (PS char). Thus, the uniformities of the three biomass
chars can be ordered as CL char > PS char > RS char. Generally,
the gasification rate decreases with the increasing uniformity.
However, it can be found from Figure 2b that gasification rates of
CL char are the highest, followed by those of RS char, and
gasification rates of PS char are the lowest. In other words, among
the three biomass chars, gasification rates have no obvious
correlations to their uniformities. Large diversities of morpholo-
gical structures of char derived from different biomasses might be
the reason.
Figure 4 shows the SEM graphs of the three biomass chars
derived from different temperatures. It can be found that initial
morphological structures of RS remained after pyrolysis at
800 °C. Slight destruction and melting happen as the tempera-
ture increases. In other words, morphological structures of RS
char are not seriously affected when the temperature increases
from 800 to 1200 °C. A similar phenomenon can be found from
those of CL char. Initial structures remained in CL char at
800 °C, and slight melting happens on CL char at 1000 °C and
CL char at 1200 °C. However, morphological structures of PS
dx.doi.org/10.1021/ef200051z |Energy Fuels 2011, 25, 2314–2321
Energy & Fuels ARTICLE

char are seriously affected by the increasing pyrolysis tempera-

ture. Slight deformations of the particle surface happen during
pyrolysis of PS at 800 °C. As the temperature increases to
1000 °C, melting happens to PS char. The melting phenomenon
becomes more serious when the temperature increases to
1200 °C.
BET specific surface areas and pore distributions of the
biomass char derived under different temperatures are shown
in Table 2 and Figure 5, respectively. Because only the pores
with diameters larger than 1.5 nm can contribute to the CO2
gasification reaction.25 Features of the pore structures
(1.7
200 nm) obtained from the N2 adsorption analysis can
reflect their effects on CO2 gasification characteristics. It can be
found that, as the pyrolysis temperature increases, specific
surface areas of the RS char increase gradually, specific surface
areas of CL char increase first and then decrease slightly, while
specific surface areas of the PS char decrease sharply. From the
comparisons of specific surface areas derived from different
biomass, it can be found that the specific surface areas of the CL
char are the highest, those of the RS char are lower, and specific

Table 2. BET Specific Surface Areas of the Biomass Char

(m2/g)
pyrolysis temperature (°C) RS CL PS

800 85.5 186.1 47.5

1000 102.6 239.3 13.1
Figure 3. Raman spectra of biomass char. 1200 133.9 225.3 8.9

Figure 4. SEM photographs of biomass char derived from different temperatures (1000).

