Chemical Engineering Science 59 (2004) 4205 4215

www.elsevier.com/locate/ces

DEM-LES simulation of coal combustion in a bubbling %uidized bed

Part II: coal combustion at the particle level
Haosheng Zhou, Gilles Flamant , Daniel Gauthier
Institut de Science et de Genie des Materiaux et Procedes, CNRS-IMP, BP.5 66125 Odeillo-Font-Romeu Cedex, France
Received 5 February 2003; received in revised form 2 December 2003; accepted 9 January 2004

Abstract
The discrete element method-large eddy simulation (DEM-LES) is used to model coal combustion at the particle level in a bubbling
%uidized bed. The gas phase is modelled as a continuum and the solid phase is modeled by DEM. Chemical reactions consist in the
heterogeneous reactions of char with O2 , CO, CO2 , NO, and N2 O, and in the homogeneous reactions involving CO, O2 , NO, and N2 O.
The colliding particleparticle heat transfer is based on the analysis of the elastic deformation of the spheres during their contact. The
model predicts the e9ects of the particle heterogeneous %ow structure on the thermal characteristics of coal particles when heating and
burning, and the gaseous emissions from a %uidized sandcoal binary mixture. The heating rates are 1627 and 432 K=s for, respectively,
0.8 and 2:0 mm diameter coal particles fed into the %uidized bed. The instantaneous contribution of the collision heat transfer is weak,
less than 5.0% of the total power exchanges (coal combustion, radiation, convection and collision) during the heating and 1.5% during
the combustion. The temperature of the coal particles exceeds the bed temperature, which is in qualitative agreement with experimental
data from literature. The e9ects of the diameter of coal particles, of the bed temperature, and of the inlet gas velocity on the thermal
characteristics are also studied.
? 2004 Elsevier Ltd. All rights reserved.
Keywords: Fluidized bed; Coal combustion; Pollutant formation; Temperature of coal particle; Numerical simulation

1. Introduction
When a solid fuel, such as coal, municipal solid waste
or biomass, is fed into a %uidized bed combustor, each particle undergoes several processes which can occur sequentially or simultaneously, including drying, volatile evolution
(and combustion), char combustion (or gasiDcation). The
solid fuel combustion is greatly in%uenced by the %uidized
bed hydrodynamics, fuel properties, oxygen supply and bed
temperature (Palchonok et al., 1997).
Proposed models to predict the performance of %uidized bed coal combustors have been extensively reviewed
(Adanez and Abanades, 1992). Most of them are based on
the 2-phase theory of %uidization, in which the %uidized bed
consists in a bubble phase and an emulsion phase. However,
2-phase models are unable to predict the gas back-mixing
and the recycle peak in solids mixing. Computational %uid
Corresponding author. Tel.: +33-4-68-30-7758;
fax: +33-4-68-30-2940.
E-mail address: %amant@imp.cnrs.fr (G. Flamant).

0009-2509/$ - see front matter ? 2004 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2004.01.070

dynamics (CFD) models of %uidized bed coal combustion

are rather scarce, due to the complex mathematical modelling and to the unsteady character of the numerous equations (Peirano and Leckner, 1988; Lathouwers and Bellan,
2001; Rong and Horio, 1999; Zhou et al., 2002). The discrete element method (DEM) model has been used to simulate gasparticle %uidization since the 1990s, it can simulate
phenomena such as bubbling, slugging and particle transport within the bed. The DEM model describes accurately
not only the particle motion (particle rotation, collision with
other particles, : : :) but also the chemical reactions, heat and
mass transfers, etc. at the individual particle level.
The inter-particle heat transfer due to collision is thought
to be signiDcant in the %uidized bed containing both cold and
hot particles. Two kinds of models were proposed to describe
the heat transfer: dominated by either conduction through
the gas lens (Delvosalle and Vanderschuren, 1985), or direct
conduction due to elastic deformation during impact (Sun
and Chen, 1988). The former was used by Rong and Horio
(1999) to investigate char combustion in a %uidized bed,
and the latter was applied to heat transfer in both dilute and

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H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

dense gassolid %ows (e.g. Li and Mason, 2000; Lathouwers

and Bellan, 2001).
The heating rate a9ects the volatile yield and the devolatilization time from coal particles fed into the combustion system (Saxena, 1990). Stubington and Sasongko
(1998) reported that the heating rate ranges from 2 to
150 K s1 for 2 to 20 mm in diameter coal particles fed in
an industrial %uidized bed combustor. The temperature of
burning coal particles exceeds the %uidized bed temperature
(Linjewile et al., 1994; Joutsenoja et al., 1999). The excess
temperature of the coal particles is very critical because
many parameters are sensitive to temperature: the char
oxidation kinetics, the products of CO=CO2 and NO=N2 O
reactions, heat transfer such as convection, radiation and
particleparticle conduction, slag and fouling formation,
etc.
This paper presents the DEM-LES model that was developed for analysing the thermal characteristics of coal particles and the gaseous emissions from a %uidized mixture of
sand and coal. It is useful to study the heating rate, the temperature of coal particles, and to clarify the contribution of
the collision heat transfer of the coal particles fed into the
%uidized bed combustor.
2. Mathematical modelling
The paper is focused on reaction kinetics since hydrodynamics is presented in Part I of this paper.
2.1. Gasparticle hydrodynamics
The gas phase model is based on locally averaged
2-dimensional NavierStokes equations for 2-phase %ow
with %uid turbulence calculated by LES, which take into
account the e9ect of particles on subgrid-scale gas %ow.
The particle motion is treated by a Lagrangian approach,
in which the particleparticle (or wall) interactions are
modelled as DEM (Zhou et al., 2004).
2.2. Main assumptions on coal combustion
The combustion model is based on the following assumptions:
(1) The heat loss through the bed walls is neglected;
(2) The particle is isothermal;
(3) The main products of coal pyrolysis are simpliDed as
CO, CO2 and H2 O;
(4) Each reaction is a Drst-order reaction.
2.3. Single coal particle pyrolysis and char combustion
model
Solomon et al. (1993) studied the various impacts of pyrolysis on coal combustion, particularly for Dne particles

