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mass transfers in a porous packed bed with Soret and Dufour effects
Mingchun Li
M
s
dr
c
dt
6
Separating the variables in Eq. (6) and integrating gives the position
of the calcination front r
c
as a function of time and the surrounding
temperature.
ah
f
M
s
=cr
in
DHq
s
_
t
0
T
b
T
c
dt
1 h
f
r
in
=k
e
1 r
c
=r
in
3
=3 h
f
r
in
=k
e
1r
c
=r
in
2
=2 7
Fig. 1. The packed bed with endothermic reaction and the decomposition scheme for a single spherical specimen.
166 M. Li et al. / International Journal of Heat and Mass Transfer 67 (2013) 164172
Noting that f
s
1 r
3
c
=r
3
in
, where f
s
is the solid fractional conversion
of REV at time t, Eq. (7) may be restated as follows
ah
f
M
s
=cr
in
DHq
s
_
t
0
T
b
T
c
dt
1 h
f
r
in
=k
e
f
s
=3 h
f
r
in
=k
e
1 1 f
s
2=3
=2 8
2.2.2. Mass transfer controlled scheme
On the basis of pseudo-steady state assumption, the rate of dif-
fusion of the gas product C away from the decomposition interface
may be given by [21]
N
C
4pD
se
C
0
C
0
r
in
r
c
=r
in
r
c
9
The diffusion rate of gas product C from particles exterior surface to
environment is given by
N
C
4pr
2
in
h
d
C
0
qc
1
10
Eqs. (9) and (10) may be solved for C
0
C
0
D
se
C
0
r
in
r
c
=r
in
r
c
r
2
in
h
d
qc
1
=r
2
in
h
d
D
se
r
in
r
c
=r
in
r
c
11
Substituting the value of C
0
in Eq. (10) and rearranging, the overall
reaction rate of a single pellet R
A
in mass transfer controlled regime
can be given as follows
R
A
4pr
2
in
h
d
C
0
qc
1
=1 h
d
r
in
=D
se
r
in
=r
c
1 12
Dening the modied Sherwood number Sh = (h
d
r
in
/D
se
). Hence the
overall reaction rate of REV in mass transfer controlled regime
(i = 2) can be given by
R
2
REV
V
REV
31 e=r
in
h
d
C
0
qc
1
=1 h
d
r
in
=D
se
r
in
=r
c
1
13
Similar to the derivation of Eq. (7), the position of the calcination
front r
c
in mass transfer controlled regime as a function of time
and the surrounding concentration are obtained as follows
aM
s
=cq
s
_
t
0
C
0
qc
1
dt r
in
1r
c
=r
in
3
=3h
d
r
2
in
=D
se
f1
r
c
=r
in
2
=21r
c
=r
in
3
=3g 14
2.3. Conservation equations
The model is two-dimensional and transient. The variables and
parameters are therefore functions of the axial position in the
packed bed x, the radial position in the packed bed r and time t.
Throughout what follows, the variables v(r), c
1
(x, r, t), T
b
(x, r, t),
T
s
(x, r, t), r
c
(x, r, t) and f
s
(x, r, t) will be termed principal variables,
and are calculated respectively from the above reaction kinetics
models and the conservation equations given below.
The mass balance for gas product C considering the cross diffu-
sion effects on the scale of REV is given by
eq
@c
1
@t
eq
1
r
@
@r
rD
@c
1
@r
_ _
e
@
@x
qc
1
c
2
D
0
gradT qDgradc
1
eqm
@c
1
@x
R
i
REV
=V
REV
15
The energy conservation equation of the main stream consider-
ing the cross diffusion effects is given by
eq
@1 c
1
C
p;d
c
1
C
p;1
T
b
@t
e
1
r
@
@r
rk
f
@T
b
@r
_ _
e
@
@x
k
f
gradT
b
qc
1
l
c
11
T
b
D
00
gradc
1
emq
@1 c
1
C
p;d
c
1
C
p;1
T
b
@x
S
v
h
f
T
b
T
s
R
i
REV
=V
REV
C
P;1
T
b
T
c
; 16
R
i
REV
=V
REV
31e=r
in
T
b
T
c
h
f
=f1h
f
r
in
=k
e
r
in
=r
c
1DHg; i 1
31e=r
in
h
d
C
0
qc
1
=1h
d
r
in
=D
se
r
in
=r
c
1; i 2
_
17
The effective velocity v may be determined from the supercial
velocity v
b
and the porosity of packed beds v = v
b
/e, and the Ergun
ForchheimerBrinkman equation [22] is used for analyzing the
uid ow in the porous packed bed,
dP
dx
150
lm
b
d
2
1 e
2
e
3
1:75
q
f
m
2
b
d
1 e
e
3
l
e
1
r
d
dr
r
dm
b
dr
_ _
18
The surface temperature of the solid pellets T
s
as a function of
surrounding temperature T
b
and the calcination front r
c
is given
by the following relationship which takes into account the heat
transfer resistances of both the external lm and the solid product
layer [22].
