Fuel 88 (2009) 2335–2339

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Fuel

j o u r n a l h o m e p a g e : w w w . e l s ev i e r . c o m / lo c a t e / f u e l

A new char combustion kinetic model 1. Formulation

a, b c a
Richelieu Barranco *, Andrés Rojas , Juan Barraza , Edward Lester
aDepartment of Chemical and Environmental Engineering, University of Nottingham, Nottingham, NG7 2RD, UK
bUniversidad Nacional de Colombia Sede Palmira, Departamento de Ingeniería, Palmira, Colombia
cGrupo de Ciencia y Tecnología del Carbón, Escuela de Ingeniería Química, Universidad del Valle, Cali, Colombia

article info abstract

Article history: This paper describes the development and formulation of a novel char combustion kinetic model for pul-verised coal. The
Received 4 November 2008 chemical reaction rate was considered as a function of coal intrinsic reactivity and fuel mass for a global reaction order n. The
Received in revised form 31 January 2009 equation for char combustion reaction rate was devised by dimen-sional analysis using the Rayleigh method. It shows the
Accepted 5 February 2009 Available online 27
dependency of chemical reactivity on coal param-eters, such as maceral and mineral composition; char parameters, such as
February 2009
specify surface area and apparent density; devolatilisation time; temperature; and activation energy. The char combustion reac-
tion rate equation developed, unlike most models, is dimensionally homogenous and is expressed by three dimensionless
Keywords:
numbers which have physical chemical meaning. The model also exhibit similarities with transport phenomena models
Char combustion model
Intrinsic reactivity
described by dimensionless numbers.
Kinetic coefficient
2009 Elsevier Ltd. All rights reserved.

1. Introduction (below 900 K, Zone I), and either intrinsic order of unity or zero at higher
temperatures (above 1100 K, Zone II).
Global models of pulverised coal combustion involve a series of chemical In their work, Hurt and Calo [12] also presented three different kinetic
reactions including coal devolatilisation [1–9], volatile combustion [10,11], models in an attempt to reproduce the aforementioned data. The first model,
char combustion [12,13] and gas-phase oxida-tion [4]. It has been established named Global Power-Law Kinetics, consid-ers the reaction between coal, the
that mathematical models which represent the intrinsic kinetics of coal active site, and oxygen as follows:
combustion depend on the combustion process used [12], reactivity of the
coal [14], coal ther-mo-physical characteristics [10], and operating conditions
C þ O2 ! CO=CO2
[15,16]. Operating conditions may include air flow rate, char preparation
temperature, and system pressure [17]. For pulverised coal com-bustion, the and the reaction rate law is given by
combustion rate of volatile matter is negligible in comparison with the
combustion rate of the char, owing to the small size of the fuel particles and rgas ¼ kPnO2 ð1Þ

the high temperatures used. Therefore, the overall combustion process is
controlled by the reac-tion rate of the char pore structure [17,18].
Hurt and Calo [12] identified a semi-global intrinsic kinetic model which
reproduces the accurate magnitudes of temperature (global intrinsic activation
energy) and concentration dependence (global intrinsic reaction order) for
steady-state combustion across a wide range of temperatures. They compiled
data on global intrin-sic reaction orders at or near atmospheric pressure
reported in the literature from the 1970s until year 2000. Oxygen partial
pressure in the range 0.1–2 bar, and evidence of detailed consideration of
transport effect, were the main data selection criteria. Global reac-tion orders
appeared to be fractional (0.6–1) at low temperatures
The second model, called two-steps Langmuir–Hinshelwood Semi-global
Kinetics, predicts an effective reaction order that varies with oxygen
concentration and temperature. Neither the first nor the second models were
found to properly describe char combus-tion kinetics across the range of
temperatures and oxygen pressures of the compiled data. However, both
Power-Law and Langmuir– Hinshelwood Kinetics can be used appropriately
under restricted conditions, especially at high temperatures, in pulverised coal
com-bustion. The reactions considered by Langmuir–Hinshelwood
mechanism are as follows:
C þ O2 ! CðOÞ
C ðOÞ ! CO

