Fuel 83 (2004) 1519–1525

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A biomass pyrolysis sub-model for CFD applications

A.A. Rostami, M.R. Hajaligol*, S.E. Wrenn
Research Center, Philip Morris USA Inc., P.O. Box 26583, Richmond, VA 23261, USA
Received 14 May 2003; revised 4 September 2003; accepted 4 September 2003; available online 5 March 2004

Abstract
The complex reactions of biomass pyrolysis and the evolution of different volatile species can be well represented by a Distributed
Activation Energy Model (DAEM). The incorporation of this model in a comprehensive Computational Fluid Dynamic model is
computationally expensive because of the requirement for multiple integrations for each computation cell at every time step. In this work, the
integrals have been mathematically expressed in closed forms so that DAEM can be incorporated more efficiently in a CFD code. A computer
program was developed to solve for the yield and rate of evolution of individual pyrolysis products with given kinetic parameters under any
given heating conditions. The model requires kinetic parameters as inputs which may be obtained from TG– FTIR or TG – MS analysis of the
sample. The results are presented for a number of pyrolysis products from cellulose, charcoal and a tobacco sample and compared with the
experimental data. The agreement between the model prediction and the data is generally good; further improvement may be achieved by a
small adjustment of the activation energy and/or the standard deviation.
q 2004 Elsevier Ltd. All rights reserved.
Keywords: Biomass pyrolysis; Distributed activation energy modeling; Pyrolysis modeling

1. Introduction as well as volatiles [2,3]. In a smoldering process, the

Substantial progress has been made in the development
and application of comprehensive, transient and multi-
dimensional computational combustion models for fossil
fuels and these models are now accessible as features in
commercially available CFD computer codes. Eaton et al.
[1] in an extensive review paper reported the state-of-the-art
of various components or submodels that are required in a
comprehensive combustion model. They also discussed the
types of data required to validate the predictions of a
combustion model and current status of combustion models
and submodels. More recently, Williams et al. [2] reviewed
the current status of computer modeling of pulverized coal
and biomass. While the emphasis is on the coal combustion,
Williams et al. [2] points out that the methodology that is
available for coal is transferable to biomass combustion
although there are still areas where there is a lack of
information.
By analogy to coal combustion, the combustion of
biomass follows four fundamental steps: heating-up,
devolatilization to char and volatiles, oxidation of chars
* Corresponding author. Tel.: þ 1-804-274-2419; fax: þ1-804-274-2891.
E-mail address: mohammad.r.hajaligol@pmusa.com (M.R. Hajaligol).
0016-2361/$ - see front matter q 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2003.09.024
volatiles may not have a chance to be oxidized, while in a
vigorous combustion process such as in a boiler, volatiles
burn fast and chars burn more slowly. In any case,
devolatilization or pyrolysis is an important part of the
entire process.
For biomass devolatilization, there are two computer
codes based on Distributed Activation Energy Model
(DAEM) currently available [4,5]: bio-FG-DVC [4] and
bio-FLASHCHAIN [5]. These models are standalone
pyrolysis models that are useful when the heating rate is
specified and the kinetic parameters including the values of
standard deviation for the activation energy distribution
function are available and can be used to predict the yield of
individual pyrolysis products. Jones et al. [6] used the
biomass version of the FG-DVC to model the pyrolysis and
combustion of wheat straw in a drop-tube furnace, and
reported that the predictions of the FG model are validated
by their experimental data. Jones et al. [6] used an assumed
heating rate for the pyrolysis, ran the FG model and then
used the products yield predictions as inputs to their CFD
combustion code.
We here present the results of an alternative mathemat-
ical formulation of a biomass pyrolysis model based on the
DAEM. This model can be directly coupled with CFD code
1520 A.A. Rostami et al. / Fuel 83 (2004) 1519–1525