as used in pulverized fuel (pf) combustion, and Saxena

(1990) reviewed the devolatilization and combustion characteristics of both Dne and coarse particles as used in %uidized bed combustion. The coal pyrolysis model used here
is that of Donskoi and McElwain (1999). It is based on a
multiple-reaction model with distributed activation energies,
it uses a N th order reaction model where the pre-exponential
factor and the apparent activation energy are functions of
the heating rate. The model predicts the evolution of di9erent species during the thermal decomposition of coal. The
pyrolysis process is modelled as follows:



dVpyrol
EA

= k0 exp
(Vpyrol
Vpyrol )N ;
(1)
dt
RTpc
where N is the order of the reaction, Vpyrol is the mass fraction

of volatiles evolved up to time t; Vpyrol

is the limit value of
Vpyrol as t ; k0 is the pre-exponential factor, EA is the
apparent energy of activation, R is the ideal gas constant,
Tpc is the absolute temperature of coal particle
k0 = A + BTR ;
EA =R = C + D ln(TR );

(2)

where A; B; C; D are constant, TR is the heating rate. The

kinetic parameters are detailed in Donskoi and McElwain
(1999).
The shrinking core model (Smoot, 1993) is adopted to
describe the evolution of coal particles during combustion:
when the carbon burns, ash falls from the particle surface
due to the inter-particle collisions and the particle diameter
decreases continuously to zero, with constant density.
During the combustion of residual char, CO and CO2 may
be produced according to the equation (Chen et al., 2001;
Hobbs et al., 1992)



2
2
+1
kA
C + O2
CO +
CO2 ;
(A)
2
+2
+2
+2
where kA is the kinetic constant for char combustion, and 
is the primary CO=CO2 product ratio given by (Rajan and
Wen, 1980)



7200
:
(A.1)
 = 750 exp
Tp
2.4. Formation of nitric oxides and combustion of
combustible gases
The formation and destruction of N2 O, a potential greenhouse gas and stratospheric ozone layer depletion agent,
is one of the main research topics in the Deld of %uidized
bed combustion. The bed temperature, type of fuel, excess
air, limestone feed, pressure, air-staging and boiler load
are the main factors a9ecting the production of NO and
N2 O in %uidized beds (Johnsson, 1994; Bonn et al., 1995;
Jensen et al., 1995). However, the complex chemistry of
both the formation and the destruction of NO and N2 O is not
completely understood. The heterogeneous reactions of char

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

with CO, CO2 , NO and N2 O within the porous particle, and

the homogeneous reactions involving CO, O2 , NO and N2 O
in the boundary layer are therefore simpliDed.
De Soete et al. (1999) proposed that the char bound to
nitrogen is Drst oxidized to NO by a reaction which is Drst
order with respect to oxygen concentration
+1
kB
[CN] +
NO + [CO]:
(B)
O2
2
The rate of this reaction is assumed to be proportional to
the rate of char combustion with  the constant of proportionality, and [CN] and [CO] representing the char bound
to nitrogen or oxygen, respectively.
NO reacts further with the bound nitrogen to produce
N2 O according to the following heterogeneous reaction
(Krammer and SaroDm, 1994; De Soete et al., 1999):
k

C
[CN] + NO
N2 O + C:

(C)

Several mechanisms have been proposed for the reduction

of NO on the surface of char (Chan et al., 1983; Johnsson,
1994; De Soete et al., 1999). These mechanisms result in
the release of N2 and of chemisorbed oxygen as CO
k

D 1
NO + C
2 N2 + CO:

(D)

The presence of CO in the gas phase enhances the rate

of NO reduction. This may occur through the reaction of
CO with surface-bound oxygen atoms, leading to the regeneration of surface sites for reaction with NO (Chan et al.,
1983). Alternatively, this reaction has been considered as
part of the heterogeneous reaction between NO and C in the
presence of CO: CO acts as an oxygen scavenger, leaving
behind a free active carbon site on the surface of carbon.
This reaction can be written as
NO +

kE 1
CO
2

N2 + CO2 :

(E)

N2 O reacts with char to form N2 and a carbonoxygen

bound. Then, this bound can react with N2 O to form N2 and
CO2 . Alternatively, the chemisorbed O2 may be released
as CO (Amand and Andersson, 1989). In our model, the
following global reaction was adopted:
k

F
N2 O + C
N2 + CO:

(F)

The thermal decomposition of N2 O is expressed as

k

G
1
N2 ON
2 + 2 O2 :

(G)

According to Kilpinen and Hupa (1991) and Allen et al.

(1997), the homogeneous destruction of N2 O in a %uidized
bed combustor can occur through reactions involving: (1)
H and OH radicals; (2) oxygen radicals; and (3) CO in the
presence of water. The overall reaction is written as:
k

H
N2 O + CON
2 + CO2 :

(H)

The oxidation rate of CO depends on the concentrations of

moisture (H2 O(g); ); O2 and CO. The reaction is expressed
as (Hobbs et al., 1992)
kI

CO + 12 O2 CO2 :

(I)

4207

The reaction rates of these homogeneous and heterogeneous reactions are summarized in Table 1.
2.5. Conservation of mass fractions of species
The mass balance for the gas species i (CO2 , CO, N2 O,
NO, H2 O and O2 ) is:
@(f Y i ) @(f u f; j Y i )
+
@t
@xj

