Fuel 86 (2007) 722–734

www.fuelfirst.com

Numerical simulation of the bubbling fluidized bed coal gasification

by the kinetic theory of granular flow (KTGF)
a,b a,b a,* a,*
Liang Yu , Jing Lu , Xiangping Zhang , Suojiang Zhang
a
Research Laboratory of Green Chemistry and Technology, Institute of Process Engineering, Chinese Academy of Sciences, 100080 Beijing, China
b
Graduate University of Chinese Academy of Sciences, 100049 Beijing, China

Received 8 May 2006; received in revised form 8 September 2006; accepted 13 September 2006
Available online 10 October 2006

Abstract

A new numerical model based on the two-fluid model (TFM) including the kinetic theory of granular flow (KTGF) and complicated
reactions has been developed to simulate coal gasification in a bubbling fluidized bed gasifier (BFBG). The collision between particles is
described by KTGF. The coal gasification rates are determined by combining Arrhenius rate and diffusion rate for heterogeneous reac-
tions or turbulent mixing rate for homogeneous reactions. The flow behaviors of gas and solid phases in the bed and freeboard can be
predicted, which are not easy to be measured through the experiments. The calculated exit values of gas composition are agreed well with
the experimental data. The relationship between gas composition profiles with the height of gasifier and the distributions of temperature,
gas and solid velocity and solid volume fraction were discussed.
 2006 Elsevier Ltd. All rights reserved.

Keywords: Bubbling fluidized bed coal gasifier; Two-fluid model; Kinetic theory of granular flow

1. Introduction Since the two-phase model was firstly proposed by Too-

The oil crisis and global environmental problems have
become critical challenge worldwide, therefore more and
more attentions have been paid to the clean coal technol-
ogy, among which the coal gasification is one of the critical
technologies for the efficient utilization of coal. Comparing
to the coal combustion, there is a lower reaction rate in
coal gasification process. Therefore the bubbling fluidized
bed gasifier (BFBG) is one of widely applied technologies,
because a longer residence time, uniform temperature dis-
tribution, high mass and heat transfer rates could be
achieved in such kind of reactor. However, it has been a
challengeable problem to scale-up the fluidized bed coal
process due to its complicated reaction and transfer mech-
anism [1].
*
Corresponding authors. Tel./fax: +86 10 82627080.
E-mail addresses: xpzhang@home.ipe.ac.cn (X. Zhang), sjzhang@
home.ipe.ac.cn (S. Zhang).
mey and Johnstone [2], many improvements have been
developed to simulate the coal gasification process of the
bubbling fluidized bed [3–7]. However, the inherently
existed drawbacks are impossible to be solved due to its
empirical nature in the description of gas and particle in
motions and interactions without solving the momentum
balance equations.
In recent years, mass conservation and momentum bal-
ance for gas and solid have been applied to simulate the
hydrodynamics of bubbling fluidized bed. Two approaches
have been proposed, one is based on molecular dynamics,
called discrete element method (DEM), and another is
based on the assumption that the gas and particulate
phases form two inter-penetrating continua, called two-
fluid model (TFM) [8]. A characteristic feature of bubbling
fluidized bed is the chaos motion of large numbers of
particles in the bed. So the fundamental procedure is to
closure complex particle stresses resulted from multi-body
collisions.

0016-2361/$ - see front matter  2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.fuel.2006.09.008
 L. Yu et al. / Fuel 86 (2007) 722–734 723

Nomenclature

A constant T gas mixture mean temperature, K

B constant T0 reference temperature, K
Cp,i heat capacity, J/kg K U the instantaneous velocity, m/s
Cd drag coefficient u the mean velocity, m/s
Dm,i diffusion coefficient of the mixture, m2/s u0 the fluctuating velocity, m/s
Di,j binary mass diffusion coefficient, m2/s wi molecular weight, kg/kmol
e coefficient of restitution Xi molar fraction
g gravity, m/s2 Yi the mass fraction
g0 radial distribution function
H specific enthalpy, J/kg Greek symbols
Hi enthalpy, J/kg a mixture thermal conductivity, W/m K
DHf,i enthalpy of formation, J/kg c dissipation of fluctuating energy, W/m3
hgs heat transfer coefficient, W/m2 K e dissipation rate of turbulent kinetic energy,
Jg,i diffusion flux, kg/m2 s m2 s3
KAr kinetic rate constant Hs granular temperature, (m/s)2
KEBU turbulent mixing rate constant j turbulent kinetic energy, m2/s2
KHom homogeneous rate constant ks bulk viscosity, Pa s
ks diffusion coefficient for granular energy, kg/m s l viscosity, kg/m s
Nu Nusselt number q density, kg/m3
Pk,g shear production re turbulent Prandtl number for e
Pr the continuous phase Prandtl number rj turbulent Prandtl number for j
p gas pressure, Pa rY Schmidt number
Q intensity of heat exchange between the gas and s stress tensor, Pa
solid phases, W/m2 Ugs drag, kg/m3 s
R universal gas constant, J/kmol K
Re Reynolds number Subscripts
Rg,i net rate of production of homogeneous species i g gas phase
Rs,i the heterogeneous reaction rate i the ith species
r volume fraction l laminar flow
S source term m mixture
Sh Shawood number s solid phase
SP,j associated stoichiometric coefficients of prod- t turbulent flow
ucts.
SR,i associated stoichiometric coefficients of reac-
tants

