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Operating Concept of Circulating Fluidized Bed Gasifier From The Kinetic Point of View
Operating Concept of Circulating Fluidized Bed Gasifier From The Kinetic Point of View
Operating Concept of Circulating Fluidized Bed Gasifier From The Kinetic Point of View
www.elsevier.com/locate/powtec
Research and Development Department, Cotech Engineering Corporation, Fl.1, No. 13, Wu Chuan 1st Road, Wuku Industrial Park,
Hsin Chung, Taipei Hsien, Taiwan, ROC
b
Department and Graduate Institute of Bio-Industrial Mechatronics Engineering, National Taiwan University, Taipei, Taiwan, ROC
c
College of Science and Engineering, National United University, Miaoli, Taiwan, ROC
Received in revised form 10 October 2001; accepted 19 February 2003
Abstract
Circulating fluidized bed gasifiers used in integrated gasification and combined cycle (IGCC) possess unique design and operational
features: high gas velocity, high solid loading, and a large amount of circulating chars. As a consequence, their performance is noticeably
different from the conventional fluidized bed gasifier operating at lower gas velocity. At the same time, limited information has been
published to show how to operate the circulating fluidized bed from the kinetic point of view.
In order to study these aspects, kinetic models are developed using kinetic data from previous literature and two concepts of operating the
circulating fluidized bed gasifier from the kinetic point of view are presented in this paper. The results of the kinetic analysis using Johnsons
kinetic data of a constant specific gasification rate of char (0.001 1/s) show that all species approach their equilibrium values after travelling a
distance of 2.5 m, which is set as the height of the gasifier. The resident time of the char in the bed is 0.86 s and the required circulation rate of
char and lime are 11.8 and 4.5 kg/s, respectively. In addition to Johnsons kinetic data, Wens kinetic model is also applied in the kinetic
analysis. It shows a way to operate the gasifier in the fast fluidization regime with a superficial velocity between 3.6 and 4.9 m/s and a solid
loading between 50 and 100 kg/m3, these operating conditions are recommended by industrial experience. It points out the necessity to
predict the performance of the gasifier from the kinetic point of view in order to design the optimal geometry and operating methods that will
allow the gasifier to play a successful role in the clean coal technology system such as IGCC, high-performance power system (HIPPS), etc.
D 2003 Elsevier Science B.V. All rights reserved.
Keywords: Circulating fluidized bed; Gasifier; Kinetic model; Solid loading; Circulating chars
1. Introduction
The world has large coal reserves; in the US, in particular, they constitute 90% of all known fossil energy resources in that country. Although natural gas-fired combined
cycles currently predominate the power generation market,
and interest is increasing in renewable energy sources, coal
will likely maintain its share of the power generation market
simply because it has the largest reserves and no alternative
is foreseen to replace it in the foreseeable future [1].
However, coal usage has been hampered by pollution
caused by its transport, storage, and combustion. Partly for
* Corresponding author. Department and Graduate Institute of BioIndustrial Mechatronics Engineering, National Taiwan University, Taipei,
Taiwan, ROC. Tel./fax: +886-2-23693159.
E-mail address: chwu@ccms.ntu.edu.tw (C.-H. Wu).
0032-5910/03/$ - see front matter D 2003 Elsevier Science B.V. All rights reserved.
doi:10.1016/S0032-5910(03)00060-3
168
Fig. 1. Sketch of a novel gasifier consisting of a circulating fluidized bed and a cyclone combustor.
2. Problem formulation
Table 1
Reaction mechanisms and rate expressions of char steam reaction (source:
Lowry [15])
Source
Reaction
mechanism
Walker
et al.
1
Cf H2 Og K!
Rate expression
K2
Rate
H2 g CO
K1 H2 O
1 K 1 H2 O K 2 H2
K3
K3
3
CO K!
COg
Ergun and
Menster
1
Cf H2 Og K!