The reaction rate law for non-dissociative form is expressed as:

* Corresponding author. Tel.: +44 115 8466391; fax: +44 115 9514115.
k1k2PO2
E-mail address: richelieu.barranco@nottingham.ac.uk (R. Barranco).
rgas ¼
k1PO2 þ k2 ð2Þ
0016-2361/$ - see front matter 2009 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2009.02.005
2336 R. Barranco et al. / Fuel 88 (2009) 2335–2339

Nomenclature

a, b empirical constants for the global kinetic reaction Mc mass of coal particle, g
A
model MM mineral matter content of original coal, % v/v
f pre-exponential factor M
A 2 1 nR mineral matter and non- reactive inertinite content of
g specific surface area of char pores, cm g coal, cm
3
2
As reaction area, cm Mo2 molecular weigh of oxygen, g mol
1
C M
F fixed carbon content of coal in a dry ash-free basis, R vitrinite, liptinite and reactive inertinite content of coal,
w/w% 3
2 1 cm
DO diffusion coefficient of the oxygen in the gas, cm s n global reaction order
Dp char particle diameter, cm Po2 oxygen partial pressure in the char particle surface, atm
1 2 1
dm/dt rate of mass loss of char during combustion, g s ri intrinsic reaction rate, g cm s
E 1 00
activation energy, J mol rc char combustion rate, g cm s
2 1
1 1
Ea apparent activation energy, J mol K R 3
universal gas constant, atm cm mol K
1 1
Ei apparent activation energy for region i of Arrhenius lin- Rc
2 1
chemical reaction rate coefficient, g cm s atm
n
1 1 R
earity, J mol K diff
2 1
diffusion reaction rate coefficient, g cm s atm
1
1 1
Em weighted mean activation energy, J mol K Ri
2 1
intrinsic reaction rate coefficient, g cm s atm
n
Fi weight fraction of char burned during region i of tv char devolatilisation time, s
Arrhenius linearity T temperature, K
H 1
unit of energy per mol, J mol Tg gas temperature, K
IHR high reflectance inertinite content of coal, %v/v
TO oxygen temperature, K
ILR low reflectance inertinite content of coal, %v/v
Tp char surface temperature, K
InR non-reactive inertinite content of coal, %v/v V vitrinite content of coal, % v/v
IR ractive inertinite content of coal, %v/v VPs pseudo-vitrinite content of the coal, % v/v
k kinetic coefficient of reaction in Arrhenius equation x reactive inertinite fraction
ki kinetic coefficient of reaction for reaction i Xo2 oxygen mole fraction
k0 empirical constant for the new kinetic combustion
model
2 1 1 n q
Greek letters
k0 reaction kinetic constant, cm s g atm c characteristic dimension of the char particle, cm
L unit of length, m gThiele modulus
L liptinite content of coal, %v/v
uratio of reacting surface to external (equivalent sphere)
Lm unit of length for macerals in coal surface area of particle
m car remaining mass, g q coal density, g cm
3
Munit of mass, g 3
r apparent density of the char, g cm
dm 2 XO2 1 1 1

Finally, the third model, which is know as Three-Steps Semi-global

Kinetics, suggests reactions involving gas phase oxygen with surface
complexes, which may or may not include the generation of a new complex
C(O), on the product side:
k
1

C þ O2 ! 2CðOÞ
k2

CðOÞ þ O2 ! CO2 þ CðOÞ

k3

CðOÞ ! CO
The reaction rate law for this model is as follows:
þ
k1k2PO2 k1k3PO2 k3
r ;CO=CO 3
2 ¼
gas ¼ k1PO2 þ k3=2 k2PO2 ð Þ

Model 3 is able to describe the basic trends in global reaction order, global
activation energy and the CO/CO2 relationship over a wide range of
combustion conditions. It predicts combustion in such a way that at low
temperatures, the reaction order is in be-tween 0.6 and 1, and at high
temperatures the reaction order is zero [12,19]. These three kinetic models,
however, are only a function of temperature and oxygen concentration.