!
to get the instantaneous temperature as input and deliver the 1 2ðE 2 Ei;0 Þ2
products yield as outputs. A closed-form mathematical fi ðEÞ ¼ 1=2
exp ð4Þ
si ð2pÞ 2s2i
representation is utilized, which makes it easier to integrate
into a CFD code. The results for pyrolysis are compared Using Eqs. (2) and (4), one may express Eq. (3) for the
with and validated by the existing experimental data for yield as
some biomass materials. 
Yi;0 ð1 ðt
Yi ¼ 1=2
exp 2ki;0 expð2E=RTðtÞÞdt
si ð2pÞ 0 0
2. A mathematical perspective of distributed activation #
2
ðE 2 Ei;0 Þ
enrgy model 2 dE ð5Þ
2s2i
The DAEM is by far the most comprehensive model A number of mathematical approaches have been
for analyzing complex reactions such as pyrolysis of coal pursued to deal with the double integration of Eq. (5).
and biomass in practical systems. It has been used to Suuberg [9] integrated the time integral for a constant
model the evolution of individual pyrolysis products from heating rate, ðT , tÞ; case and expressed the integral over E
different precursors in a set of simultaneous first-order in terms of complementary error function. Following
reactions. The model assumes that the distribution of Suuberg [9], Du et al. [10] employed the step function
reactivity caused by the reaction complexity can be approximation technique to determine the activation energy
represented by a set of independent and parallel reactions, distribution corresponding to the thermal decomposition of
each with its own frequency factor and activation energy. (C – O) surface complex. Du et al. concluded that a Gaussian
Usually, it is further assumed that all reactions share the distribution gives a good approximation to the real
same frequency factor, so the reactivity distribution is distribution function, f ðEÞ; for carbon materials investi-
represented by a continuous distribution of activation gated. Varhegyi et al. [11] replaced the lower limit of the
energies [7]. integral with E ¼ 21 and used the Gauss – Hermite
DAEM assumes that the evolution of a given product Quadrature formula to do the integration
involves an infinite number of independent chemical
ð1 X
n
reactions. Each reaction contributes to the formation of a 2
e2x gðxÞ < wi gðxi Þ ð6Þ
product according to 21 i¼1

dYi where xi are the zeros of appropriate Hermite polynomials

¼ 2ki Yi ð1Þ
dt and wi are the weights [12]. By changing variables and
simple transformation, Eq. (5) can be expressed in a form
where Yi refers to the unreacted mass fraction of species i similar to Eq. (6). The resulting integral is evaluated by the
in the initial material and ki denotes the rate constant of the available computational routines [12]. However, a separate
corresponding reaction. The notation used here is not the integration of Eq. (2) using Eq. (3) at each step would be
same as that often used in the kinetics literature, where Vi necessary to have the final solution. The accuracy of this
is the fraction reacted, so Vi ¼ Yi;0 2 Yi where Yi;0 is the method has been improved by the modification of the
initial mass fraction of species i in the material before Gauss – Hermite Quadrature formula introduced earlier by
pyrolysis starts. The rate constant ki typically has Donskoi and McElwain [13].
Arrhenius form


2E
ki ¼ ki;0 exp ð2Þ 3. An alternative approach
RTðtÞ
For CFD purposes, it is the rate of yield of species which
It is assumed that the number of reactions is large
is really needed, rather than the yield itself. The rates are
enough to permit the distribution of energy to be expressed
used as source terms in the species transport equations. The
as fi ðEÞ: Then the fraction of sources with activation
rate equation for each reaction is obtained by differentiation
energies between E and E þ dE is Yi;0 fi ðEÞdE and the total
of Eq. (3) with respect to time
amount of the volatile material released up to time t is
ð1
ðt 
given by dYi
¼ Yi;0 2 ki ðEÞexp 2 ki ðEÞdt fi ðEÞdE ð7Þ