 @Y 

@
t
i
f Di +
+ "i ;
=
@xj
! @xj

(3)

where Yi is the local mass fraction of species i; Di (i = 1

6 corresponding to the six gas species in the transport gas)
is the molecular di9usion coeQcient, t is the time,  is the
porosity, f is the gas density, uf is the gas velocity, t
is the subgrid scale (SGS) gas kinetic viscosity, ! is the
turbulent Schmidt number, ! = 0:7. The last term on the
right
is the average mass source arising from reactions, "i =
nR
f i=1
Wi Ri =(Rx Ry), where Wi is the molecular weight.
There is no collisional term since the mass fractions do not
change during a collision, Rx and Ry are mesh spacing in
x and y directions. Table 2 lists the di9usion coeQcients of
H2 O; CO2 , CO, N2 O, NO and O2 . The carrier gas is N2 , and
the di9usion due to other species gradient is neglected. This
is an approximation for multicomponent transport because
N2 represents more than 78% (vol) of the transport gas.
2.6. Heat transfer model
2.6.1. Colliding particleparticle heat transfer
The colliding particleparticle heat transfer is modelled
according to the heat conduction analysis for impinging particle by Sun and Chen (1988). Their theory is based on the
analysis of the elastic deformation of the spheres as they
contact. According to these authors, the spheres have indices
1 and 2, and one deDnes the average radius, r, the average
mass, m, and the average elastic modulus, G, as
rp1 rp2
r=
;
(4)
rp1 + rp2
mp1 mp2
m=
;
(5)
mp1 + mp2
G=

(1

4=3
;
+ (1 (22 )=G2

(6)

(21 )=G1

where rpi is the particle radius, mpi is the particle mass,

(i and Gi are the Poisson ratios and the Young moduli of
the respective materials. For small Fourier numbers for both
spheres, based on the total contact time and on the contact
area, the problem may be approximated by two contacting
inDnite plates, with the heat exchange Qcoll given by
Qcoll =

5:36(m=G)3=5 (rvpn )7=10 (Tp02 Tp01 )

(Cp +)11=2 + (Cp +)21=2

(7)

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H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

Table 1
Reactions included in the model
Reaction

Catalyst

Reaction rate
(mol m3 s1 )

Kinetic constant
(s1 )

Heat release
(J mol1 )

Reference

(A)

Heterogeneous

RA = k A C O 2

Char
Char

R B = kB CO 2
RC = kC CNO

4:04 105
(2=( + 2))
Negligible
Negligible

Field et al. (1967)

(B)
(C)

kA = KOXDN Tpc exp(21578=Tpc )fp

KOXDN = 35
kB = 2(+1)
kA ;  = 1
+2
kC = k1 fp exp(9000=Tpc ); k1 = 3:0

(D)

Char

RD = kD CNO

kD =

(E)
(F)
(G)
(H)

Char
Homogeneous
Homogeneous
Char

RE = kE CNO
RF = k F C N 2 O
RG = kG CN2 O
RH = kH CN2 O

0:159fp exp(6255=Tpc );

Tpc 6 973 K

555:6fp exp(14193=Tpc );

Tpc 973 K

kE = 5:67 103 Tf exp(13952=Tf )

kF = 13:36fp exp(16677=Tpc )
kG = 1:75 108 exp(23800=Tf )
kH = 2:51 108 exp(23180=Tf )CCO; avre

Negligible

Negligible
Negligible
Negligible
Negligible

kI = 1:254 1010 1(CO2 =2)0:25 CH0:52 O

(I)

Homogeneous

RI = kI CCO

2:82 105

exp(20130=Tf )
1 = 7:93 exp(2:48CCO =CO2 )

De Soete et al. (1999)

De Soete et al. (1999)
Krammer and SaroDm (1994)
Chan et al. (1983)
Johnsson (1994)
De Soete et al. (1999)
Chan et al. (1983)
Amand and Andersson (1989)
Bonn et al. (1995)
Kilpinen and Hupa (1991)
Allen et al. (1997)
Dryer and Glassman (1973),
Hautman et al. (1981)

Table 2
Di9usion coeQcients of H2 O; CO2 , CO, N2 O, NO and O2 (Massman, 1998; Canu, 2001)
Gas

H2 O

CO2

CO

N2 O

NO

O2

CoeQcient (104 m2 s1 )

0.2178

0.1381

0.1807

0.1436

0.1729

D O2 = DN 2 O (

WN2 O 0:5
)
WO2

Note: (1) The given values are at D(0, 1) (Tf0 = 273:15 K and p0 = 1:013 105 Pa). (2) Di9usion coeQcients can be expressed as Di (Tf ; p) =
T

Di (0; 1)( PP0 )( T f )1:81 .

f0

where Tp02 ; Tp01 are the temperatures of the particles before collision, vpn is the normal relative velocity, pi is the
particle density, Cpi is the heat capacity of the particle, +i
is the particle thermal conductivity.
For particlewall contact, the temperature and properties
of the second particle are replaced by those of the wall.
Table 3 lists the thermophysical properties of air, sand, and
coal.
2.6.2. Particlegas convective heat transfer
For calculating the particlegas heat convection Qc , the
correlation of Ranz (1952) was adopted to determine the
heat transfer coeQcient hp . Then
Qc = hp Ap (Tp Tf );

(8)

where Ap is the particle surface area, hp =Nu+f =dp ; +f is the

gas thermal conductivity, dp is the diameter of the particle,
Nu is the Nusselt number, Nu = 2 + 0:69Rep1=2 Pr 1=3 ; Pr is
the Prandtl number, Pr = Cf 5f =+f ; Cf is the heat capacity
of the gas, and 5f is the gas viscosity, Rep is the particle
Reynolds number.

2.6.3. Particlebed radiation heat transfer

The particle-bed radiation Qr is given by(assuming that
the emissivity of the %uidized bed bulk is unity)
Qr = !S B &p Ap (Tp4 Tb4 );

(9)

where !S B is the StefanBoltzmann constant, &p is the

particle emissivity, which is assumed to be 0.7 and 0.85
for sand and char, respectively. Tb is the bed temperature
approximated by averaging the temperature of particles over
the bed.
2.6.4. Heating rate of a particle
The rate of change of the particle internal energy is due to
the heat exchange with the surrounding gas resulting from
convection (Qc ), from thermal radiation (Qr ), from the heat
of combustion of char (Qcomb ), and from the energy exchanged during the collision (Qcoll )
mp Cp

dTp
= Qcomb Qc Qr Qcoll ;
dt

where Qcomb = 0 for the sand particle.