By following a different approach, some other researchers [10,14,20–23]

to determine char
presented two different models and their variants
combustion reaction rate. The first model, known as Baum
and Street model, is based on apparent activation energy,
whereas the second model, developed by Smith, is funda-
mentally an intrinsic reactivity model. The Baum and Street
model is expressed by the following equation:
dt ¼ pDp qRTMO2 Rdiff þ Rc ð4Þ
 This model assumes that the superficial reaction rate deter-mines the
chemical and/or diffusion kinetics rate. The mass loss rate during combustion,
dm/dt, depends on particle density and diameter, and the relationship between
the reaction area and the particle external surface area. The particle is
assumed to be spher-ical. The chemical and diffusion reaction rate
coefficients in the model are represented by [10,24,25]:

Ea

Rc ¼ Af ue RT ð5Þ

R 2/DOMc T p þ Tg 0:75 6
¼
diff RTODp 2 ðÞ
For the second model, the reactivity or intrinsic reaction rate, r i, is expressed
by the following equation:
ri ¼ RiPnO2 ð7Þ

where the intrinsic reaction rate coefficient is given by:

Rc
Ri ¼
gcrAg ð8Þ
Under conditions of chemical control (Zone I), in the case of pulver-ised coal
technology, the chemical reaction is the controlling step, and consequently,
the chemical reaction rate is the true reaction rate, which is given by:

rc ¼ Rc PnO2 ð9Þ

Here n is the true reaction order.

This latter model assumes that the char has an average
surface area and constant effectiveness factor during
combustion. It was
 R. Barranco et al. / Fuel 88 (2009) 2335–2339
established [14], experimentally, that the chemical reaction coeffi-cient
depended on char parameters such as apparent density, specific pore surface
area, fixed carbon content, and particle tem-perature; and on the maceral
content of the parent coal. The chem-ical reaction rate coefficient devised is
given by the following equation [12,24–26]:
Rc ¼ e 89r 7:5Ag 0:5CF3:5Tp9:5 þ FMAC ð10Þ
where
FMAC ¼ ½1:4ðV þ 0:8VPSÞ& ½0:6ðIHR þ 1:6ILRÞ& ð11Þ
In terms of coal combustion kinetics, Cumming and McLaughlin [27,28]
developed a model which considers the coal combustion rate as a function of
the kinetic constant and the coal residual mass, as follows:
dm n Rayleigh method [29]. According to this method, R c can be expressed by the
dt ¼ km ð12Þ
The kinetic constant is expressed as a function of temperature by the
Arrhenius equation:
E
k ¼ Af RT ð13Þ
A graph of log k against 1/T allows the apparent activation energy, E, and the
frequency factor, Af, to be determined.
Cumming and his co-worker assumed the combustion process followed a
pseudo-first order kinetic. This assumption was based on the fact that coal
sample mass used in the thermogravimetric analysis is small, the coal
particles are fine, and the air supply is in excess, hence the oxygen
concentration remain virtually un-changed as the reaction progresses. They
also considered that coal combustion reactivity may be estimated by means of
combustion profiles using a parameter know as weighted mean activation en-
ergy, Em. This parameter may be obtained from Arrhenius plots where one to
four linear zones can be observed. These represent the type of reaction
mechanism occurring at specified temperature intervals. Every linear zone
exhibits its own activation energy, E a, which can be associated with the
various stages of the combustion process. These associated activation energies
may give an indica-tion of global reactivity of the fuel when the fraction of
the fuel consumed during each stage, (Fi), is incorporated as follows:
Em ¼ E1F1 þ E2F2 þ þ EjFj ð14Þ
2337
the char, fixed carbon content, apparent density of the char, and maceral
composition of the original coal, according to Eq. (10), for instance. In spite
of the effort to obtain a general equation, Eq. (10) does not show dimensional
consistency with respect to the parameters and exponents involved. One of
the reason is that Rc depends on others parameters such as coal
devolatilisation time, which has influence on the residual volatile content of
the char, and the mineral matter content of the original coal. Overall, this
means that the reaction kinetic constant, Rc is influenced by factors related to
coal characteristics, char properties, and intrinsic reac-tion characteristics.
Coal characteristics include percentage of reac-tive macerals, M R, which
groups vitrinite, liptinite, and ‘‘reactive” inertinite; and percentage of mineral
matter and ‘‘unreactive” inertinite, MnR. Char parameters include apparent
density, specific pore surface area, and devolatilisation time. In terms of char
intrin-sic reaction characteristics, this includes activation energy and char
oxidation temperature. By considering all these independent variables, an
equation to determine Rc can be derived by dimen-sional analysis using the
following theoretical equation:
Rc ¼ f ðr; Ag ; T; E; R; MR; MnR; tv Þ ð17Þ
In general terms this equation can further be expressed as follows:
Rc ¼ raAgbTc EdReMRfMnRgtvh ð18Þ
where the exponents a, b, c, d, e, f, g, and h are constants which make the
equation dimensionally consistent. By substituting the corre-sponding
dimensions for each parameter, the following expression is obtained:
M
L2tMn ¼ MaL 3aL2bM bTc HdHeT eLm3f Lm3g tvh ð19Þ
Solving for the exponents: a = 2n, b = 3n 1, c = e = d, g = f, and h = 1.After
substitution of these exponents, Eq. (18) becomes:
Rc ¼ r2nAg3n 1T dEdR dMRfMnRf tv 1 ð20Þ
Parameters with the same exponent can be grouped to the
right side of the equation while the rest are placed on the lef
side:
g
Rc tv E d MR f
3n 1 "
r2nA ¼f RT MnR # ð21Þ
It is then possible to determine the differences in reactivity among coals since A proportionality constant, k0,
can then be introduced in the equa-
the smallest the weighted mean activation energy is, the more reactive the tion and constants d and f can be renamed as a and b,
coal is considered to be. respectively. Therefore, Eq. (21) can be rewritten as:
Rc tv E a MR b
2. Formulation of the kinetic equation