Based on DEM, the soft sphere simulation by means of
the empirical coefficient of restitution and friction and the
hard sphere simulation by means of empirical spring stiff-
ness and a friction coefficient were performed to describe
particle collisions and to predict frequency of pressure fluc-
tuations, bubble formation and particles segregation [9–
12]. However, if one requires modeling complex industrial
systems like the BFBG with the millions of particles, many
computational practices indicate that huge computational
times put DEM at a disadvantage [8,13]. On the contrary,
TFM cannot only save computational time, but obtain the
mean particulate flow fields which are convenient to facili-
tate quantifiable decisions for an engineering design. Com-
putational simulations done by several group in many
countries have been shown it is feasible to compute the
observed bubbles and clusters and the flow regime using
TFM [14].
By analogy with the kinetic theory of gas molecules to
improve the description of particle collision, the kinetic
theory of granular flow (KTGF) was introduced into
TFM [15]. Many people who participate in modeling
gas–solid flows in fluidized beds and risers use kinetic the-
ory of granular flow to predict and validate lots of flow
phenomena in the systems of dilute phases and dense
phases, e.g., [16–18]. Applying KTGF into bubbling fluid-
ized bed model, Enwald and Almstedt [19] compared
numerical solutions with experimental results using four
different two-fluid model closures, and obtained the statis-
tical consistency of bubble frequency, mean pierced bubble
length, mean bubble rise velocity and mean bubble volume
fraction. According to this literature, our group carried out
the similar TFM to investigate fluid dynamics in a gas–
solid bubbling fluidized bed [20], and concluded that it is
a success for the simulation of bubble characteristics using
724 L. Yu et al. / Fuel 86 (2007) 722–734
Enwald’s method. Critical comparison of hydrodynamic
models for jet bubbling fluidized beds and freely bubbling
fluidized beds, Patil et al. [21,22] came to the conclusion
that the KTGF was in good agreement with the experimen-
tal data and correlations from the literature compared to
the constant viscosity model (CVM) for the prediction of
bubble size distribution, bubble rise velocity, and visible
bubble flow rate. It is more importance that KTGF can
be applied into the wider variety of cases due to no assump-
tion of solid phase viscosity.
Although KTGF based on TFM has given a reasonable
flow description of dense gas–solid flows, it is difficult that
the complicated chemical reactions are introduced to simu-
late the bubbling fluidized gasification process due to com-
plex mechanism of heat transfer and chemical reaction
need to be modeled. More careful consideration has to be
given on the solution of large numbers of energy and spe-
cies transport equations and the nonlinear source term of
complicated chemical reactions. However, the scale-up
and optimal design of industrial reactors cannot be carried
out without considering chemical reaction. Until now, not
much effort has been devoted to couple multi-phase flow
with complex gasification in the bubbling fluidized bed.
In this work, TFM, which includes KTGF and chemical
reaction kinetics, is extended to simulate the bubbling
fluidized bed coal gasification. Particles collision and fluc-
tuation in the bed can be described by KTGF. The compli-
cated coal gasification process includes a system of 15
species and 11 chemical equations. The devolatalization
and drying can be considered as instantaneous process in
feed zone, and the proportion of products distribution is
derived from pyrolysis results in the experiment [23–25].
Heterogeneous reaction rates are determined by kinetics
and diffusion and the mass, momentum and heat exchange
between gas and solid phases are caused by the reactions.
Homogeneous reactions are controlled by the smaller one
of Arrhenius rate and eddy-dissipation rate presented by
D.B. Spalding [26]. With proposed model, the exit simula-
tion results are compared with experimental data [7] and
the relationship between composition profile with tempera-
ture profile and coal volume fraction can be obtained.
2. Mathematical model
2.1. Main assumptions on coal gasification process
In order to decrease the impact of the strong nonlinear
characteristic of the model and ensure the good conver-
gence and acceptable computational time, the gas–solid
hydrodynamic and coal gasification models are simplified
as follows:
(1) The vertical section of BFBG is rectangular, which
can be assumed as two-dimensional. The 2D flow
behavior has been verified by comparing the experi-
mentation with CFD [27–29]. The frictional stresses
models are not taken into account by TMF equations
in here and their actions on flow behavior will be
compared in next work. Other interaction forces such
as lift force, thermophoretic force, Brownian force
and virtual mass force are neglected.
(2) The intensity of particles collision does not vary with
temperature, i.e., exothermic or endothermic reaction
has no impact on the fluctuation of solid velocity and
does not have a rise in the temperature of granular.
(3) The coal gasification is an overall endothermic and its
temperature is lower than that of combustion. The
heat for gasification should be supplied. The solid
phase is dense and continuous in the bed, and contact
with the wall, in which the mean free path of radia-
tion is much smaller than the solid dimensions so as
to limit the contribution of radiative heat transfer.
The gas phase is also continuous in the freeboard
and can be assumed as transparent so that the radia-
tive energy is neither absorbed nor emitted [25]. The
bed temperature will be uniform rapidly due to strong
agitation of particles. There is not much temperature
difference to drive radiative heat transfer among the
particles. Thus it is reasonable to assume that the
heat loss by radiation is negligible.
(4) Particle is isothermal. The particles are assumed
inelastic, smooth and monodispersed spheres.
2.2. Gas–solid hydrodynamics
The general model of multiphase flow was derived from
Eulerian–Eulerian approach, and developed to describe the
flow behavior of the BFBG based on conservation equa-
tions for mass and momentum for both gas and solid
phase.
2.2.1. Continuity equations
The continuity equations for gas and solid phases are
given by
o
ðrg qg Þ þ r  ðrg qg U g Þ ¼ S gs ð1Þ
ot
o
ðrs qs Þ þ r  ðrs qs U s Þ ¼ S sg ð2Þ
ot
where r, q and U are the volume fraction, the density and
the instantaneous velocity, respectively. In a laminar field,
the entire field of values is either time-steady or changing
systematically. Thus the instantaneous velocity of particles
Us can be substituted by the solid mean velocity us. This
form was also derived from the Boltzmann integral–differ-
ential equation by Ding and Gidaspow [30]. Even for gas
phase of continuity equation, ug can take the place of Ug
due to Reynolds averaging, which will be described in
detail at Section 2.2.4. S on the right-hand side is the source
term and set to zero only in flow field [31,32]. When the
continuity equations are used in heterogeneous reaction,
there is the mass, momentum and heat exchange between
gas phase and solid phase. In the present work, coal reacts
 L. Yu et al. / Fuel 86 (2007) 722–734 725