2317 dx.doi.org/10.1021/ef200051z |Energy Fuels 2011, 25, 2314–2321

Energy & Fuels
Figure 5. Pore size distributions of the biomass char.
surface areas of the PS char are the lowest. As melting happens to
PS char, leading to the disappearance and decrease of the specific
surface area, gasification rates are sharply restrained. From
comparisons, it can be found that, although initial morphological
structures of both RS and CL are reserved after pyrolysis, CL
char presents a higher porosity and specific surface area than RS
char. It is the reason that gasification rates of CL char are higher
than those of RS char.
In the studies by Cetin and co-workers, melting of woody
samples was also found during rapid pyrolysis, while melting of
herbaceous samples was very slight and just some destruction
happened when the temperature was very high.17,18 Biagini and
co-workers consider that melting of cell structures and plastic
transformation are the reasons for the disappearance of pore
structures during rapid pyrolysis of biomass.19,21 However,
morphologic structures of PS char in this study are different
from those of PS char produced from a drop-tube furnace.17
Although melting also happened during rapid pyrolysis of PS in
the drop-tube furnace at 1000 °C, the cell structure with a high
inner porosity appeared in PS char. Differently, PS char at
1000 °C in this study as shown in Figure 4 presents a solid
structure with poor porosity. The reason might be that, during
rapid pyrolysis of PS in a drop-tube furnace, volatiles released
from inside of the molten char lead to the formation of bubbles
in char. However, the residence time of char in the drop-tube
furnace is short, and char can be quickly quenched when it
dropped into the char collector. Shrinkage of the molten char
can be stopped rapidly, and bubble structures can be reserved.
During rapid pyrolysis of PS in the high-frequency furnace of
2318
ARTICLE
this study, the residence time of PS char in the crucible is longer
than that of the drop-tube furnace, shrinkage of the molten char
happened after volatiles completely released, and the solid
structure can be formed.
In addition, large diversities of char coking characteristics
indicate that, although biomasses all constitute lignin, cellulose,
and hemicellulose, properties of the components vary with the
plants, especially for lignin and hemicellulose.26 It is also the
reason that pyrolysis products cannot be predicted just by the
additivity rule of products derived from pyrolysis of lignin,
cellulose, and hemicellulose separately.27
Indigenous mineral species in biomass may also play impor-
tant roles on the char gasification rates. During CO2 gasification
of biomass char, potassium (K) is the strongest catalyst, followed
by sodium (Na), the catalysis effect of calcium (Ca) is much
weaker, and magnesium (Mg) performs almost no catalysis
effect. Silicon (Si) has a strong inhibition effect on the gasification
reaction.28 It can be found from Table 1 that contents of the
mineral elements in PS are low, especially for K and Na, which
have strong catalysis. Therefore, the catalysis effects of mineral
elements on the gasification of PS char should be weak. Zhang
and co-workers found that, when the Si content is higher than
those of K and Na, the catalysis effects of K and Na can be
completely dismissed.28 It can be found from Table 1 that,
although the contents of K and Na in RS are 2.3 and 1.7 times
those of CL, respectively, the Si content of RS is much higher,
which is 4.5 times that of CL. Therefore, the high Si content in RS
dismisses the catalysis effects of K and Na and may also be one of
the reasons that gasification rates of RS are lower than CL.
dx.doi.org/10.1021/ef200051z |Energy Fuels 2011, 25, 2314–2321
Energy & Fuels
Figure 6. Arrhenius curves of biomass char gasification reactions: (a)
RS char, (b) CL char, and (c) PS char.
3.3. Gasification Kinetics of Char. RPM is the most success-
ful model to describe biomass char gasification rates. Its function
is r = dX/dt = K(1
X)(1
ψ ln(1
X))1/2, where K is the
reaction rate constant and ψ is a parameter of the particle
structure.29 Fitting results of RPM on gasification rates are
shown in the dotted lines of Figure 2. It can be found that
RPM performs well in most conditions. Taking gasification rates
at a conversion of 0.5 (r0.5) as the basis, ln r0.5 versus 1/T is
plotted in Figure 6. It can be found that linear correlations
appear between ln r0.5 and 1/T at a gasification temperature
lower than 950 °C in most conditions. As the temperature
further increases, ln r0.5 slopes to be lower to the straight line. In
the study by Fermoso and co-workers, a similar phenomenon
was found.16 They consider that the gasification reactions are
2319
ARTICLE
Table 3. Frequency Factors and Apparent Activation Energy
char at 800 °C char at 1000 °C char at 1200 °C
A0 Ea A0 Ea A0 Ea
(105 s
1) (kJ/mol) (105 s
1) (kJ/mol) (105 s
1) (kJ/mol)
RS 3.937  102 238.3 8.464 202.9 5.983 203.4
CL 0.359 159.7 2.306 179.7 4.798  101 215.7
PS 8.589  102 248.5 2.457  102 236.5 1.229  102 232.4
chemically controlled when the gasification temperature is not
very high. As the temperature increases to a high enough level,
gasification reactions will turn to the diffusion-controlled re-
gime. Therefore, the gasification reaction turned to the diffusion-
controlled regime at 950
1000 °C during gasification of biomass
in this study. Frequency factors, A0, and activation energy, Ea,
were calculated and listed in Table 3. It can be found that A0 and
Ea of RS char and PS char present increasing trends with the
increasing pyrolysis temperature, while A0 and Ea of CL char
show opposite trends.
Although RPM can fit well on gasification rates of biomass
char in most conditions, in several conditions, RPM cannot
obtain good results. Typical conditions are shown in the dotted
lines of Figure 7. In Figure 7a, high gasification rates can be kept
in the high conversion range. In this condition, satisfactory
results cannot also be obtained by RPM, which is suitable for
the conditions where peak values appear at conversion ranges
lower than 0.393. To this condition, a modified random pore
model (M-RPM) developed by Zhang and co-workers was
chosen to fit the gasification rates. The M-RPM is a semi-
empirical model based on RPM by introducing a conversion
term to RPM.28 It can be written as r = dX/dt = K(1
X)(1
ψ
ln(1
X))1/2(1 þ (cX)p), where c is a dimensionless constant
and p is a dimensionless power law constant. Fitting results of
M-RPM are shown in the dotted line of Figure 7a and Table 4. It
can be found that better results can be obtained by M-RPM
than RPM.
In panels b and c of Figure 7, where gasification rates increase
in the low conversion range but decrease sharply and present
trailing phenomenon, RPM cannot perform well. This phenom-
enon seems just opposite to the condition of Figure 7a; therefore,
the gasification rates of RS char at 1200 °C and CL char at 800 °C
might be fitted by changing the conversion term (1 þ (cX)p) of
M-RPM from multiplication to division. The shifted M-RPM can
be written as r = dX/dt = K(1
X)(1
ψ ln(1
X))1/2/(1 þ
(cX)p). Fitting results are shown in the solid lines of panels b and
c of Figure 7 and Table 4, and obviously, the shifted M-RPM also
performs much better than RPM.
With regard to the condition of Figure 7a (PS char), some
researchers consider that the increase of the specific area caused
by pore collapse and development during gasification is the
reason.30,31 Some researchers consider that the increase of active
sites caused by alkalis is the reason.32 Wigman and co-workers
believe that alkalis might be covered by some inert products
during char preparation and, with the increasing conversion of
char during gasification, this part of alkalis could be released and
leads to the high gasification rates in high conversion ranges.33 It
can be found from Figure 4 that serious melting happened to PS
char, solid particles with poor porosity were produced, and pore
collapse should not be happened during gasification. Therefore,
the mechanism proposed by Wigman and co-workers should be
more likely in this study. During rapid pyrolysis of PS, particle
melting makes some of the alkalis be wrapped and, with the
dx.doi.org/10.1021/ef200051z |Energy Fuels 2011, 25, 2314–2321
Energy & Fuels ARTICLE