r2nAg3n 1 ¼ k0 RT MnR ð22Þ

When coal particle size is below 75 lm, the chemical kinetic governs the
Generally speaking, vitrinite and liptinite are chemically reactive during
char oxidation process and the effect of oxygen diffu-sion into the char pores
pyrolysis [30–35]. In the case of inertinite, however, there are some points of
is negligible [14]. Thus the char combustion rate depends on the oxygen
controversy. Several workers have considered this maceral group as inert
partial pressure and the char remaining mass on a dry-mineral-matter free
during combustion and this behaviour has been attributed to being primarily
basis. This can be expressed, for a q + n global order reaction, by the
due to its aromatic nature [31]. Part of the inertinite group, mainly low
following equation:
reflectance semifusi-nite, may also be deemed as reactive [36,37]. This debate
1 dm has led researchers to define a coal maceral in terms of its reactivity. Thus, a
¼ maceral is deemed to be reactive if it exhibits thermoplasticity during
rc00 As dt ¼ k0POq2 mn ð15Þ pyrolysis and char formation, and the type of char generated is referred to as
When the oxygen concentration is in excess, the reaction rate be-comes and fused char [38]. Further to this, the proportion of the reactive fraction of a
equation of pseudo n-order:
coal has usually been determined by com-bining the liptinite and vitrinite
1 dm percentages with the fusible inert-inite fraction of the inertinite [38,39].
¼
rc00 As dt ¼ Rc mn ð16Þ
The chemical reaction rate coefficient, Rc , may be expressed by several Subdivision of the inertinite group into ‘reactive’ and ‘unreactive’
empirical correlations [23–26]. It is a function of parame-ters such as particle components on the basis of their reflectance values with respect to the
temperature, specific pore surface area of vitrinite maceral was intended to clarify these discrepancies
2338 R. Barranco et al. / Fuel 88 (2009) 2335–2339