with oxygen, steam and carbon dioxide to change solid where Hs is granular temperature; e is the coefficient of res-
phase into gas phase, so mass source for the phases yield titution for particle collisions; g0 is the radial distribution
X function.
S sg ¼ wC cC RC ¼ S gs ð3Þ For the restitution coefficient, the different values were
For the gas phase density, a mixture of ideal gas was presented, from 0.8 to 1 in the literature [22,33,34]. In this
assumed work, a restitution coefficient value of 0.9 was used due to
the fact that the granular diameter of 0.62 mm is close to
p that of 0.7 mm in the literature [35]. For the radial distribu-
qg ¼ Pn Y i ð4Þ
RT i¼1 wi tion function of solid phase, g0 is expressed as [16]
"  1 #1
where p, T, Yi and wi are gas pressure, gas mixture mean 3 rs 3
temperature, mass fraction and the molecular weight for g0 ¼ 1 ð12Þ
5 rs;max
every species, respectively. The solid phase density is as-
sumed as constant. The granular temperature Hs is a pseudo-temperature
which can be defined as
2.2.2. Momentum equations 3 1
The momentum equation for gas phase can be written as Hs ¼ hu0s u0s i ð13Þ
2 2
o where u0s is the fluctuating velocity of the particles and can
ðrg qg U g Þ þ r  ðrg qg U g U g Þ
ot be derived from
¼ rg rp  Ugs ðU g  us Þ þ ðr  rg sg Þ þ rg qg g þ S gs us
u0s ¼ U s  us ð14Þ
ð5Þ
where Us is the instantaneous velocity of the particles. The
where Ugs is the drag coefficient between the gas phase and solid mean velocity us is defined as
solid phase, and g is gravity. The stress tensor sg is given by Z
1
us ¼ hU s;i i ¼ U s;i f dU s ð15Þ
2 n
sg ¼ ll;g ðrU g þ rU Tg Þ  ll;g r  U g ð6Þ
3 where f, n are single-particle velocity distribution function
In the right hand of Eq. (5), the fifth term Sgsus describes and particle number density respectively.
the momentum transfer of the coal. The momentum equa- The details can be obtained from Ding and Gidaspow’s
tion for the solid phase should obtain the reverse source work [30], where the derivation of the granular temperature
term and can be expressed as transport equation has been reported.
o
ðrs qs us Þ þ r  ðrs qs us us Þ ¼ rs rp  ps  Ugs ðus  U g Þ 2.2.3. Kinetic theory of granular flow (KTGF)
ot A transport equation which describes particles collide
þ ðr  rs ss Þ þ rs qs g þ S sg us ð7Þ resulting in a random granular motion is defined for solid
where the solid stress tensor ss is given by phase [21]
 
  3 o
2 ðrs qs Hs Þ þ r  ðrs qs Hs us Þ
ss ¼ ks  ls rus þ ls ðrus þ ruTs Þ ð8Þ 2 ot
3
¼ ðps I þ rsss Þ : r~
us þ r  ðk s rHs Þ  c  3Ugs Hs ð16Þ
In the equation above, ks is bulk viscosity, which can be
obtained as follow: The diffusion coefficient for granular energy ks is given by
 1=2 pffiffiffiffiffiffiffiffiffi  2
4 Hs 150qs d s Hs p 6
ks ¼ rs qs d s g0 ð1  eÞ ð9Þ ks ¼ 1 þ rs g0 ð1 þ eÞ
3 p 384ð1 þ eÞg0 5
rffiffiffiffiffiffi
and the equation of the solid shear viscosity ls is derived Hs
þ 2qs r2s d s g0 ð1 þ eÞ ð17Þ
from Gidaspow [18] p
rffiffiffiffiffiffi The dissipation of fluctuating energy due to inelastic colli-
4 2 Hs
ls ¼ rs qs d s g0 ð1 þ eÞ sion takes the form
5 p " rffiffiffiffiffiffi! #
pffiffiffiffiffiffiffiffiffi  2 4 Hs
10qs d s pHs 4 2 2
c ¼ 3ð1  e Þrs qs d s g0 Hs  rus ð18Þ
þ 1 þ g0 rs ð1 þ eÞ ð10Þ ds p
96ð1 þ eÞes g0 5
The solid pressure ps is defined in analogy with ls and con- The remaining term which needs to be considered is the
sists of a collision and a kinetic term interphase momentum transfer. It is thought for the drag
between gas phase and solid phase to play important role
ps ¼ rs qs Hs þ 2ð1 þ eÞr2s g0 qs Hs ð11Þ in the momentum exchange. If eg < 0.8, the well-known
726 L. Yu et al. / Fuel 86 (2007) 722–734