(10)

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

4209

Table 3
Thermophysical properties of air, coal and sand (in SI system units)
For air (Flamant et al., 1993)
Density

f (Tf ) =

7

i=1

Wi Ymi

(i = CO2 , CO, N2 O, NO, N2 ; H2 O, and O2 )

+f (Tf ) = 5:66 105 Tf + 1:1 102
Cf (Tf ) = (0:99 + 1:22 104 Tf 5:68 103 Tf2 ) 103

Thermal conductivity
SpeciDc thermal capacity

2=3

5f (Tf ) = 0:42 106 Tf

Dynamic viscosity
For char (Tripathi et al., 2002)
Thermal conductivity
SpeciDc thermal capacity

1=2

+pc (Tpc ) = 0:03171Tpc

Cpc (Tpc ) = C0 [g(:1 =Tpc ) + 2 g(:2 =Tpc )],
where g(:) = : 2 e: =(e: 1)2 ,
:1 = 380; :2 = 1800; C0 = 693
100%
5: 106

Potential pyrolysis loss Vpyrol

SpeciDc internal surface area of the char, fp
For sand (Flamant et al., 1993).
Thermal conductivity
SpeciDc thermal capacity

+ps = 1:87
Cps = 860

(11)

where q is the heat source in a unit volume. The heat source

consists in the heat transfer between the particle and the gas
(Qc ), and the heat release of burning CO in the computational cell, (QCO ). Therefore, the heat source is
Qc + QCO
:
(12)
q=
RxRy
2.7. Computation conditions

3. Results
3.1. Heating stage of coal
Fig. 1 shows the variations of the heating rate and of
the temperature of coal particles with time. The heating
rate decreases with time, and the temperature of coal particles increases. At very early stage, the heating rate is much

2000

1200

1600

1000

1200
800

dc = 0.8 mm
800
dc = 2.0 mm

600

Temperature / K

The well-known semi-implicit method for pressure-linked

equations (SIMPLE) scheme (Patankar, 1980) was used to
solve the equations of continuity, momentum, SGS kinetic
energy (3) and (11).
The simulated %uidized bed is 4:84 7:26 cm2 in width
and height. For the gas calculation, the bed is divided into
9 13 cells (width height). A binary mixture of particles
is initially set in the bed: the sand particle diameter is 1 mm
and 3 cases of coal particle diameter are considered: 0.8, 1.5
and 2:0 mm. The number of sand particles is 1460 and that
of coal particles is 20, and the coal and sand densities are
1100 and 2600 kg=m3 , respectively. Both initial bed temperatures of the bed and of the sand particles are 1123:15 K;
the %uidization gas is air at 1123:15 K and the moisture content is 1% (mass fraction), and the gas velocities are 0.4
and 0:6 m=s (umf and 1:5umf ; umf is the minimum %uidization velocity of 1 mm diameter sand). The time step for
particle motion is 2 105 s. The fuel analysis of coal is
(wt% dry): C (83.0), H (5.4), N (1.4), S (1.2), Ash (3.0),
Moisture (2.6).

When coal is fed into a hot %uidized bed, each coal particle
undergoes heating and combustion stages. It takes several
seconds to burn out, depending on the coal particle diameter,
oxygen concentration, %uidizing velocity, etc. However, the
simulation showed that most coal particles %oat and burn at
the bed surface after 1:5 s (see Part I). To study the e9ect of
the particle heterogeneous %ow structure on the coal combustion, heating and combustion are artiDcally separated,
i.e. the initial coal particle temperature is set as 423.15 and
1123:15 K, respectively, then %uidization begins.

Heating rate / K.s-1

2.6.5. Energy conservation for gas in a 7uid cell

The energy balance is written as follows:
@(f Cf Tf ) @(f Cf u f; i Tf )
+
@t
@xi
 

f t  @Tf
@
 +f +
+ q;
=
@xi
Pr
@xi

p
RTf

400
400

0
0.0

0.5

1.0
Time / s

1.5

2.0

Fig. 1. Variations of the temperature and heating rate of coal particles

with time.

4210

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

Power exchange rate /J.s-1

3.0x10-4

2.0x10-4
(2)

(1)x10

1.0x10-4

Pyrolysis rate / kg.s-1

1.0x10-7

combustion (1) radiation (2)

convection (3) collision (4)

8.0x10-8

800
(3)
(2)

2.0x10-8

1.0

1.5

2.0

200

0.0
0.5

2.5

1.0
1.5
Time / s

2.0

2.5

Fig. 3. Coal pyrolysis during the heating stage (dc0 = 1:5 mm).

Time / s

1800

3200

1600

2400
Sample 1
1600

1400
Sample 2

800

1200

Heating rate/K.s-1

Temperature /K

Fig. 2. Contributions of the di9erent power exchanges for all the coal
particles during the heating stage (dc0 = 1:5 mm).