ðt  dt 0 0
ð1
Yi ¼ Yi;0 exp 2 kðEÞdt fi ðEÞdE ð3Þ or
0 0
dYi ð1
Usually, fi ðEÞ is taken to be a Gaussian distribution ¼ Yi;0 2 ki ðEÞfip ðE; tÞdE ð8Þ
dt 0
with a mean activation energy of Ei;0 and a standard
deviation si ; so where
 A.A. Rostami et al. / Fuel 83 (2004) 1519–1525 1521

ðt 
p
fi ðE; tÞ ¼ exp 2 ki ðEÞdt fi ðEÞ ð9Þ By introducing the following variables
0

p 
1 E 2 E0;i 1 E 2 Ei;0
h ¼ pffiffi and u ¼ pffiffi
Following Howard [8] and Suuberg [9], fip ðE; tÞ can be 2 si 2 si
approximated with a series of truncated fi ðEÞ with the lower- we may express Eqs. (14) and (15) as
bound truncation at Emin ðtÞ; which increases gradually with !
p
time. The shape of fip ðE; tÞ remains unchanged during the dYi 1 Emin 2 Ei;0
e2Ei;0 =RTðtÞþð1=2Þðsi =RTðtÞÞ
2
¼ ki;0 Yi;0 erfc pffiffi
course of devolatilization while the lower truncation point dt 2 2s i
Emin ðtÞ varies. The physical interpretation of this assumption
ð16Þ
is as follows. As the sample heats up and partially converts !
to gas phase, the weakest bonds break first and the Yi 1 E 2 Ei;0
¼ erfc min
pffiffi ð17Þ
components with the lowest activation energies leave the Yi;0 2 2 si
pool faster. In other words, only material with activation
energies below Emin ; leave the pool and this dividing line Eqs. (16) and (17) are the main equations to be used to
rises with time as pyrolysis takes place calculate the rate of evolution of a species from a
( reaction. The data input for each reaction are the pre-
p
fi ðEÞ; E . Emin ðtÞ exponential factor, ki;0 (s21), mean activation energy, Ei;0
fi ðE; tÞ ¼ ð10Þ (J/mol K), standard deviation, si (J/mol K), the initial
0; E , Emin ðtÞ
concentration of the precursor i in the solid, Yi;0 and the
Using Eq. (2) for ki ðEÞ and Eq. (4) for fi ðEÞ; Eq. (8) may heating rate TðtÞ:
be expressed as:
!
dYi Yi;0 ki;0 ð1 ðE 2 Ei;0 Þ2 4. Calculation procedure
¼2 exp 2E=RTðtÞ 2 dE
dt si ð2pÞ1=2 Emin ðtÞ 2s2i
ð11Þ Solution of Eqs. (16) and (17) requires the knowledge
of heating rate and the kinetic data for each reaction. The
kinetic parameters for evolving materials from thermal
We break the integrand into two parts: one containing the devalitization are generally obtained under conditions
variable E and the other independent of E where neglecting the heat and mass transfer limitations is
a reasonable assumption. This is acceptable if the particles
ðE 2 Ei;0 Þ2
2E=RTðtÞ 2 ; 212 ðEÞ þ C ð12Þ are small enough and the heating rate is not too high so
2s2i that the internal transport mechanisms can be ignored.
After some mathematical manipulations, one may arrive Chen et al. [4] used thermogravimetry –Fourier transform
at: infrared (TG – FTIR) data to determine the kinetic

parameters for the evolving species from pyrolysis of
p 

1 E 2 Ei;0 Ei;0 1 si 2 biomass samples.
1ðEÞ ¼ pffiffi and C ¼ 2 þ
2 s RTðtÞ 2 RTðtÞ When pyrolysis is done under a controlled environment,
the heating rate is an independent parameter and is normally
where
known. In a real combustion process, however, the spatial
p s2i and temporal distributions of temperature have to be
Ei;0 ¼ Ei;0 2 ð13Þ calculated using a comprehensive combustion code. At
RTðtÞ
every time step, the temperature is used in the pyrolysis
Then Eq. (11) takes the following form: equations (16) and (17) to calculate the rate of evolution of