Ergun equation [36] is suitable for describing the dense o

ðrg qg jÞ þ r  ðrg qg ug jÞ
regime ot  
ð1  rg Þrs lg qg rs jug  us j lT;g
Ugs ¼ 150 þ 1:75 ð19Þ ¼ r  rg ll;g þ r  j þ rg P j;g  rg qg e ð28Þ
2
ds rj
rg d s
o
If eg > 0.8, the drag coefficient was given based on the ðrg qg eÞ þ r  ðrg qg ug eÞ
ot  
work by Wen and Yu [31] lT;g rg e
¼ r  rg ll;g þ re þ ðC e;1 P j;g  C e;2 qg eÞ
3 jug  us j 2:65 re j
Ugs ¼ C d rg ð20Þ
4 ds ð29Þ
where In these equations, Pj,g is the shear production defined by
( T 2
24
ð1 þ 0:15Re0:687 Þ Re 6 1000 P j;g ¼ lt;g rug  ½rug þ ðrug Þ   rug ðlt;g rug þ qg jÞ
Cd ¼ Re
ð21Þ 3
0:44 Re > 1000 ð30Þ
jug  us jrg qg d s and rj, re is the turbulent Prandtl numbers for j and e.
Re ¼ ð22Þ Let the model constants take these values
lg
C e;1 ¼ 1:44; C e;2 ¼ 1:92; C l ¼ 0:09; rj ¼ 1:0;
re ¼ 1:3
2.2.4. j–e turbulence models
Unlike the single-phase j–e models, there is no ‘indus-
trial standard’ model for multiphase flow to perform rea- 2.3. Coal gasification reactions
sonably well to engineering accuracy in a wide range of
application. To the bubbling fluidized bed, prediction will As part of gasification models, the complicated pro-
be in good agreement with experimental data for laminar cesses of chemical reactions were simulated and set as the
gas phase and laminar solid phase [21,22]. In the present source term of species transport equations when the reac-
work, the competition between turbulent mixing rate and tants were consumed and the products were created. The
chemical kinetic rates will be considered in the homoge- heat exchanged between gas phase and solid phase was
neous reaction. So we assume that gas phase is in turbulent taken into account by energy equations.
flow and solid phase is in laminar flow. When turbulent
flows are taken into account, the interesting is in obtaining 2.3.1. Chemical reactions
the mean values of the independent variables of interest. In this work, only char belongs to solid phase, which is
Thus the process of Reynolds decomposition may be released by coal particles and the continue equation of
employed. The instantaneous values of the independent solid phase can ensure the mass balance of char. So there
variables are represented by the sum of a time-mean value is no further species transport equation proposed for char.
and an instantaneous fluctuating value At the feed position, the drying process and the devolatal-
ization reactions take place very quickly according to
U g ¼ ug þ u0g ð23Þ
experimental results [7], so it is assumed that the pyrolytic
U¼/  þ /0 ð24Þ process of the raw coal is completed in this region. The
Eq. (5) is averaged over a sufficiently long time and yield of each product is determined by the proximate anal-
expressed as [38] ysis of the raw coal. The sum of the mass fraction of prod-
ucts is calculated to be unity in the raw coal
o
ðrg qg ug Þ þ r  ½rg qg ðug ug þ hu0g u0g iÞ Y Char þ Y Volatile þ Y Water þ Y ash ¼ 1
ot ðR1Þ
¼ rg rp  Ugs ðug  us Þ þ ðr  rg sg Þ þ rg qg g þ S gs us Coal ! Char þ Volatile þ H2 O þ Ash
ð25Þ The following chemical processes are included in the
present model: (1) pyrolysis of the released volatile, (2) het-
where long-time average of u0g and p 0 are zero and hu0g u0g i erogeneous char reactions, (3) homogeneous reactions of
is called Reynolds stress closed by gas phase.
T 2 There is no standard chemical stoichiometrically equa-
qg hu0g u0g i ¼ lt;g  ½rug þ ðrug Þ   ðlt;g rug þ qg jÞ ð26Þ
3 tion for the pyrolysis of the volatile due to its complex com-
lt,g is the turbulent viscosity and computed as a function of position. For the sake of simplification it was assumed the
j and e molecular formula of the volatile is determined by the final
pyrolysates [23–25]. In the present work, the volatile matter
j2 is composed of several species as follow:
lt;g ¼ qg C l ð27Þ
e
Volatile ! m1 CO2 þ m2 CO þ m3 H2 þ m4 CH4
The transport equations for j and e only take the gas phase
form þ m5 C2 H6 þ m6 H2 S þ m7 NH3 þ m8 tar ðR2Þ
 L. Yu et al. / Fuel 86 (2007) 722–734 727

Table 1
Homogeneous reaction and the kinetic equations
Chemical reactions Equations Units
h i
CO + H2O M CO2 + H2 Y Y
R6 ¼ K 6 Y CO Y H2 O  COK2  H2 R6 (kg m3 s1)
6
h i
2CO + O2 ! 2CO2 R7 ¼ K 6 Y CO Y 0:5
O2 gq 1:5
R7 (kg m3 s1)
K 7 1:5
2H2 + O2 ! 2H2O R8 ¼ ½Y H2 Y O2 qg2:5  R8 (kg m3 s1)
T 1:5
g
K9
CH4 + 2O2 ! CO2 + 2H2O R9 ¼ Y CH4 Y O2 q2g R9 (kg m3 s1)
Tg
K 10
2C2H6 + 7O2 ! 4CO2 + 6H2O R10 ¼ Y C2 H6 Y O2 q2g R10 (kg m3 s1)
Tg
4NH3 + 5O2 ! 4NO + 6H2O 0:86 1:04 1:9
R11 ¼ K 11 Y NH 3
Y O2 qg R11 (kg m3 s1)

The composition of tar is usually regarded as condensed- The char reaction rate is obtained as a mixture of kinetic
nuclei aromatics, so it is reasonable to further propose and diffusion controlled mass transfer rate
C6H6 instead of tar [24]. Combined the element analysis 6ðvolÞrs
of coal with the final pyrolysates, the molecular formula RC ¼ ½ðK Dif Þ1 þ ðK Ar Þ1 1 pX i ð33Þ
ds
of the volatile can be determined as C24.2H46.2O8.5N1.1S.
Although the drying and devolatalisation process is han- The different expressions of homogeneous reactions can
dled into two steps – pyrolysis of coal and volatile, it can be provided from several references, it is convenient to
be considered as an instantaneous phenomenon that we make use of Souza-Santos [25] and Chejne’s works [7],
can calculate the kinetic coefficient from the mass balance which are summarized in Tables 1 and 2. The extended
principle. work is to consider that chemistry does not play any expli-
The heterogeneous reactions between char and gases cit role while turbulent motions control the overall reaction
(O2, H2O, CO2) can be described by different reaction rate. So the chemical reaction rates are computed by
mechanisms which are take account for possible diffusion K Hom ¼ minðK Ar ; K EBU Þ ð34Þ
effect or further simplified by kinetic model. For example,
Souza-Santos [25] and Chejne and Hernandez [7] used the where KHom is homogeneous rate constant and KAr is
unreacted core model to combine reaction with diffusion kinetic rate constant; KEBU is the turbulent mixing rate
resistance. In Eaton and Smoot’s review [37], Reade et al. constant and calculated with an Eddy Break-up model
 