T
s
h
f
r
in
=k
e
T
b
r
c
T
c
=r
in
r
c
=h
f
r
in
=k
e
r
c
=r
in
r
c
19
The function of the calcination front r
c
included in Eqs. (15),
(16), (17), and (19) depend on the reaction kinetics model chosen.
The expression of Eq. (7) is used in the heat transfer controlled
model, while that of Eq. (14) is used in the mass transfer controlled
model.
The following dimensionless variables are introduced for nor-
malizing the governing equations
t tD=L
2
; x x=L; r r=R; T T
b
=T
in
; T
c
T
c
=T
in
; T
s
T
s
=T
in
20
Utilizing Eq. (20), the dimensionless governing balance equation of
Eqs. (15)(17) can be rewritten as:
@c
1
@
t
L
2
R
2
r
@
@r
r
@c
1
@r
_ _
@
2
c
1
@x
2
D
0
T
in
D
@
@x
c
1
c
2
@T
@x
_ _
m
L
D
@c
1
@x
R
i
REV
=V
REV
_ _
21
Fig. 2. Comparison of the calculated results under different chemical reaction
mechanisms with the experimental data in literature [14]. (T
c
= 1073 K; e
p
= 0.09;
q
p
= 2.47 10
3
kg m
3
; v
b
= 1.32 cm s
1
; e = 0.47) calculated results, D
0
= D
00
= 0,
i = 1; calculated results, D
0
= D
00
= 0, i = 2; s calculated results,
D
0
= D
00
= 0.0008 cm
2
s
1
K
1
, i = 1; r calculated results, D
0
= D
00
= 0.0008 cm
2
s
1
-
K
1
, i = 2.
M. Li et al. / International Journal of Heat and Mass Transfer 67 (2013) 164172 167
@1 C
p;1
=C
p;d
1c
1
T
@
t
L
2
R
2
1
qC
p;d
D
1
r
@
@r
rk
f
@T
@r
_ _
k
f
qC
p;d
D
@
2
T
@x
2
D
00
DC
p;d
@
@x
c
1
l
c
11
T
@c
1
@x
Lm
D
@1 C
p;1
=C
p;d
1c
1
T
@x
L
2
DeqC
p;d
S
v
h
f
T T
s
R
i
REV
=V
REV
C
P;1
T T
c
C
p;d
22
Let Pe = vL/D, Th=R
(i)
REV
L
2
/(Deq), Pe is the modied Peclet number
which represents the relative convection velocity and diffusion
velocity, Th is the Thiele modulus that reects the relative endo-
thermic chemical reaction rate and diffusion velocity.
The initial and boundary conditions for the problem are:
c
1
x; r; 0 0; Tx; r; 0 T
c
; r
c
x; r; 0 r
in
; c
1
0; r;
t 0;
T0; r;
t 1; @c
1
x; 0;
t=@r 0; @Tx; 0;
t=@r 0;
@c
1
1; r;
t=@x 0; @T1; r;
t=@x 0; @c
1
x; 1;
t=@r 0;
@Tx; 1;
t=@r
q
w
2.4. Expression of parameters
The specic heats, density and the enthalpy of reaction are
known for a given reaction and constituents. This work takes the
limestone decomposition as an example for computation. The
other parameters are determined as follows.