 ! species.
dYi Yi;0 ki;0 Ei;0 1 si 2 Given the kinetic parameters and the heating rate, at
¼2 exp 2 þ
dt si ð2pÞ1=2 RTðtÞ 2 RTðtÞ every time step during the heating process, the value of

!
ð1 p 2 Emin ; is calculated form Eq. (17) and is substituted back in
1 E 2 Ei;0
 exp 2 dE ð14Þ Eq. (16) to calculate the evolution rate. Then, the rate is
Emin ðtÞ 2 si
used to determine the cumulative yield at time t and the
Similarly, from Eq. (3) for individual reactions, we have procedure is repeated. This process requires frequent
evaluation of the error function and the inverse error
ð1 function. Numerical integration will not be needed at
Yi
¼ fip ðEÞdE every time step.
Yi;0 0 A computer program using Cþ þ has been written to
ð1
 ! perform the calculations. The results for a few cases
1 1 E 2 Ei;0 2
¼ pffiffiffiffi exp 2 dE ð15Þ together with the experimental data will be presented
si 2p Emin ðtÞ 2 si here.
1522 A.A. Rostami et al. / Fuel 83 (2004) 1519–1525

5. Input data that they best fit the TG – FTIR data. TG – MS analysis may
also be used to determine the kinetic parameter [11].
Predictions by the present pyrolysis model are compared
with a number of experimental data from different sources.
Unless otherwise specified, the data for the present 6. Results
calculation are exclusively provided by Advanced Fuel
Research, Inc. under a contract with Philip Morris USA, Inc.
First we compare the model prediction with the
The corresponding experimental procedure is described in
experimental data. Fig. 1 shows the rate of evolution of
Refs. [4,14,15]. The experimental setup consists of a
methane from cellulose pyrolysis. The heating rates are
thermogravimetric analyzer (TG) coupled with a Fourier
constant at 30 and 100 K/min and only one peak is observed
Transform Infrared (FTIR) spectrometer for the analysis of
in the evolution rate data. The corresponding kinetic
the evolved species. The biomass samples are suspended
parameters are provided by Advanced Fuel Research, Inc.
from a balance in a gas stream inside a furnace. As the
for Philip Morris USA, Inc. and are k0 ¼ 1:2 £ 1012 s21,
sample is heated, the evolving volatile products are carried
E0 =R ¼ 38; 000 K and s=R ¼ 4000 K. The initial precursor
into a gas cell held at 155 8C where the volatiles are
concentration in the solid is 0.19% on a weight basis. The
analyzed by FTIR spectroscopy. The evolution rate and
agreement is excellent, partly because of the fact that only
cumulative yield of several products are measured under
one source in cellulose contributes to the evolution of
three heating rates ranging from 3 to 100 K/min. The system
methane. The yield of methane under the same conditions is
continuously monitors the time-dependent evolution of
gases, heavy liquids (tars) and the weight of the residues. shown in Fig. 2, where again the model prediction matches
The so-called Tmax method originally introduced by well with the experimental data.
Kissinger [16] was employed to determine the kinetic Fig. 3 shows the evolution rate of hydrogen from
parameters k0 and E0 : Tmax is the temperature at which the devolatilization of a nutshell charcoal under a constant
yield rate of a species is maximum. Typically, this value is heating rate of 10 K/min. The kinetic parameters are
measured at several different constant heating rate exper- obtained by thermogravimetry – mass spectrometry (TG –
iments and the kinetic parameters are obtained from a plot MS) by Varhegyi et al. [11]. Hydrogen evolution is
2
of ðH=RTmax Þ versus ð1=Tmax Þ together with the following characterized by two parallel reactions with a distributed
equation activation energy, where the smaller peak is hardly visible
in the figure. In fact about 90% of the contribution to the
H formation of hydrogen comes from the main peak, which
ln 2
¼ 2E0 =RTmax þ lnðk0 =E0 Þ ð18Þ occurs at about 700 8C. The kinetic parameters for the two
RTmax
precursors are k0;1 ¼ 2 £ 105 s 21, E0;1 =R ¼ 15; 270 K,