presented char oxidation model based on measured intrin- e Y R;i Y P;j
sic char kinetic rates and a pore diffusion model. Chen et al. K EBU ¼ A min ;B ð35Þ
j S R;i S P;j
[39] assumed that the oxygen, carbon dioxide and steam
react with char on the char particle surface and the value Here A and B are constants, SR,i and SP,j are the associated
for reaction order was 0.5. In this study, we assumed char stoichiometric coefficients of reactants and products.
particle is a spherical particle surrounded by a stagnant
boundary layer through which gas species must diffuse 2.3.2. Species transport equations
before they react with the char. The overall char reaction Gas phase is assumed as a mixture from 14 species, rep-
rate of a particle is controlled by the smaller of the rates resented by their mass fraction as follows: volatile, O2,
of diffusion and kinetic CO2, H2O, NO, CH4, H2S, H2, C2H6, CO, NH3, Tar,
Ash and N2. The conservation equations take the general
3C þ 2O2 ! CO2 þ 2CO ðR3Þ form as (36) for these chemical species but the N2, which
C þ H2 O ! CO þ H2 ðR4Þ
C þ CO2 ! 2CO ðR5Þ Table 2
Arrhenius coefficients related to the R3–R11
The diffusion rate can be derived from the definition of Reaction Equations Units
Shawood number R3 K3 = 17.9 exp[13,750/Ts] Pa1 s1
R4 K4 = 5.95 · 105 exp[13,650/Ts] Pa1 s1
ShDgs wC
K Dif ¼ ð31Þ R5 K5 = 3.92 exp[26,927/Ts] Pa1 s1
RT s d s R6 K6 = 2.78 · 103 exp[1510/Tg] kmol1 m3 s1
R6* K 6 ¼ 0:0265 exp½3968=T g  —
where Sh and R are Shawood number and the universal gas R7 K7 = 1.0 · 1015 exp[16,000/Tg] kmol0.75 m2.25 K1.5 s1
constant, respectively. For the gas, Shawood number is R8 K8 = 5.159 · 1015 exp[3430/Tg] kmol1.5 m4.5 K1.5 s1
written as R9 K9 = 3.552 · 1014 exp[15,700/Tg] kmol1 m3 K s1
R10 K10 = 3.552 · 1014 exp[15,700/Tg] kmol1 m3 K s1
Sh ¼ 2:0 þ 0:552Re1=2 Pr1=3 ð32Þ R11 K11 = 9.78 · 1011 exp[19,655/Tg] kmol0.9 m2.7 s1
728 L. Yu et al. / Fuel 86 (2007) 722–734

is computed from the fact the sum of all mass fractions is For the ideal gas, the mixture thermal conductivity is
equal to one in the gas phase computed as
o X
13
ðq rg Y g;i Þ þ rðqg rg ug Y g;i Þ X i ai
oT g ag ¼ P ð43Þ
i6¼j X j /ij
¼ r  rg J g;i þ rg Rg;i þ Rs;i ð36Þ i¼1
  1=2 
where Jg,i, Rg,i and Rs,i are the diffusion flux of species i in 1þ
li
lj
wj 1=4
ð Þ
wi
gas phase, the net rate of production of homogeneous spe- where /ij ¼ h i1=2 , Xi is the molar fraction of the
cies i and the heterogeneous reaction rate, respectively. w
8 1þw i
j
In the species transport equations of gas phase, mass dif- ith species.
fusion coefficients are used to calculate the diffusion flux of The heat exchange between phases can be expressed as a
chemical species in turbulent flow using modified Fick’s function of the temperature difference and conform to the
law local balance condition Qgs = Qsg
 
l Qgs ¼ hgs ðT g  T s Þ ð44Þ
J g;i ¼  qg Dm;i þ t r  Y g;i ð37Þ
rY
where rY is the Schmidt number, which is set as 0.7.
The diffusion coefficient of the mixture, Dm,i is calcu-
lated from the binary mass diffusion coefficient Di,j as
follow:
1  Xi
Dm;i ¼ P X j ð38Þ
j6¼i Di;j

2.3.3. Energy conservation equations

This section describes the heat transfer treatment for
multiphase flow. In our work, although the compressibility
of gas phase and solid phase are taken into account, the
flow at low Mach numbers (M  0.3) makes some approx-
imations valid. So the pressure work, kinetic terms and vis-
cous heating are negligible. The energy transport equations
are solved for the specific enthalpy of gas phase and solid
phase, which take the form
o
ðrg qg H g Þ þ r  ðrg qg ug H g Þ ¼ rðag rT g Þ þ Qgs þ S gs H s
ot
ð39Þ
o
ðrs qs H s Þ þ r  ðrs qs us H s Þ ¼ rðas rT s Þ þ Qsg þ ssg H s ð40Þ
ot Fig. 1. Schematics of the reactor and simulation grid [40].
where H, a, Q are the specific enthalpy, the mixture thermal
conductivity and the intensity of heat exchange between the Table 3
gas and solid phases, respectively. The third term on the Coal analyses and properties [7]
right hand is the heat transfer in that the solid phase chan- Parameters Values
ged into gas phase. Proximate analysis (wt%)
The specific enthalpy is defined by Moisture 2.6
X n Volatile matter 41.8
H¼ Y iH i ð41Þ Fixed carbon 54.1
i¼1
Ash 1.5

where Hi is the enthalpy for each chemical species in the Ultimate analysis (wt%)
Carbon 75.3
mixture and considers both, thermal and chemical enthalpy Hydrogen 5.4
Z T
Nitrogen 1.8
Hi ¼ C P;i dT þ DH f;i ð42Þ Oxygen 15.6
T0 Sulfur 0.4
where the term T0, Cp,i and DHf,i are the reference temper- Others
ature, the heat capacity at constant pressure for the ith spe- Mean particle size (mm) 0.62
cies, and the enthalpy of formation for the ith species in the Density (kg m3) 1250
standard state. High heating value (kJ kg1) 29, 695
 L. Yu et al. / Fuel 86 (2007) 722–734 729

where hgs is the heat transfer coefficient between the gas Nu  ag  As 6rs  Nu  ag
hgs ¼ ¼ ð45Þ
phase and the solid phase, and expressed in terms of a ds d 2s
no-dimensional Nusselt number
In the case of fluidized beds, Gunn [36] proposed the
following empirical correlation:
Table 4
1
Operating conditions and experimental results [7] Nu ¼ ð7  10rg þ 5r2g Þð1 þ 0:7Re0:2 Pr3 Þ
Exp. no. 1 2 3 4 5 6 1