higher for small particles (the heating rates are 1627, 621,
and 432 K=s for coal diameter of 0.8, 1.5, and 2:0 mm,
respectively). Moreover, the temperature and heating rate
of coal particles increase with the gas inlet velocity because of the higher gasparticle convective heat transfer
(Eq. (8)). After 2 s for a given particle diameter, the temperature range of the coal particles is very narrow. For
example, it ranges from 1137.2 to 1140:6 K for 0:8 mm
coal particles and from 875.7 to 881:6 K for 2:0 mm coal
particles. The simulation shows that it is reasonable to
separate the heating and burning stages. The larger the
coal particle diameter, the lower the temperature of coal
particles after 2 s. The mean temperatures of coal particles are 1133:0 K (0:8 mm); 989:0 K(1:5 mm)m and
878:0 K (2 mm), respectively.
Fig. 2 plots the instantaneous contributions of the four
power exchanges, i.e., heat of coal combustion, radiation,
convection and collision, for the whole set of coal particles.
The heat of combustion is small due to the very low temperature of coal particles, and so does the heat of collision in
comparison to the contributions of radiation and convection,
which are about ten-fold bigger. The collision heat transfer
%uctuates and it decreases with time because of the discontinuous coalsand particle collisions and because of the decreasing temperature di9erence between coal and sand. The
instantaneous contribution of collision ranges from 0% to
2.6%. The maximum contributions increase with the coal
particle diameter (2.0% and 3.4% for 0.8 and 2:0 mm, respectively) and the inlet gas velocity (4.2% for 0:6 m=s).
Fig. 3 plots an example of coal pyrolysis and combustion
during the heating stage (particle diameter is 1:5 mm). The
volatiles release very quickly (less than 2 s). The maximum
release rate of CO2 is at the very early stage (about 0:25 s)
whereas it is about 1 s for CO and the curve is more %at.
There are two peaks for the CO2 release because the release
rate depends on the coal temperature and its heating rate, but
also on the time. The burning point of coal is about 800 K.

400
(1)

0.0

0.5

600

4.0x10-8

0.0
0.0

1000

6.0x10-8

(4)x10

(3)

1200
CO (1)
CO2 (2)
Temperature of coal particle (3)

Temperature of the coal particle/ K

4.0x10-4

0
1000

0.0

0.5

1.0

1.5

2.0

Time / s
Fig. 4. Variations of the temperature and heating rate of coal particles
with time during the combustion (dc0 = 1:5 mm).

3.2. Combustion stage of coal

Both the temperature and the heating rate may vary a lot
during the combustion of coal particles (Fig. 4). As can be
seen, the considered samples behave similarly in the Drst
half of second; then Sample 1 is heated very fast, especially
after 1:5 s, and its heating rate %uctuates strongly. On the
contrary, the temperature of Sample 2 increases smoothly
and reaches a plateau after 1 s. This results in a very big
di9erence in particle temperature (1738 K for Sample 1,
1180 K for Sample 2, after 2 s). This points out that the
thermal characteristics of burning coal particles may di9er
strongly, even if the initial conditions are almost the same.
Fig. 5 plots the instantaneous contributions of the four
power exchanges for the whole set of coal particles during
their combustion. The heat of combustion is the largest; the
contribution of radiation is somewhat larger that of convection, and the collision heat transfer is much smaller than all
others. The collision heat transfer %uctuates with time and
its instantaneous contribution ranges from 0% to 0.8%. So,
the simulation shows that the contribution of the particle
collisions on the heat transfer is lower during the coal combustion than during the heating stage. Moreover, depending

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

Power exchange rate /J.s-1

4.0x10-4
combustion (1)
radiation (2)
convection (3)
collision (4)

3.0x10-4

(1)

2.0x10-4
(2)

(4)x20
1.0x10-4

(3)

0.0
0.0

0.5

1.0
Time / s

1.5

2.0

Fig. 5. Instantaneous contributions of the four di9erent power exchanges

during the combustion (dc0 = 1:5 mm).

750
Time =1 s
Time =2 s

Excess temperature / K

600

450
164.0 K

300

72.7 K

4211

bottom (air injection) and it decreases along the bed height.

Oppositely, CO2 concentration is very low at the bottom
and it is always higher in the upper part of the bed, especially in its center. CO concentration is very high in the
regions of coal particles due to coal combustion, then it decreases because of the CO and O2 reaction. NO concentration is always higher than that of N2 O in most part of the
bed, except for the regions of coal particles. The local maximum concentrations of NO and N2 O are 41.2 and 49:2 ppm
at 1 s, respectively.
Fig. 8 plots the gas species concentrations at the outlet
of the %uidized bed versus time. O2 concentration decreases
regularly. Both CO and CO2 concentrations increase regularly at early stage (t 1:4 s), then CO2 concentration decreases, whereas CO concentration increases sharply. The
temperature of some coal particles increases rapidly, thus
resulting in more CO and less CO2 production during the
combustion (see reaction A). Moreover, because of the small
size of the simulated %uidized bed (height = 7:26 cm), CO
does not have enough time to burn o9 before it exhausts.
N2 O concentration increases slightly (t 1:4 s) then it decreases because of the CO and N2 O reaction (see reaction
H), around coal particles. NO concentration increases %uctuating. The higher the temperature of the coal particle, the
higher the NO production (see reaction B). On the contrary,
the higher the temperature of the coal particle, the higher
the reduction of NO at the surface of coal particles (see
reaction E).

150

3.3. In7uence of the diameter of coal particle

0
0

10
15
Series of particle number

20

Fig. 6. Excess temperature of the coal particles at di9erent times

(dc0 = 1:5 mm).

on the coal particle, the absolute values for the same heat
transfer mode may vary up to almost tenfold.
The temperature of coal particles is always higher than
the bed temperature (Fig. 6). The maximum excess temperature is 105:0 K at 1 s, it reaches 614:0 K at 2 s. The
mean excess temperature increases with time, whereas the
bed temperature remains almost constant. The mean excess
temperatures are 72.7 and 164:0 K at 1 and 2 s, respectively.
The standard deviation of the temperature of coal particles
is 17.6 at 1 s and it increases to 141.2 at 2 s, which indicates
that the temperature of coal particles can vary strongly, and
the range widens strongly with time: It is 58:3 K at 1 s, and
559:0 K at 2 s. This big temperature di9erence results from
the di9erent routes followed by the coal particles, where the
O2 concentration, the gas velocity, the in%uence of other
coal particles, : : : may vary deeply.
Fig. 7 shows the distributions of the gas species at 1 s
in the %uidized bed. The O2 concentration is higher at the