K2
Rate
H2 g CO
K1 H2 O Kd CO2
K1
K2
K5
1 H2 O H2 CO
K3
K3
K4
K3
169
CO ! COg
4
CO CO K!
K5
CO2 g Cf
Wen
C + H2O(g) !
CO + H2
CH2 CCORT
1 x where:
CH2 O
K
Kv = volumetric rate constant;
K = equilibrium constant
dx
dt kv
CaOs H2 S ! CaSs H2 O:
170
dN
K3 AC;
dt
According to Abel et al. [16], the rate of Eq. (2) is fast, but
the rate of Eq. (1) is relatively slow. In addition, CaCO3 is
chemically inert to H2S. One potential reason for limestone
not being able to remove H2S effectively is the relatively slow
calcinations, Eq. (1), that occurs under gasification conditions. This problem can be solved in the proposed reactor
configuration. A large amount of CaO is recycled in the
gasifier, making the removal of H2S from the gas stream
relatively rapid. According to Schrodt and Hahnn [17], CaS
formed on the exterior of the sorbent prohibits further
reactions of the sorbent with H2S. Thus, CaS appears to form
a diffusion barrier for H2S penetration and this limits the
calcium utilization efficiency. This effect is taken into
account in modeling the process of desulfurization as follows.
A theoretical model for the reaction of CaO with H2S was
developed and experimentally verified by Pell et al. [18].
This model assumes that there is nothing adsorbed on the
surface of CaO at the beginning of reaction of desulfurization. As reaction (2) proceeds, the rate slows down, and this
suggests that CaS is adsorbed upon the surface thereby
inactivating the surface. The total amount of lime (CaO) in
the calcined limestone could be categorized into two groups,
according to Pell et al. [18]. One group is the available lime
that can react with H2S to form CaS through reaction (2). The
other group is inactivated lime that cannot react with H2S
due to the adsorption of CaS layer on the surface of lime. The
concentrations of the total amount of lime, available lime,
and inactivated lime in the calcined limestone are specified
as N, A, and B, respectively. The rate of reaction (dN/dt)
dA
K1 AC K2 B K3 AC;
dt
Preexponential
constants ( Pi)
Activation energy
(Ei, kcal/gmol K)
K1
K2
K3
Ke
8.3
9.5
13.1
1.2
13.1
28.2
22.9
15.1
dt
1 Ke C
Ei
Ki Pi exp
:
RT
k2
k3
Co ! COg :
H2 Og Cf !
H2g Co
kV
171
10
_
There are four unknowns, N c, X, Y, and Z, in_Eqs. (11)
and (12). Even if the rate of char gasification (N c) can be
obtained from experiments, there are still three unknowns
X, Y, and Zin Eqs. (11) and (12). In order to solve the
problem, another governing equation was applied as follows. The equilibrium constants, K1 and K2, of Eqs. (8) and
(9), respectively, can be written as Eqs. (13) and (14).
Dividing Eq. (14) by Eq. (13) and simplifying it will result
to Eq. (15). It is interesting to note that Eq. (15) represents
the equilibrium condition for the water gas shift Eq. (16).
172
K1
CO2 Cf
k1V
Wc Wc0 Nc Dt
17
0
Y
WCO WCO
18
WH2 WH0 2 Z
19
WH2 O WH0 2 O Z
20
13
H2 Co
k2
k2V H2 O Cf
14
K2
CO2 H2
K1 CO H2 O
15
0
WCO2 WCO
X
2
21
16
0
WCaO WCaO
NH2 S Dt
22
WH2 S WH0 2 S NH2 S Dt:
23
K2
CO H2 O CO2 H2 :
2.4. One-dimensional control volume analysis
A one-dimensional control volume analysis was developed to determine the extent to which the chemical reactions
of char gasification approach equilibrium in the region from
X1 = 0 to X1 = 2.5 m (the gasifier height) as shown in Fig. 1.