1
þ ð1:33  2:4rg þ 1:2r2g ÞðRe0:7 Pr3 Þ ð46Þ
Coal feed (kg h ) 8.0 8.0 8.0 8.0 8.0 6.6
Air supply (kg h1) 21.9 17.0 19.4 21.9 28.4 14.8 where the continuous phase Prandtl number is defined by
Steam supply 4.6 4.6 4.6 4.6 4.6 4.0
(kg h1) lg C P;g
Air and steam 420 413 422 435 368 336 Pr ¼ ð47Þ
ag
temperature at
entrance (C)
Temperature of 855 812 841 866 826 829
reactor (C) 3. Numerical considerations
Exp. result
H2 (%) 8.53 8.84 9.63 7.88 6.48 10.80 The simulated case is a bubble fluidized bed coal gasifier
CO2 (%) 19.31 18.38 14.40 15.60 14.86 21.59 which was designed and built for studying the gasification
N2 (%) 60.37 61.10 64.62 64.52 71.54 56.60 of Colombia coal [40]. A schematic view of the BFGB is
CH4 (%) 0.84 1.07 1.34 1.01 1.29 0.86 shown in Fig. 1. The calculation domain is divided into
CO (%) 10.94 10.59 9.97 10.94 5.80 10.14
standard uniform grids (22 · 100 control volumes) accord-

Fig. 2. Comparisons between predictions and experimental data in different cases.

730 L. Yu et al. / Fuel 86 (2007) 722–734

ing to the literature [19]. The air and steam flow into the
bottom of the gasifier at uniform velocity so there is unes-
sential to propose an air distributor model for the sake of
fully gas and solid mixing. Only gas phase is allowed to
outflow the reactor due to the assumption of particles in
uniform size and ash in gas phase. The outlet pressure is
fixed to atmosphere. The bed is initially filled particles with
a 1.0 m high, where the total volume fraction of solids is
patched as 0.48 [7]. To prevent the spacing between parti-
cles from decreasing to zero, the maximum particle packing
is rs,max = 0.64 [19]. At the walls, a zero gradient condition
is used for the turbulent kinetic energy. The no-slip wall
condition is used for the gas phase and solid phase [30].
The value of all the compositions into the gasifier can be
obtained from Tables 3 and 4. The simulation was carried
out with the finite volume method (FVM), in which the
inter-phase slip algorithm (IPSA) of Spalding was used to
solve velocity–pressure coupled differential equations. For
the evaluation of the convective terms, the second order
QUICK scheme was used. The time steps was set as
1 · 104. The governing equations were discretized into
algebraic equations that can be solved numerically.
Gauss–Seidel method was applied to solve these equations
which can be stable due to point by point iteration. In
order to reduce the number of iteration and to accelerate
the convergence of solution, algebraic multigrid (AMG)
scheme was also used to coarsen grids [41].
4. Results and discussion
The six different cases were calculated and their results
were validated by the experimental data with Colombia

Fig. 3. Concentration distributions of H2, CO2, N2, CH4 and CO in different cases.
 L. Yu et al. / Fuel 86 (2007) 722–734 731

coal. The simulation results of outlet molar fraction of gas
composition can be compared with experimental data by
the following form of area average:
Z taneously, the quantity of CO2 can be compensated by
1
Xi ¼ X i dA ð48Þ
A be used to explain why the contents of H2 and CH4 drop
Fig. 2 shows that the prediction results are well in agree-
ment with the experimental data. It can be observed that
the calculation errors of CO2 and N2 molar fraction are less
than 5% and most of other results are within the 20%
range. One or two calculation errors of CH4 molar fraction
are more than 10% due to the fact that it only comes from
devolatalisation but the reaction of char and H2 is
neglected. The higher differences of these cases are pre-
sented in the H2 and CO molar fraction due to the fact that
the effect of limestone is ignored. According to the decom-
position reactions of limestone in the work of Souza-
Santos [25], CO2 can be produced. Through the impact
of the equilibrium of water–gas shift reaction (R6), it will
take place for the phenomenon that the contents of H2
decrease and the contents of CO increase. This tendency
can contribute to improve the predicted exit value of H2
concentration and CO concentration. But it is reasonable
to ignore the effect of limestone due to its lower contents
and higher decomposing temperature. The results of H2
step. On the contrary, the contents of H2 and CO2 are high
enough to move the water–gas shift reaction toward the
backward step. Although H2 and CO2 are depleted simul-
combusting the methane. So the (R8) and the (R9) can
down to the top of reactor. However, due to the existence
of water–gas exothermic reaction, on the top of gasifier, the
radial profile of CO concentration is favored by high tem-
perature and the radial profile of H2 concentration is
favored by low temperature. Besides the common rules,
each case has its own characteristics which can be observed
from the contour of molar fraction for each composition in
Fig. 3 due to different operating conditions, for example,
the most evident difference of composition contour can
be shown at the top of gasifier between case 6 and others.
Due to lower flow rate of air supply for case 6, the upwards
parabolic contour of molar fraction for each composition
cannot be formed at the exit and the content of N2 is less
than that of other cases.
0.0020
0.002 m (Bed height)
0.004 m
Molar Concentration of Oxygen

concentration and CO concentration in lower calculation 0.0019 0.006 m

error can verify this assumption.
Simulated distributions for gas compositions of these 0.0018
(kmol/m3 )

cases are shown in Fig. 3. Observed from Fig. 3, the overall

trend of each composition profile is coincident in different 0.0017
cases. For example, the concentrations of CO2 and CO
increase along the height of the gasifier, while the contents 0.0016
of H2 and CH4 go up at first then drop down to the top of
reactor due to the devolatalisation and the equilibrium of 0.0015
water–gas shift reaction. Although the water–gas shift reac- -0.10 -0.05 0.00 0.05 0.10
tion is exothermic and low temperature favors the forward Bed diameter (m)
step [42], the content of CO is so low that it is impossible to Fig. 5. Radial profiles of oxygen concentration at the bottom of gasifier in
move the water–gas shift reaction toward the backward different heights.