The contributions of radiation and convection are comparable whatever the diameter and the contribution of collision
decreases slightly with the diameter (the maximum contributions are 1.1% for dc0 =0:8 mm and 0.8% for dc0 =2:0 mm).
So, the heat transfer due to particle collisions is always very
weak during the coal combustion.
Fig. 9 shows that the coal particle temperature is much
higher than the bed temperature. The di9erence ranges between 93.0 and 142:0 K for the three diameters of coal particles after 2 s. The maximum excess temperature is 274.0,
614.0 and 229:0 K for the diameter of 0.8, 1.5 and 2:0 mm,
respectively. The mean temperature and the excess temperature of coal particles are the highest when the diameter
of coal is 1:5 mm. The simulation shows that the heating
rate of coal particle does not vary inversely to the diameter
during the combustion stage, contrary to the heating stage.
Radiation and convection heating transfers, which increase
with the diameter, dominate during the heating. However,
the heat of combustion is larger during combustion; it depends mainly on the coal temperature and on its diameter,
but also on O2 and H2 O concentrations.
The combustion rate per unit mass is the same whatever
the particle diameter when the temperature of coal particle
is low ( 1400 K) then a di9erence exists, which increases

4212

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

CO

O2

0.023

0.11

0.023

0.05

0.10

0.11

0.10 0.11

0.07

0.09

0.10

0.10

0.07

0.14

0.130.14

0.09

0.0230.11
0.05

0.16

0.09

0.05

0.05

0.18 0.21
0.22

0.19

0.07
0.11

0.16

CO2

N2O

NO

0.16

0.18

1.4E-5

8E-6

0.18
0.16

1.6E-5
9E-6

0.14

9E-6
2.3E-5

0.12
0.10

0.060.08

2.3E-5

0.04
0.020

9E-6
1.4E-5
1.8E-5

2.7E-5 1.4E-5
2.3E-5
9E-6

2.7E-5
4.5E-6

0.08

3.2E-5

1.8E-5
1.8E-5

2.4E-5

3.2E-5
3.2E-5

4E-53.2E-5
1.6E-5
8E-6
4.8E-5

1.8E-5

2.4E-5

1.6E-5
2.4E-5

2.3E-5

NO and N2O concentration (mg.m-3)

0.24

CO concentration (mg.m-3)

0.20
O2

0.16
0.12

CO2

10
8

3x104

0.08

2x104

0.04

N2O

1x104

0.00

CO

0.0

0.5

1.0
Time / s

1.5

dc0 = 0.8 mm,

dc0 = 1.5 mm,
dc0 = 2.0 mm,

600

4x104

NO

700

12 5x104

Excess temperature / K

O2 and CO2 concentration (vol %)

Fig. 7. Instantaneous gas species (O2 ; CO2 , CO, NO, and N2 O) distributions (mass fraction, time = 1:0 s).

Tmean = 142.0 K
Tmean = 164.0 K
Tmean = 93.0 K

500

400

300

200

2.0

Fig. 8. Gas species at the outlet of the %uidized bed.

100

0
0

10

15

20

Series of particle number

with temperature (Fig. 10). The combustion rate decreases

for dc0 = 1:5 mm after 1:8 s because of the decrease of O2
concentration surrounding the coal particles. The temperature of coal particles (or the combustion rate) increases
very rapidly after it reaches a threshold temperature. For

Fig. 9. Excess temperature for di9erent diameters of coal particles

after 2 s.

example, it takes about 1:75 s for the temperature of coal

particle (1:5 mm) to increase from 1123.15 to 1430:0 K, but
only 0:25 s from 1430.0 to 1738:0 K.

3000

3.0

2500

2.5

2000

2.0

1500

1.5

4213

280

1000
500

1.0
dc0= 1.5 mm

dc0 = 0.8 mm

0.5
0.0

1100 1200 1300 1400 1500 1600 1700 1800

Excess temperature / K

240
Time / s

Combustion rate per unit mass / s-1

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

200
160
120
80

Temperature / K
Fig. 10. Temperature of coal particles versus combustion rate and time.

72

40
0

10
15
Series of particle number

20

Fig. 12. Excess temperature of the di9erent coal particles after 1 s

(dc0 = 0:8 mm, bed temperature = 1173:15 K; uf0 = 0:6 m s1 ).

0.6 m/s
0.4 m/s

Excess temperature / K

68

4. Discussion
64

60

56

52

10

15

20

Series of particle number

Fig. 11. E9ect of the inlet gas velocity on the excess temperature after
1 s (dc0 = 0:8 mm, bed temperature = 1123:15 K).

3.4. In7uence of the 7uidizing gas velocity and of the bed

temperature
The excess temperature decreases when the inlet gas velocity increases because of increasing convection (Fig. 11).
The contribution of the collision heat transfer is lower at
0:4 m=s (0:7%) than at 0:6 m=s (1:1%). This is due to the
increase of the relative particle collision velocity.
Fig. 12 shows the excess temperature of the di9erent coal
particles when the bed temperature is 1173:15 K. The mean
excess temperature is much higher when the bed temperature is 1173:15 K than when it is 1123:15 K. They are 61.0
and 134:0 K at 1 s, respectively. The temperature of coal
particles ranges from 1253.0 to 1372:0 K (bed temperature
1173:15 K) and from 1178.0 to 1189:0 K (bed temperature
1123:15 K). The heating rate increases strongly although
the bed temperature increases of only 50 K. That-is-to-say,
the burn-out time of coal particles is signiDcantly reduced
when the bed temperature increases.