The heat transfer coefcient h
f
and mass transfer coefcient h
d
through the stagnant gas lm are calculated from the following
equations [23],
h
f
k
f
2:0 1:1C
p;1
l=k
f
1=3
qmd=l
0:6
=d;
h
d
D2:0 0:6lq=D
1=3
qmd=l
1=2
=d 24
The Soret and Dufour coefcients are expressed by [24]
D
0
L
1q
=qc
1
c
2
T
2
; D
00
L
q1
=qc
1
c
2
T
2
25
the Dufour coefcient is equal to the Soret coefcient in value for
the same research system by the Onsagers reciprocity relation
L
1q
= L
q1
, and the value of which is 0.0008 cm
2
s
1
K
1
in this work
corresponding to the conditions of the owing gas in the xed bed
of limestone calcinations at 1373 K.
l
c
11
R
gas
TM
1
=fc
1
M
1
c
1
M
1
M
2
g 26
In the present work, the equilibrium concentration C
0
is calcu-
lated from the equilibrium dissociation pressure of gaseous prod-
uct (carbon dioxide) over the solid pellets as follows [25]
log p
CO
2
8792:3=T 10:4; C
0
p
CO
2
=R
gas
T 27
3. Results and discussion
The ADI (alternate dimension implicit) method [26,27] was
used to solve numerically the two-dimensional mathematical
model established in previous sections. Computations have been
carried out for a half of the cylindrical packed bed (L R). The re-
sults are independent of the time step size Dt = 0.01 s and the
number of grids 50 40. L = 0.18 m, R = 0.045 m, r
in
= 0.004 m.
3.1. Model validation
A comparison is made among the results of the experimental
data in literature [14] and the two groups of numerical solutions
obtained by the established mathematical model under different
chemical reaction mechanisms as shown in Fig. 2. It can be seen
in Fig. 2 that the chemical reaction mechanisms have a great inu-
ence on the simulated solutions. The results calculated by the heat
transfer controlled regime are in good agreement with the experi-
mental data, especially at the initial and middle stages of the
decomposition, the maximum relative error being less than
13.5%. But as the solid fractional conversion exceeds 80%, the max-
imum relative error between the simulation results and experi-
mental data increases to 23.6%. In contrast, the simulation results
under mass transfer control mechanism are much higher than
the experimental results at the initial and middle stages of the
thermal decomposition and the maximum relative error reaches
43.4%, while in good agreement with the experimental results at
the latter stage (f
s
> 80%) with the maximum relative error being
less than 12.1%. This shows that with the continuously thickening
0.0 0.2 0.4 0.6 0.8 1.0
0.00
0.05
0.10
0.15
D'=D''=0
---- D'=0, D''=0.0008 cm
2
.s
-1
.K
-1 f
s
x/L
1- v
b
=18.7 cm.s
-1
2- v
b
=37.9 cm.s
-1
3- v
b
=53.3 cm.s
-1
3
2
1
(b). Solid fractional conversion along axial direction
Fig. 3. Inuences of the supercial velocity on the concentration gradient and the Dufour effect. (i = 1; T
c
= 1170 K; T
in
= 1373 K; e = 0.42; t = 120 s; Nu = 1.9; r 0).
R
i
REV
=V
REV
31 e=r
in
L
2
h
f
T
in
T T
c
=fDeq1 h
f
r
in
=k
e
r
in
=r
c
1DHg; i 1
31 e=r
in
L
2
h
d
qc
1
C
0
=fDeq1 h
d
r
in
=D
se
r
in
=r
c
1g; i 2
_
23
168 M. Li et al. / International Journal of Heat and Mass Transfer 67 (2013) 164172
of the solid product layer, the controlling step of reaction rate is
also continually changing. For the heat transfer controlled model
(i = 1), the solid fractional conversions calculated considering the
cross-diffusion effects are lower than those obtained by neglecting
the cross-diffusion effects and the decrease being less than 10%.
However for the mass transfer controlled model (i = 2), the solid
fractional conversions calculated considering the cross-diffusion
effects are higher than that obtained by neglecting the cross-diffu-
sion effects and the increase being less than 12.6%. Hence, it is nec-
essary to discuss and identify the specic chemical reaction
mechanism for an endothermic or exothermic reaction system
with gas product during the researches of the cross-diffusion
effects.