1150

1100
Gas Temperature (K)

1050

1000

950
0.002 m
0.004 m
900 0.006 m (Bed height)

-0.10 -0.05 0.00 0.05 0.10

Bed diameter (m)

Fig. 6. Radial profiles of gas temperature at the bottom of gasifier in

Fig. 4. Contours of the simulated gas temperature in different cases. different heights.
732 L. Yu et al. / Fuel 86 (2007) 722–734

4.1. Relationship between temperature and gas

composition profile

The composition distribution is strongly relative with

the temperature profile in reactor. In the gasifier, the pre-
dicted temperature profile shown in Fig. 4 further illus-
trates that the high temperature zone of the top section
contribute to increase the molar fraction of carbon monox-
ide and decrease the molar fraction of Hydrogen. The
higher wall temperature promotes the upward parabolic
change of radial temperature profile. Moreover, Fig. 4
shows that there is a clear division in the upper of reactor.
Above the division, the calculated zone can be considered
as a pure gas phase region while the gas phase and solid
phase existed in the low regime of gasifier. The heat
exchange of gas–solid mixture is different from that of
the pure gas phase. It leads to the evidently different tem-
perature distribution between the up regime of pure gas
phase and the low regime of gas–solid mixture.
At the feed point, the temperature dropped down rap-
idly at first due to the devolatalisation and drying then Fig. 7. Velocity vector distributions: (A) gas; (B) solid.
went up gradually. The methane is released from the vola-
tile at the feed region and reduced along the height of gas-
ifier due to oxidization reaction. At the gas inlet, the Fig. 7 gives gas and solid velocity vector distribution to
oxygen is supplied into the gasifier and was depleted along further illustrate the effect of flow behavior on the heat
the gasifier height due to the gasification reaction. The heat transfer. The coal bed was agitated by the gas up-flow
of combustion is released and the temperature of the reac- and vortex field is formed due to the unbalanced forces
tor bottom was elevated rapidly. of drag and gravity. It is the internal circulation of coal
From Figs. 5 and 6, the relationship between oxygen bed that promotes the bed temperature uniform. However,
concentration and gas temperature can be revealed clearly. in the freeboard of the gasifier, there exists a strong up-flow
The similar radial profile of oxygen concentration and gas which will keep from the occurrence of backmixing. Then
temperature but reversed trend further illustrate that the the radial profile of freeboard temperature is formed due
heat of combustion is the key reason of elevating the tem- to thermal diffusion. So the gasifier can be divided into high
perature of gasifier. When the oxygen is depleted, the tem- temperature zone and low temperature zone by the clear
perature of gasifier will decrease due to the fact that the division that is different from the circulating fluidized bed
overall gasification is an endothermal reaction. [43].

Fig. 8. Relationship between coal volume fraction and reaction rates.