Table 4. Fitting Parameters of M-RPM and Shifted M-RPM

gasification r0
temperature (°C) (10
3 s
1) ψ c p R2

PS char at 1000 °C 1050 1.68 50.01 1.08 3.48 0.997

RS char at 1200 °C 950 1.16 12.60 1.29 2.04 0.996
CL char at 800 °C 850 1.36 8.60 1.15 2.02 0.996

4. CONCLUSION
(1) Under the morphologic structure reserved condition,
gasification rates are obviously affected by surface characteristics
and porosity of char. Melting and accumulation happen during
rapid pyrolysis of PS, leading to the destruction of pore struc-
tures, low specific surface area, and gasification rates of PS char.
Initial structures of RS and CL can be reserved during rapid
pyrolysis, just some slight destruction happens at the high-
temperature conditions. The higher porosity and specific surface
area of CL char make its gasification rates higher than those of RS
char. (2) RPM performs well in most conditions. However, for
gasification of PS char at high temperatures, where high gasifica-
tion rates can remain for high conversion ranges, M-RPM
performs better. For gasification of RS char and CL char at low
temperatures, where gasification rates present a sharp decrease
and trailing in the medium
high conversion range, the shifted
M-RPM performs better.

’ AUTHOR INFORMATION
Corresponding Author
*Telephone/Fax: þ86-21-64250734. E-mail: cxl@ecust.edu.cn.

’ ACKNOWLEDGMENT
This study was financially supported by the National Basic
Research Program of China (2010CB227000), the Shanghai
“Technology Innovation Action Plan”, and the Fundamental
Research Funds for the Central Universities.

’ REFERENCES
Figure 7. Fitting result comparisons of M-RPM, shifted M-RPM, and
RPM on gasification rates of biomass char: (a) PS char at 1000 °C, (b)
RS char at 1200 °C, and (c) CL char at 800 °C.
conversion of char, alkalis can be released gradually. It is the reason
that, although gasification rates of PS char are low, relatively high
gasification rates can remain for high conversion ranges.
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