The gasification of CWSF is assumed to occur in three
consecutive steps: evaporation, combustion, and slow reaction between char and steam. The processes of water
evaporation, coal pyrolysis, and combustion complete at
X1 = 0. This assumption may not fit reality because the
evolution rate of the volatiles, which depends on various
factors such as particle size, pressure, and heating rate, may
be too slow to assume that coal pyrolysis has been completed
at X1 = 0. A complete pyrolysis model would describe the
composition and physical state of the char particle and the
composition and evolution rate of the volatiles at all stages of
pyrolysis. However, the detailed mechanism of the evolution
and combustion of volatiles is not very well understood and
detailed experimental work is still required. Nevertheless,
this assumption is still a good approximation because in
general the reaction rates of water evaporation, coal pyrolysis, and combustion are much faster than that of the
gasification of the char. Based on this assumption, the initial
composition and superficial velocity of the gas mixture can
be obtained from the thermodynamic analysis.
The variation of the composition and the superficial gas
velocity as X1 increases can be determined using Eqs. (17)
(23). The variation of the number of mole of species (based
on 1 mol of carbon in feed CWSF) as X1 increases can be
calculated from these equations. This information is then
utilized to obtain the composition of the gas mixture (mole
fraction) and the superficial gas velocity. The variation in
the gas composition and the increase in the superficial gas
0
WCO
X WH0 2 Z
K2
2
0
K1 WCO
Y WH0 2 O Z
24
Z X Nc Dt
25
Y X Nc Dt:
26
Substituting Eqs. (25) and (26) into Eq. (24), results to Eq.
(27), which contains only X.
aX 2 bX c 0
27
where
a=1K
_
0
0
b = KW H
KW CO
+ W 0CO2_+ W0H2 N cDt _
_
_
2O
0
0
0
0
0
0
N cDt + K(N cDt)2+ W CO
W CO
N CDt.
c = KW H2OWH2O +KW H2O N cDt KWCO
2
2
b
p
b2 4ac
:
2a
29
_
The rate of desulfurization N H2S is obtained from the
kinetic model of Pell et al. [18], as indicated by Eq. (30).
The rate constants K3 and equilibrium constant Ke are
obtained from experiments [19] of the reaction between
CaO and H2S from 700 to 1200 K
K3 WCaO CH2 S :
N
H2 S
1 Ke CH2 S
173
30
dUr
1
Mp Uh2 FD :
r
dt
31
174
q
Ur Vr 2 :
2
32
24
:
Rep
33
Substituting Eqs. (32) and (33) into Eq. (31) results to Eq.
(34), which is the equation of motion in the radial
direction in Stokes flow.
Mp
dUr
1
Mp Uh2 3pldp Ur Vr :
r
dt
34
qp
d2 V 2 :
9l De p h2
35
Q
:
pDe H
36
Substituting Eq. (36) into Eq. (35) results to Eq. (37), which
is the expression for the cut-off diameter
dpc
1
Vh2
9Ql
pqp H
!1=2
:
37
175
and H into Eq. (37), the relation between dpc and Vh2 is
written as Eq. (38).
1
4
dpc 1:816 10
:
38
Vh2
Vh rh constant:
39
For the forced vortex, h equals 1 and for the free vortex h
is found between 0.45 and 0.8 [25]. Based on condition (5),
176
Fig. 6. Mole ratio of gas species as a function of axial distance along the
gasifier.
Fig. 5. Sketch of the Rankine vortex [25].
DWi
0:5
0:5
r
9
Vh
6:13
9:19 m=s:
r2
4
1
DWgi 3:194 104 dp2i1 : 41
0:9
0:9
pqp
W0
n
X
! 13
DWi
i1
n
X
p
qp dp30 3:194 104
dp2i1
6
i1
! 13
42
40
Fig. 7. Mole ratio of gas species as a function of axial distance along the
gasifier.