3.2. Discussion with heat transfer controlled scheme
The temperature of the owing gas in the pores of packed beds
is a key factor affecting the endothermic reaction rate under heat
transfer control mechanism (i = 1). The Dufour coefcient D
00
de-
notes the heat transfer resulting from concentration gradient,
which affects chiey the temperature distribution and chemical
reaction rate as i = 1. Fig. 3 shows the variation of the concentration
of gas product andthe solid fractional conversion with the super-
cial velocity v
b
. As seen from Fig. 3, for heat transfer control mech-
anism, the concentration gradient of the gas product increases
with the supercial velocity and the decrease in the solid fractional
conversion caused by the Dufour effect intense accordingly. The
maximum relative error of the solid fractional conversion increases
from 4.7% to 11.1% as the supercial velocity increases from 18.7 to
53.3 cm s
1
.
Fig. 4 shows the variation of the temperature elds of the ow-
ing gas and the solid matrix, the concentration distribution of the
gas product and the conversion ratio of the solid pellets with the
Nusselt number and the cross-diffusion coefcients. From
Fig. 4(a)(c) we can see that, as the Nusselt number increases,
the temperature eld of the owing gas decreases, while the con-
centration distribution of gas product and the surface temperature
eld of the solid pellets increase. This is expected since a higher
Nusselt number can improve the quantity of heat exchange be-
tween the owing gas and the solid matrix, which results in the de-
crease in the temperature of the owing gas and the increase in the
decomposition rate near the entrance correspondingly. It was also
found that the solid conversion degree increases near the entrance
as the Nusslet number increases. But with the region where the
decomposition reaction takes place deepens down to the exit, an
increase in the Nusslet number results in an opposite effect for
the solid conversion degree (see Fig. 4(d)). Fig. 5 portrays the vari-
ations of the ratio of Th/Pe with spatial coordinate under different
Nusselt number, which means that relative to the ability of heat
Fig. 4. Inuences of the Soret and Dufour effects on the temperature elds for both the owing gas and the solid matrix, the concentration distribution of the product gas and
the solid fractional conversion at different Nusselt number. (i = 1; T
c
= 1170 K; T
in
= 1373 K; e = 0.42; t = 120 s; v
b
= 53.3 cm s
1
; r 0).
Fig. 5. Inuence of the Nusselt number on the ratio of Th/Pe in the packed bed.
(i = 1; T
c
= 1170 K; T
in
= 1373 K; e = 0.42; t = 120 s; v
b
= 53.3 cm s
1
; r 0).
M. Li et al. / International Journal of Heat and Mass Transfer 67 (2013) 164172 169
and mass transfer, the ability of endothermic chemical reaction in-
creases in the upstream of the packed bed, whereas decreases in
the downstream as the Nusselt number increases. The overall reac-
tion rate is determined by the product of the effective heat transfer
coefcient and the temperature difference between the two
phases. Hence, the inuences of the Nusselt number on the endo-
thermic reaction rate are diverse at different spatial coordinate.
The effect of the Nusslet number on the cross-diffusion effects is
also shown in Fig. 4. A higher Nusselt number results in a larger
difference between the two groups of results calculated separately
at D
0
= D
00
= 0 and D
0
= D
00
= 0.0008 cm
2
s
1
K
1
. As the Nusselt num-
ber increases from 0.93 to 4.1, the temperature gradient of the bulk
stream and the concentration gradient of the gas product in the
packed bed both increase, which improve the Soret and Dufour ef-
fects. As a result, the maximum relative error of the concentration
of the gas product increases from 3.2% to 25.1% and that of the so-
lid fractional conversion increases from 2.6% to 14.4%. Because the
positive thermal diffusion coefcient implies the mass transfer
resulting from higher temperature to lower temperature, the
existing temperature gradient (see Fig. 4(a)) in the endothermic
Fig. 6. Inuences of the supercial velocity on the temperature gradient and the Soret effect. (i = 2; T
c
= 1170 K; T
in
= 1373 K; e = 0.42; t = 120 s; Sh = 23.5; r 0).
Fig. 7. Inuences of the Soret and Dufour effects on the temperature elds of owing gas, the concentration distribution of gas product and the solid fractional conversion at
different Sherwood number.(i = 2; T
c
= 1170 K; T
in
= 1373 K; e = 0.42; t = 120 s; v
b
= 11.9 cm s
1
; r 0).