where H is the heating rate (K/s). Eq. (18) is exact for both s1 =R ¼ 6 K, k0;2 ¼ 2:5 £ 106 s21, E0;2 =R ¼ 21; 290 K and
first-order and nth-order reactions and is considered an s2 =R ¼ 1563 K, respectively. The corresponding initial
excellent approximation for distributed reactivity models precursor concentrations are Y0;1 ¼ 0:09 and Y0;2 ¼ 0:91:
[7]. Once the pre-exponential factor and the activation The evolution rate in Fig. 3 has an arbitrary unit. The
energy are calculated for each reaction, the width of the heating rate of 10 K/min is also shown in Fig. 3. The model
standard deviation, s; can be determined from the width of prediction does a great job up to a temperature of about
the peak representing the rate of weight loss. The use of Tmax
approach guarantees matching of the predicted distribution
peak with the experimental data peak. It remains the width
of the distribution curve that can be matched by choosing an
appropriate value for s: At the end of the above procedure,
the following information is available for the evolution of
each precursor pool [14]: k0 ; E0 ; s; and the pool size, i.e. the
concentration of a precursor in the initial sample, Y0 : In
general, each volatile species (light gases and tars) may
evolve from multiple precursors each of which represented
by the corresponding peak in the yield rate curve. Therefore,
we may need to account for the contribution of more than
one precursor to the evolution of each species. This
procedure is simple and provides a set of reasonable
parameters. However, the approximations used to estimate
the parameters would affect the accuracy of the resultant
parameters. The size of precursor pools for individual peak Fig. 1. Methane evolution rate from cellulose pyrolysis at a heating rate of
is determined by adjusting the simulated peak heights so 30 and 100 K/min.
 A.A. Rostami et al. / Fuel 83 (2004) 1519–1525
Fig. 2. Methane yield from cellulose pyrolysis at a heating rate of 30 and
100 K/min.
700 8C, however, does not agree well with the experimental
data for temperatures above 700 8C. The agreement can be
greatly improved by a slight (less than 3%) change of the
mean activation energy of the larger peak from 21,390 to
20,800 K and by choosing a standard deviation of
s2 =R ¼ 800 K to match the data. This result is also shown
by the thin line in Fig. 3. Both reactions were included in the
model, but the contribution from the lower peak is small as
it is shown in Fig. 3. This is indicated in the figure as a small
widening of the model prediction at a temperature around
550 8C (at a heating time of about 54 min).
The evolution rate of tars (long-chain acids) from a
Burley tobacco sample is shown in Fig. 4. The data
correspond to a constant heating rate of 10 K/min.
Experimental data show only one evolution peak with
kinetic parameters of k0 ¼ 5:2 £ 1011 s 21, E0 =R ¼
18; 600 K and s=R ¼ 800 K and the initial source concen-
tration of Y0 ¼ 17:0% on dry weight basis. Two model
predictions are shown in Fig. 4 together with the
experimental data. Model prediction using above mentioned
Fig. 3. Hydrogen evolution rate from charcoal at a heating rate of 10 K/min
[11].
1523
Fig. 4. Tar evolution rate from pyrolysis of a tobacco sample at a heating
rate of 10 K/min.
kinetic parameters deviates from the experimental data
particularly at higher temperatures (the right shoulder of the
curve). The predicted temperature at which the yield rate is
maximum, Tmax ; matches reasonably with the data simply
because the kinetic parameters are calculated by using the
Tmax method. The predicted rate at the peak, however, does
not match the measured value. This discrepancy is not
expected to result in a significant error in the total tar yield
as the area covered by the top three data point is small. The
general agreement between the prediction and the data
points improves significantly by a slight adjustment of the
mean activation energy from the proposed value of E0 =R ¼