 L. Yu et al. / Fuel 86 (2007) 722–734
4.2. Relationship between coal volume fraction and gas
composition profile
Fig. 8 shows the calculated distributions of coal volume
fraction and heterogeneous reaction rates. It is noted that
the contents of CO, CO2 and H2 increase subsequently at
the bottom of gasifier due to coal combustion, char-CO2
and Char-H2O gasifications in all cases, while significant
difference of these heterogeneous reaction rates are shown
in Fig. 8. The predicted result is consistent with that of a
review on char oxidization mechanisms [44]. According
to this review, the first product which was observed near
the gas inlet is CO whether two-step or three-step reaction
mechanism were proposed. Fig. 3 gives the distributions of
CO, CO2 and H2 concentration that are released along the
bed height subsequently in the low regime of gasifier. Due
to the fact that there is few coal particles in the bubble
phase, the heterogeneous reaction rates is lower than that
of emulsion phase which can be verified by contrasting
the heterogeneous reaction rates with coal volume fraction
in Fig. 8.
5. Conclusion
A comprehensive model based on TFM including
KTGF and complicated reactions was developed to simu-
late BFBG numerically which can be used to predict and
analyze the impact of flow behavior on chemical reaction.
The simulation results would give much more exact predic-
tions of the distributions of pressure, temperature, velocity,
volume fraction of the phases and gas composition along
the reactor which cannot be described by two-phase or
three-phase model. The calculated exit gas compositions
are in well agreement with the experiment data which is
available from Colombia coal. From these results, a rea-
sonable interpretation of the change trend of gas composi-
tion profile along the gasifier with the distributions of
temperature, gas and coal velocity and coal volume frac-
tion can be obtained.
References
[1] Yan HM, Heidenreich C, Zhang DK. Mathematical modeling of a
bubbling fluidized-bed coal gasifier and the significance of ‘net flow’.
Fuel 1998;77:1067–79.
[2] Toomey RD, Johnstone HF. Gaseous fluidization of solid particles.
Chem Eng Prog 1952;48:220.
[3] Yan HM, Heidenreich C, Zhang DK. Modelling of bubbling fluidised
bed coal gasifiers. Fuel 1999;78:1027–47.
[4] Ross DP, Yan HM, Zhong ZP, Zhang DK. A non-isothermal model
of a bubbling fluidised-bed coal gasifier. Fuel 2005;84:1469–81.
[5] Hamel S, Krumm W. Mathematical modeling and simulation of
bubbling fluidized bed gasifiers. Powder Technol 2001;120:105–12.
[6] Sadaka SS, Ghaly AE, Sabbah MA. Two phase biomass air–steam
gasification model for fluidized bed reactors: Part I—model develop-
ment. Biomass Bioenergy 2002;22:439–62.
[7] Chejne F, Hernandez JP. Modeling and simulation of coal gasifica-
tion process in fluidized bed. Fuel 2002;81:1687–702.
733
[8] Gera D, Gautam M, Tsuji Y, Kawaguchi T, Tanaka T. Computer
simulation of bubbles in large-particle fluidized beds. Powder Technol
1998;98:38–47.
[9] Tsuji Y, Kawaguchi T, Tanaka T. Discrete particle simulation of two-
dimensional fluidized bed. Powder Technol 1993;77:79–87.
[10] Rong DG, Mikami T, Horio M. Particle and bubble movements
around tubes immersed in fluidized beds – a numerical study. Chem
Eng Sci 1999;54:5737–54.
[11] Hoomans BPB, Kuipers JAM, Briels WJ, Swaaij WPM. Discrete
particle simulation of bubble and slug formation in a two-dimen-
sional gas-fluidised bed: a hard-sphere approach. Chem Eng Sci 1996;
51:99.
[12] Hoomans BPB, Kuipers JAM, van Swaaij WPM. Granular dynamics
simulation of segregation phenomena in bubbling gas-fluidized beds.
Powder Technol 2000;109:41–8.
[13] Chiesa M, Mathiesen V, Melheim JA, Halvorsen B. Numerical
simulation of particulate flow by the Eulerian–Lagrangian and the
Eulerian–Eulerian approach with application to a fluidized bed.
Comput Chem Eng 2005;29:291–304.
[14] Gidaspow D, Jung J, Singh RK. Hydrodynamics of fluidization using
kinetic theory: an emerging paradigm 2002 Flour-Daniel lecture.
Powder Technol 2004;148:123–41.
[15] Chapman S, Cowling TG. The mathematical theory of non-uniform
gases. Cambridge University Press; 1970.
[16] Arastoopour H. Numerical simulation and experimental analysis of
gas–solid flow systems: 1999 Fluor-Daniel Plenary lecture. Powder
Technol 2001;119:59–67.
[17] Bi HT, Ellis N, Abba IA, Grace JR. A state-of-the-art review of gas–
solid turbulent fluidization. Chem Eng Sci 2000;55:4789–825.
[18] Gidaspow D. Multiphase flow and fluidization: continuum and
kinetic theory description. Academic Press; 1994.
[19] Enwald H, Almstedt AE. Fluid dynamics of a pressurized fluidized
bed: comparison between numerical solutions from two-fluid models
and experimental results. Chem Eng Sci 1999;54:329–42.
[20] Yang TY, Wang AR, Zhang SJ, Zhang XP. Numerical simulation for
fluid dynamics in a gas–solid bubbling fluidized bed. Comput Appl
Chem 2005;22:206–10.
[21] Patil DJ, Annaland MS, Kuipers JAM. Critical comparison of
hydrodynamic models for gas–solid fluidized beds – Part I: bubbling
gas–solid fluidized beds operated with a jet. Chem Eng Sci 2005;60:
57–72.
[22] Patil DJ, Annaland MS, Kuipers JAM. Critical comparison of
hydrodynamic models for gas–solid fluidized beds – Part II:
freely bubbling gas–solid fluidized beds. Chem Eng Sci 2005;60:
73–84.
[23] Cho HC. A numerical study on parametric sensitivity of the flow
characteristics on pulverized coal gasification. Int J Energy Res 2000;
24:511–23.
[24] Petersen I, Werther J. Experimental investigation and modeling of
gasification of sewage sludge in the circulating fluidized bed. Chem
Eng Process 2005;44:717–36.
[25] de Souza-Santos ML. Comprehensive modeling and simulation of
fluidized bed boilers and gasifiers. Fuel 1989;68:1507–21.
[26] Zhou LX. Dynamics of multiphase turbulent reacting fluid
flows. Beijing: National Defence Industry Press; 2002.
[27] Mathiesen V, Solberg T, Arastoopour H, Hjertager BH. Experimen-
tal and computational study of multiphase gas/particle flow in a CFB
riser. AIChE J 1999;45(12):2503–18.
[28] van Wachem BGM, Schouten JC, van den Bleek CM. Comparative
analysis of CFD models of dense gas–solid systems. AIChE J 2001;
47(5):1035–51.
[29] Cooper S, Coronella CJ. CFD simulations of particle mixing in a
binary fluidized bed. Powder Technol 2005;151:27–36.
[30] Ding J, Gidaspow D. A bubbling fluidization model using kinetic
theory of granular flow. AIChE J 1990;32(1):523–38.
[31] Lu HL, He YR, Gidaspow D. Hydrodynamic modeling of binary
mixture in a gas bubbling fluidized bed using the kinetic theory of
granular flow. Chem Eng Sci 2003;58:1197–205.
734 L. Yu et al. / Fuel 86 (2007) 722–734
[32] Mckeen T, Pugsley T. Simulation and experimental validation of a
freely bubbling bed of FCC catalyst. Powder Technol 2003;129:
139–52.
[33] Claus Hubbe Ibsen. An experimental and computational study of gas-
particle flow in circulating fluidised reactors. PhD thesis, Group for
Chemical Fluid Flow Processes, Department of Chemistry and
Applied Engineering Science, Aalborg University, Esbjerg Niels
Bohrs Vej 8, DK-6700 Esbjerg, Denmark, 2002.
[34] Pain CC, Mansoorzadeh S, Gomes JLM, de Oliveira CRE. A
numerical investigation of bubbling gas–solid fluidized bed dynamics
in 2-D geometries. Powder Technol 2002;128:56–77.
[35] Enwald H, Peirano E, Almstedt AE, Leckner B. Simulation of the
fluid dynamics of a bubbling fluidized bed experimental validation of
the two-fluid model and evaluation of a parallel multiblock solver.
Chem Eng Sci 1999;54:311–28.
[36] Gunn DJ. Transfer of heat or mass to particles in fixed and fluidized
beds. Int J Heat Mass Transfer 1978;21:467–76.
[37] Eaton AM, Smoot LD, Hill SC, Eatough CN. Components,
formulations, solutions, evaluation, and application of comprehen-
sive combustion models. Progr Energy Combust Sci 1999;25:387–
436.
[38] Smoot LD, Pratt DT. Pulverized-coal combustion and gasification –
theory and applications for continuous flow process. New York: Ple-
num Press; 1979.
[39] Chen CX, Horio M, Kojima T. Numerical simulation of entrained
flow coal gasifiers. Part I: modeling of coal gasification in an
entrained flow gasifier. Chem Eng Sci 2000;55:3861–74.
[40] Ocampo A, Arenas E, Chejne F, Espinel J, London C, Aguirre J,
et al. An experimental study on gasification of Colombian coal in
fluidised bed. Fuel 2003;82:161–4.
[41] Tao WQ. Recent advance of numerical heat transfer. Beijing: Science
Press; 2000.
[42] Hoang DL, Chan SH. Modeling of a catalytic autothermal methane
reformer for fuel cell applications. Appl Catal A: Gen 2004;268:
207–16.
[43] Chen CX, Horio M, Kojima T. Use of numerical modeling in the
design and scale-up entrained flow coal gasifiers. Fuel 2001;80:
1513–23.
[44] Wall TF, Liu GS, Wu HW, Roberts DG, Benfell KE, Gupta S, et al.
The effects of pressure on coal reactions during pulverised coal
combustion and gasification. Progr Energy Combust Sci 2002;28:
405–33.