[32,40–44]. Barranco et al. [40], for example, adopted a reflectance of 2.2%

to differentiate between fusible and non-fusible inertinite. Conversely, by
studying a wide variety of coals, Jones et al. [32] re-ported that there was a
fairly well defined reflectance level below which inertinite became fluid
during pyrolysis. This boundary was found to be coal dependent and
increased with rank from 1.3% to 1.8% for coals of vitrinite random
reflectance ranging from 0.5% to
1.2%. On this basis, the percentage by volume of coal reactive mate-rial, M R,
can be considered as the percentage by volume of vitrinite, V, liptinite, L, and
Fig. 2. Analogy of the char combustion kinetic model with Arrhenius equation.
‘‘reactive” inertinite, IR; whereas the percentage by volume of non-reactive
inertinite, InR, and mineral matter content, MM, can be deemed as non-
reactive material, MnR. Therefore, Eq.
(22) can be expressed as:

Rc tv Ea a V þ L þ IR b

k0 23
3n 1
r2nAg ¼ RT MM þ InR ð Þ
The reactive inertinite percentage, I R, is a fraction of the total inert-inite, I,
present in a coal. Therefore, if x is defined as the inertinite reactive fraction,
then IR is equivalent to xI. Consequently the non-reactive inertinite content,
InR, is equal to (1 x)I. The reactive inertinite fraction, x, is a function of coal
rank and independent on the inertinite content [38,39]. Thus Eq. (23) can be
rewritten as:
a b Fig. 3. Analogy of the char combustion kinetic model with heat transfer coefficient model.
Rc tv Ea V þ L þ xI
k0 24
r2nAg 3n 1 while the dimensionless number 3 in the char combustion model is a
¼ RT MM þ ð1 xÞI ð Þ
combination of the properties of the coal. Nusselt number gives a measure of
It can be observed that the left side term of this equation relates the
the ratio of total heat transfer to conductive heat transfer and dimensionless
reaction kinetic constant, Rc ; with char characteristics such as specific
number 1 is related to the char chem-ical reaction rate and the physical
density and specific surface area, as well as devolatilisation time. The first
properties of the char.
factor on the right side represents the Arrhenius number which relates the
activation energy, the ideal gas constant, and the combustion temperature. The
rightmost factor represents the relationship between the percentage of reactive 3. Conclusions
and non-reac-tive material of coal.When substituting Eq. (24) into Eq. (16),
the overall combustion rate is obtained: Most of the char combustion models found in the literature are empirical
in nature and are not dimensionally homogenous. The new char combustion
þð Þ kinetic model presented in this paper is no-vel and was obtained by
3n 1
R00 1 dm k r2nAg Ea a
V L þ xI b
mn 25 dimensional analysis where char and coal parameters and combustion reaction
¼ characteristics were corre-lated using the Rayleigh method. The equation
c As dt ¼ 0 tv ! RT MM þ 1 xI ð Þ obtained is dimen-sionally consistent and is given by a combination of three
Apart from exhibiting dimensional homogeneity, the dimensionless numbers dimensionless numbers with have physical–chemical meaning. The three
in the model have some physical chemical mining. These numbers are shown dimensionless numbers are related to the physical char-acteristics of the char;
in Fig. 1. The dimensionless number 1 repre-sents the relation of the char the chemical characteristic of the coal/char combustion process; and the
chemical reactivity and its physical properties. The dimensionless number 2 is composition of the coal in terms of reactive and non-reactive entities. The
associated with the chemical characteristics of the combustion process, while new model presents simi-larities with models of dimensionless numbers used
number 3 considers the physical–chemical characteristics of coal by the in transport phenomena and with the Arrhenius equation.
relation of its reactive and non-reactive fractions.

The char combustion model equation has some similarities with Arrhenius
equation as it can be seen in Fig. 2. In addition, this mod-el resembles
transport phenomena models represented by dimen-sionless numbers. For
instance, the equation used to calculate heat transfer coefficients (Fig. 3)
which is a function of Nusselt, Rey-nolds and Prandtl dimensionless numbers.
The heat transfer driv-ing force is given by the Reynolds number.
Correspondingly the chemical reaction driving force is represented by the
Arrhenius number (dimensionless number 1) in the char combustion model.
Prandtl number provides a combination of properties of the fluid,
Acknowledgments
The authors wish to thank COLCIENCIAS for the financial sup-port of
this work. Also the technical support of ‘‘Universidad del Valle” and The
University of Nottingham is greatly acknowledged.
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