18; 600 to 18,000 K. The improvement in results due to this
change is also shown in Fig. 4.
Fig. 5 shows the evolution rate of carbon monoxide
from the same tobacco sample as above but at a heating
rate of 100 K/min. Three evolution peaks are observed in
the experimental data and the corresponding kinetic
parameters are: k0;1 ¼ 5:2 £ 1011 ; E0;1 =R ¼ 18600 K,
s1 =R ¼ 1500 K, k0;2 ¼ 4:4 £ 1018 s21, E0;2 =R ¼ 34000 K,
s2 =R ¼ 1500 K, k0;3 ¼ 1:4 £ 1011 s21, E0;3 =R ¼ 29400 K
Fig. 5. CO evolution rate from pyrolysis of a tobacco sample at a heating
rate of 100 K/min.
1524 A.A. Rostami et al. / Fuel 83 (2004) 1519–1525
Fig. 6. CO desorption rate from a Carbon sample at slow and fast heating
rates. Data from Ref. [10].
and s3 =R ¼ 2000 K. The initial concentration of each
source is 2.04, 0.73 and 5.1%, respectively. It is not a
coincidence that the agreement between the present model
and the data on the temperatures at which the evolution
rates are maximum, Tmax ; are excellent as the kinetic
parameters are calculated from the same data by using the
Tmax method. Reasonable agreement between the present
model prediction and the data point also exists, except for
the data points from the second source (around the middle
peak). Also shown in the figure is the prediction made by
FG-Biomass pyrolysis model [14].
Finally in Fig. 6, the model prediction is compared
with the experimental data for CO desorption rate from a
carbon sample in a temperature programmed heating
process. The data are obtained from Du et al. [10]
corresponding to slow and fast heating rates where the
temperature is increased non-linearly from 598 to 1173 K
in about 25 and 35 min, respectively. Du et al. concluded
that the best fit of f ðEÞ with a Gaussian distribution results
when the mean and standard deviation of distribution are
E0 =R ¼ 23500 K and s=R ¼ 2260 K for k0 ¼ 1010 min21
and E0 =R ¼ 35000 K and s=R ¼ 3900 K for k0 ¼
6 £ 014 min21. The first set of values is used for the
model prediction in Fig. 6. As indicated in Fig. 6, using
the standard deviation of s=R ¼ 2260 K, in the model
under predicts the experimental data for the slow heating
case. By lowering its value to 1700 K, while using the
same values E0 =R ¼ 23500 K and k0 ¼ 1010 min21 as
suggested by Du et al. [10], a better agreement with data
is achieved. These values of kinetic parameters when used
for the fast heating rate conditions result in excellent
agreement with data (Fig. 6).
The present pyrolysis model may be used for the
standalone devolatilization applications as well as a sub-
model in a CFD code. The results presented in this work
indicate that the model can predict the experimental data
with a reasonable accuracy. The accuracy can be
improved by minor adjustment in the kinetic parameters
or by changing the width of the activation energy
distribution.
7. Conclusions
The DAEM was applied to biomass pyrolysis. This
model was expressed in terms of error function. The model
was used to predict the evolution rate and yield of some
volatiles from pyrolysis of cellulose, charcoal and a tobacco
sample. The prediction is generally in good agreement with
the experimental data and the accuracy can be improved by
slight changes in the kinetic parameters. The kinetic
parameters and the initial concentration of the contributing
sources to the evolution of a species must be obtained from
experiments and are used as inputs to the model. Although
the model was applied to standalone pyrolysis cases, the
mathematically closed form representation of the results
makes the integration of the model with a CFD program
more convenient.
Acknowledgements
Authors would like to acknowledge Drs Eric Suuberg of
Brown University and Marek Wojtowicz of Advanced Fuel
Research, Inc. for their helpful comments. Authors are also
grateful to Philip Morris USA management for their support
of this fundamental research.
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