Much e9ort has been devoted to measure the temperature of burning coal particles in %uidized bed combustors
(LaNauze et al., 1987; Linjewile et al., 1994; Joutsenoja
et al., 1999). All authors observed that the coal particle
temperature is much higher than the bed temperature. For
example, Linjewile et al. (1994) found that the average temperature of petroleum coke particle exceeded the bed temperature by 60360 K. Joutsenoja et al. (1999) showed that
the average char particle temperature exceeded the bed temperature by about 100200 K, whereas the maximum char
particle temperature was nearly 600 K above the bed temperature. Although our simulation conditions (e.g. the particle number, particle size distribution, simulation time, etc.)
are di9erent from their operating conditions because of the
computer capacity limitations, the temperature of coal particles is in qualitative agreement with these experimental data.
They agreement is better than with the results of Rong and
Horio (1999) who simulated char combustion in a bubbling
%uidized bed. They found that the maximum temperature of
char particles was about 50 C 5 C higher than the average bed temperature, which is much lower than the experimental measurements. Their model seems to overestimate
the particleparticle heat conduction.
5. Conclusions
Coal combustion was numerically studied at the particle
level in a bubbling %uidized bed. The mathematical model
is based on the discrete element method (DEM) model with
heat transfer and chemical reactions. The model predicts the
e9ects of the particle heterogeneous %ow structure on the
thermal characteristics of coal particles when heating and

4214

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

burning, and the gaseous emissions from a %uidized binary

mixture of sand and coal.
It is reasonable to calculate the heating and combustion
stages separately. The initial instantaneous heating rates are
1627 and 432 K=s for coal fed into a hot %uidized bed (coal
particle diameter of 0.8 and 2:0 mm, respectively), and the
rates decrease with time. Heating rates are very di9erent
during combustion. They may be very large or even negative depending on the local conditions surrounding the coal
particle. The instantaneous contribution of the collision heat
transfer is weak, less than 5.0% and 1.5% of the total heat
transfer during the heating and the combustion stages, respectively. The temperature of coal particles is much higher
than the bed temperature for di9erent conditions. This is in
qualitative agreement with experimental data from literature.
The model also predicts the devolatilization of coal, the gas
species distribution in the %uidized bed, and the emissions
at the outlet.

Notation
A; B; C; D
Ap
Cf
CH2 O
CNO
CN 2 O
CCO
CO 2
Cp
dp
Di
EA
fp
G
Gi
hp
kA ; kB ; : : : ; kJ
k0
m
mp
N
Qc
Qcoll
Qcomb
Qr
r
R
RA ; RB ; : : : ; RJ
t
Tb
Tf

constants in Eq. (2)

particle surface area, m2
heat capacity of the gas, J=(kg K)
oxygen concentration, mol m3
NO concentration, mol m3
N2 O concentration, mol m3
CO concentration, mol m3
O2 concentration, mol m3
heat capacity of particle, J=(kg K)
particle diameter, m
di9usion coeQcient, m2 s1
apparent activation energy, J mol1
speciDc internal surface area of the char,
m1
average Young moduli, GPa
Young moduli, GPa
heat transfer coeQcient, J=(m2 s)
rate constant of reactions, s1
pre-exponential factor in Eq. (1), s1
average mass of particle, kg
mass of particle, kg
order of reaction in Eq. (1)
convective heat transfer, J s1
collision heat transfer, J s1
heat of combustion, J s1
radiation heat transfer, J s1
average radius, m
ideal gas constant, (8:314 J mol1
K 1 )
reaction rate, mol m3 s1
time, s
bed absolute temperature, K
gas absolute temperature, K

Tp
TR
u f
umf
vpn
Vpyrol

Vpyrol
Wi
Yi
Ymi

particle absolute temperature, K

heating rate, K s1
Dltered gas phase velocity, m s1
minimum %uidization velocity, m s1
normal relative velocity, m s1
mass fraction of volatiles evolved up to
time t
limit value of Vpyrol as t
molecular weight, kg mol1
local mass fraction of species
local mole fraction of species

Greek letters

(i

Rt
RT
Rx
Ry
&p
+f
+p
t

f
p
!
!S B

primary CO=CO2 product ratio

Poisson ratio
porosity in %uid cell
time step, s
mean excess temperature, K
x direction mesh spacing, m
y direction mesh spacing, m
emissivity of the particle
gas conductivity, J=(s m K)
particle conductivity, J=(s m K)
SGS kinetic gas viscosity, m2 s1
gas density, kg m3
particle density, kg m3
turbulent Schmidt number, ! = 0:7
StefanBoltzmann constant

Subscripts
c
s
0

coal
sand
initial

References
Adanez, J., Abanades, J.C., 1992. Modeling of lignite combustion in
atmospheric %uidized bed combustors, 1. Selection of submodels and
sensitivity analysis. Industrial Engineering and Chemical Research 31,
22862296.
Allen, M.T., Yetter, R.A., Dryer, F.L., 1997. High pressure studies of
moist carbon monoxide/nitrous oxide kinetics. Combustion and Flame
108, 449470.
Amand, L.E., Andersson, S., 1989. Emissions of nitrous oxide (N2 O)
from %uidized bed boilers. In: Proceedings of the 10th International
Conference on Fluidized Bed Combustion. ASME, pp. 4955.
Bonn, B., Pelz, G., Baumann, H., 1995. Formation and decomposition of
N2 O in %uidized bed boilers. Fuel 74 (2), 165171.
Canu, P., 2001. Simulation and interpretation of catalytic combustion
experimental data. Catalysis Today 64, 239252.
Chan, L.K., SaroDm, A.F., Beer, J.M., 1983. Kinetics of NO-carbon
reaction at %uidized bed combustion conditions. Combustion and Flame
52, 3744.
Chen, Z., Lin, M., Ignowski, J., Kelly, B., Linjewile, T.M., Agarwal,
P.K., 2001. Mathematical modelling of %uidized bed combustion.