177
gasifier, the_ number of char particles fed into the gasifier per
unit time N is obtained by dividing the feeding rate of char
by the mass of a single char particle
Wf Fc
:
43
Np
dp30 qp
6
The circulation rate of char after n circulations can be
written as Eq. (44)
Wn N W0 W0 DW1 W0 DW1 DW2
W0 DW1 DW2 DW3 K W0 DW1
DW2 DW3 K DWn
!
n
X
N n 1W0
n i 1DWi
i1
wf Fc
p
n 1W0 3:194
dp30 qp
6
!
n
X
4
2
10
n i 1dpi1 :
44
i1
Eqs. (42) and (44) are the transient mass equations of char
particles circulating in the fluidized bed and cyclone combustor. The system will reach steady state when the initial
diameter of char shrinks to become the cut-off diameter of
the cyclone combustor after n circulations
As the system reaches steady state the particle size distribution and the circulating rate of char will not vary with
time. A trial-and-error method is used to solve Eqs. (42) and
Fig. 8. Mole ratio of gas species as a function of axial distance along the
gasifier.
Fig. 10. Gas velocity as a function of axial distance along the gasifier.
dpn dpc
45
46
178
Fig. 11. Solid loading density as a function of axial distance along the
gasifier.
Fig. 12. Operating concept of the gasifier with equilibrium feed rates at 1150 K using Johnsons [10] kinetic data.
47
179
Cs H2 O
! CO H2
48
Fig. 13. Operating concept of the gasifier with equilibrium feeding rates using Wens [9] kinetic model.
180
Fig. 15. The composition of gas as a function of axial distance along the
gasifier using Wens [9] kinetic model.
Fig. 14. The consumption of steam as a function of axial distance along the
gasifier using Wens [9] kinetic model.
Fig. 16. Gas velocity as a function of axial distance along the gasifier using
Wens [9] kinetic model.
181
Fig. 19. Circulating rate of char as a function of axial distance along the
gasifier.
Fig. 17. Solid loading density as a function of axial distance along the
gasifier using Wens [9] kinetic model.
decrease in the gasification rate of the char as the concentrations of CO and H2 increase in Wens kinetic model.
3.3. Circulation rate and shrinkage of chars
The transient Eqs. 42 and 44 developed in Section 2.5
are solved by varying the initial diameter and the number
of circulation of the chars until the char particle shrinks to
be the cut-off diameter and the circulation rate of chars
equals the required circulation rate of chars. Figs. 18 and
19 show the results obtained by using Johnsons kinetic
data at 1150 K. The circulation rate of char is accumulated
to such amount that the chemical reaction of char gasification reach equilibrium at X1 = 2.5 m. The diameter of
the char is plotted as a function of the number of circulations in Fig. 18, and the circulation rate of the char is
plotted as a function of the number of circulations in Fig.
19. Figs. 18 and 19 show that the circulation rate of char
will reach a steady value of 11.8 kg/s after 2860 circulations from the startup if the initial diameter of the char is
80.5 Am. The char particle is expected to shrink from 80.5
Am to the cut-off diameter of the cyclone combustor, 19.7
Am, and be carried out of the cyclone combustor after 2860
circulations.
Fig. 18. Shrinkage of char as a function of axial distance along the gasifier.
(1) The char steam reaction in the gasifier does not reach
equilibrium at low char circulation of 11.8 kg/s and low
temperature of 1150 K. It needs to operate at higher char
circulation rate (15 kg/s) and higher temperature (1450
K) for the char steam reaction to reach equilibrium. It is
suggested to predict the performance of the gasifier from
the kinetic point of view in order to design the optimal
geometry and operating methods that will allow the
gasifier to play a successful role in the clean coal
technology system such as IGCC, HIPPS, etc.
182
K2
K3
Ke
K1
K2
K
kC H2O
Ks
Kv
n
N_
N
_
N_c
N H 2S
Mp
P
_i
Q
r
R
Rep
T
t
Dt
Ur
Uh
Ug
Vr
Vr2
Vh
Vh2
W
_
W
_c
Wf
W0
W0
DWgi
DWi
X
X1
DX1
_
X_
Xeq
Y
Z
q
qp
m
l
c
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