170 M. Li et al. / International Journal of Heat and Mass Transfer 67 (2013) 164172
reaction packed bed improves the transmission speed of the gas
product to downstream which results in the decrease of the con-
centration elds (see Fig. 4(b)). The positive Dufour coefcient D
00
means the heat transfer resulting from higher concentration to
lower concentration. As the Dufour effect is taken into account,
the heat transmission rate is reduced, which leads to the lower
temperatures for both the owing gas in the pore and the solid ma-
trix as well as a lower endothermic reaction rate (see Fig. 4(d)).
3.3. Results with mass transfer controlled scheme
For the mass transfer controlled scheme (i = 2), the concentra-
tion of gas product in the bulk ow is a key factor affecting the
endothermic reaction rate. The Soret coefcient D
0
denotes the
mass transfer resulting from temperature gradient, which chiey
affects the concentration distribution and the reaction rate. Fig. 6
shows the variation of the temperature gradient and the solid frac-
tional conversion with the supercial velocity v
b
. As seen from
Fig. 6, the temperature gradient of the owing gas decreases with
the supercial velocity and the increase in the solid fractional con-
version induced by the Soret effect decreases accordingly. The
maximum relative error of the solid fractional conversion increases
from 2.7% to 13.7% as the supercial velocity decreases from 47.4
to 11.9 cm s
1
.
The inuences of Soret and Dufour effects on the reaction char-
acteristics, the heat and mass transfer in the packed bed at differ-
ent Sherwood number are compared in Fig. 7. As seen from Fig. 7
(a) and (b), the concentration of gas product and the temperature
of the owing gas both decrease due to the additional mass and
heat transfer caused by cross-diffusion effects. Hence, the solid
conversion fraction calculated considering the cross-diffusion ef-
fects are higher than that obtained by neglecting the cross-diffu-
sion effects as i = 2 (see Fig. 7 (c)). From the comparison of the
solid curves (D
0
= D
00
= 0) and the dashed lines (D
0
= D
00
=
0.0008 cm
2
s
1
K
1
) at different Sherwood number in Fig. 7, the
authors nd that the higher Sherwood number is, the larger effects
of the Soret and Dufour coefcients are. Under the mass transfer
controlled mechanism, a high Sherwood number results in a high
decomposition rate meaning the increases in both the thermal gra-
dient of owing gas and the concentration gradient of gas product.
As a result, the Soret and Dufour effects are intensied. The maxi-
mum relative error of the concentration of gas product increases
from 7.2% to 17.7% and that of the solid fractional conversion in-
creases from 6.5% to 15.8%, as the Sherwood number increases
from 11.8 to 47.1.
4. Conclusion
Through the chemical reaction kinetics, the thermodynamics of
irreversible processes and the assumption of local thermal non-
equilibrium, a two dimensional mathematical model describing
the coupling among the heat transfer, the mass transfer and the
endothermic reaction in a non-thermal equilibrium packed bed
was established and solved. The inuences of the Soret and Dufour
effects under different chemical reaction mechanisms were
discussed.
The inuence of the cross-diffusion effects on the reactive char-
acteristics of packed beds is diverse at different chemical reaction
mechanisms. The solid fractional conversion calculated consider-
ing the cross-diffusion effects are higher than that obtained by
neglecting the cross-diffusion effects under mass transfer con-
trolled mechanism. While the cross-diffusion effects results in an
opposite effect for the solid fractional conversion under heat trans-
fer controlled mechanism. The weakened heat transfer and the
intensied mass transfer caused by the Soret and Dufour effects
lead to a decrease in the temperature of the owing gas and a
reduction in the concentration of gas product. The differences be-
tween the results including the temperature elds, the concentra-
tion of gas product and the solid fractional conversion calculated
separately at D
0
= D
00
= 0, D
0
= D
00
= 0.0008 cm
2
s
1
K
1
, are all inten-
sied by the increase either in the Nusselt number or in the Sher-
wood number. Whatever the chemical reaction mechanism, the
ignored Soret and Dufour effects willcause much error for the
endothermic reaction packed bed with high reaction rate.
Acknowledgments
This work was nancially supported by the National Natural
Science Foundation of China (51004071), the Special Project for
High-end CNC machine tools and basic manufacturing equipment
of China (2012ZX04007-021) and Liaoning Province College Excel-
lent Young Talents Fund Project (LJQ2013012).
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