H. Zhou et al. / Chemical Engineering Science 59 (2004) 4205 4215

4: N2 O and NOx emissions from the combustion char. Fuel 80,
12591272.
Delvosalle, C., Vanderschuren, J., 1985. Gas-to-particle and
particle-to-particle heat transfer in %uidized beds of large particles.
Chemical Engineering Science 40 (5), 769779.
De Soete, G.G., Croiset, E., Richard, J.R., 1999. Heterogeneous formation
of nitrous oxide from char bound nitrogen. Combustion and Flame
117, 140154.
Donskoi, E., McElwain, D.L.S., 1999. Approximate modelling of coal
pyrolysis. Fuel 78, 825835.
Dryer, F.L., Glassman, I., 1973. High temperature oxidation of CO
and CH4 . Prov. 14th Symposium (International) on Combustion, The
Combustion Institute, Pittsburgh, PA, pp. 957963.
Field, J.A., Gill, D.W., Morgan, B.B., Hawksley, P.G.W., 1967.
Combustion of pulverized coal. BCURA, Leatherhead.
Flamant, G., Lu, J., Variot, B., 1993. Towards a generalized model for
vertical walls to gassolid %uidized beds heat transferII. Radiative
transfer and temperature e9ects. Chemical Engineering Science 48
(13), 24932503.
Hautman, D.J., Dryer, F.L., Schug, K.p., Glassman, I., 1981.
A multiple-step over kinetic mechanism for the oxidation of
hydrocarbons. Combustion Science Technology 25, 219232.
Hobbs, M.L., Radulovic, P.T., Smoot, L.D., 1992. Modelling Dxed-bed
coal gasiDer. A.I.Ch.E. Journal 681702.
Jensen, A., Johnsson, J.E., Andries, J., Laughlin, K., Read, G., Mayer,
M., 1995. Formation and reduction of NOx in pressured %uidized bed
combustion of coal. Fuel 74 (11), 15551569.
Johnsson, J.E., 1994. Formation and reduction of nitrogen oxides in
%uidized-bed combustion. Fuel 73, 13891415.
Joutsenoja, T., Heino, P., Hernberg, R., 1999. Pyrometric temperature
and size measurements of burning coal particles in a %uidized bed
combustion reactor. Combustion and Flame 118, 707717.
Kilpinen, P., Hupa, M., 1991. Homogenous N2 O chemistry at %uidized
bed combustion conditionsa kinetic modeling study. Combustion
and Flame 85, 94104.
Krammer, G.F., SaroDm, A.F., 1994. Reaction of char nitrogen during
%uidized bed coal combustionin%uence of nitric oxide and oxygen
on nitrous oxide. Combustion and Flame 97, 118124.
LaNauze, R.D., Jung, K., Dent, D.C., Joyce, T., 1987. Measurement of the
temperature of burning particles in %uidized bed. Ninth International
Conference on Fluidized Bed Combustion, ASME, pp. 707712.
Lathouwers, D., Bellan, J., 2001. Modeling of dense gassolid reactive
mixtures applied to biomass pyrolysis in a %uidized bed. International
Journal of Multiphase Flow 27, 21552187.
Li, J., Mason, D.J., 2000. A computational investigation of transient
heat transfer in pneumatic transport of granular particles. Powder
Technology 112, 273282.

4215

Linjewile, T.M., Hull, A.S., Agarwal, P.K., 1994. Optical probe

measurements of the temperature of burning particles in %uidized beds.
Fuel 73 (12), 18801888.
Massman, W.J., 1998. A Review of the molecular of di9usivities of
H2 O; CO2 ; CH4 , CO, O3 ; O2 ; NH3 ; N2 O, NO, and NO2 in air, O2
and N2 NEAR STP. Atmospheric Environment 32 (6), 11111127.
Palchonok, G.I., Breitholtz, C., Thunman, H., Leckner, B., 1997. Impact
of heat and mass transfer on combustion of a fuel particle in CFB
boilers. 14th International Conference on Fluidized Bed Combustion,
ASME, pp. 871878.
Patankar, S.V., 1980. Numerical Heat Transfer and Fluid Flow.
Hemisphere, New York, USA.
Peirano, E., Leckner, B., 1988. Fundamentals of turbulent gassolid %ows
applied to circulating %uidized bed combustion. Progress in Energy
and Combustion Science 24 (4), 259296.
Rajan, R.R., Wen, C.Y., 1980. A comprehensive model for %uidized bed
coal combustors. A.I.Ch.E. Journal 26, 642655.
Ranz, W.E., 1952. Friction and transfer coeQcients for single particles
and packed beds. Chemical Engineering Progress 48, 247253.
Rong, D., Horio, M., 1999. DEM simulation of char combustion in a
%uidized bed. Second International Conference on CFD in the Minerals
and Process industries. CSIRO, Melbourne, Australia, pp. 6570.
Saxena, S.C., 1990. Devolatilization and combustion characteristics of
coal particles. Progress in Energy and Combustion Science 15, 5594.
Smoot, L.D., 1993. Fundamentals of Coal Combustion. Elsevier, The
Netherlands.
Solomon, P.R., Fletcher, T.H., Pugmire, R.J., 1993. Progress in Coal
Pyrolysis. Fuel 72 (5), 587596.
Stubington, J.F., Sasongko, J.F., 1998. On the heating rate and volatile
yield for coal particles injected into %uidized bed combustors. Fuel
77, 10211025.
Sun, J., Chen, M.M., 1988. A theoretical analysis of heat transfer to
particle impact. International Journal of Heat and Mass Transfer 31
(3), 969975.
Tripathi, A., Vaughn, C.L., Maswadeh, W., Meuzelaar, H.L.C., 2002.
Measurement and modeling of individual arbonaceous particle
temperature proDles during fast CO2 laser heating Part 1. Model char.
Thermochimica Acta 183197.
Zhou, H., Abanades, S., Flamant, G., Gauthier, D., Lu, J., 2002. Simulation
of heavy metal vaporization dynamics in a %uidized bed. Chemical
Engineering Science 57, 26032614.
Zhou, H., Flamant, G., Gauthier, D., 2004. DEM-LES simulation of
coal combustion in a bubbling %uidized bed. Part I: gasparticle
turbulent %ow structure. Chemical Engineering Science, this issue
(doi:10.1016/j.ces.2004.01.069).