ELSEVIER

PII: $0016-2361(97)00112-9

Fuel Vol. 76, No. 11, pp. 1067-1073, 1997 1997 Elsevier Science Ltd. All rights reserved Printed in Great Britain 0016-2361/97 $17.00+0.00

Coal gasification characteristics in an internally circulating fluidized bed with draught tube
Yong Jeon Kim, Jong Min Lee and Sang Done Kim
Department of Chemical Engineering and Energy & Environment Research Center, Korea Advanced Institute of Science and Technology, Taejon 305-701, Korea (Received 18 April 1996; revised 17 March 1997)
Australian coal was gasified at atmospheric pressure in an internally circulating fiuidized bed (0.3 m i.d. x 2.7 m high) with a draught tube (0.1 m i.d. X 0.9 m high) and a gas separator over the draught tube. The effects of reaction temperature (780-900C), oxygen/coal mass ratio (0.30-0.53), coal feed rate (5.3-12.1 kg h -z) and steam/coal mass ratio (0.30-0.81) on composition of product gas, carbon conversion, cold gas efficiency and gas yield and calorific value were determined. Low-CV gas in the draught tube region and medium-CV gas in the annulus region can be obtained. In the annulus region, the composition of the product gas (vol.%) is H2 31.8-46.2, CO 18.8-25.6, CO2 13.2-20.4 and C H 4 5.3-10.4, with a CV of 8.6-13.2 MJ m -3. In the draught tube region, the composition is H2 8.3-19.7, CO 6.7-13.1, CO2 18.9-35.3 and C H 4 1.9-4.4, with a CV of 3.3-5.9 MJ m -3.

1997 Elsevier Science Ltd.

(Keywords: coal gasification; draught-tube; internally circulating fluidized bed; product gas q u a l i t y )

Gasification in a fluidized bed can be used to convert coal 1-6, biomass 7 and waste materials 7'8 to fuel or synthesis gas. The intrinsic problems of coal conversion in fluidized beds are known to be high carbon losses due to coal shattering and subsequent elutriation of fines, and low conversion of reactant gases due to gas bypassing4'6'9"1. To solve these problems, a draught tube has been inserted in a fluidized bed to divide it into two reaction zones 9-13. Two reaction zones can be achieved: combustion in the draught tube with air, and gasification with steam in the annulus zone 9-12, or vice versa 13. By fluidizing solids in a draught tube at a velocity of seven to ten times the minimum fluidizing velocity (Umf) and in the annulus at 0.7-1.5 Umf, it is possible to induce gross circulation of the bed material up the draught tube and down the annulus. Circulation of the solid material within the reactor provides energy transfer from the combustion zone to the gasification zone. By installing a gas separator over the draught tube, gas of high calorific value can be produced in the annulus (gasification)
zone.

tube to annulus was reduced from 6-11% to - 1 % , while bypassing from annulus to draught tube was increased from 7.7-17.3% to 29.4-38.9% by changing the type of draught tube. Due to the high rate of bypassing from the annulus to the draught tube, the draught tube region acts as a conventional fluidized bed gasifier rather than a combustor. The objective of this study was to develop a new type of coal gasifier, namely an internally circulating ttuidized bed gasifier with an orifice-type draught tube and a gas separator over the draught tube to improve product gas quality. The gasifier was operated at atmospheric pressure to determine the effects of reaction temperature (780-900C), oxygen/ coal mass ratio (0.30-0.53), coal feed rate (5.312.1 kg h -1) and steam/coal mass ratio (0.30-0.81) on the product gas composition, carbon conversion, cold gas efficiency and gas yield and calorific value. EXPERIMENTAL Experiments were carried out in a stainless steel column (0.3 m i.d. x 2.7 m high) with a centrally located draught tube (0.1 m i.d. X 0.9 m high) as shown in Figure 2. The air chamber comprised two plenums to supply gases separately into the draught tube and the annulus zone. For draught tube air supply, a distributor (0.1 m i.d.) with seven bubble caps (four holes x 2.5 mm i.d.) was used. A 60 conical base having 18 bubble caps (four holes X 2.5 mm i.d.) was used for steam supply to the annulus region. To determine the effect of oxygen/coal ratio, oxygen was added to the air stream. Steam was introduced into the plenum chamber and its flow rate was measured by an orifice meter. To preheat air and steam, an electric

To increase the calorific value of the product gas in the annulus zone, gas bypassing from the draught tube to the annulus region should be minimized, since this would cause dilution and burning of the product gas from gasification and consequent degradation of its quality. To reduce this bypassing, a draught tube having orifices in the bottom part has been devised r4. By changing the type of draught tube, different flow characteristics can be observed. The draught tube with orifices (Figure lb) provides less bypassing from the draught tube to the annulus region than that of gap height type (Figure la) with about the same solids circulation rate 14 . In cold bed experiments 14, bypassing from draught

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An internally circulating fluidized bed with draught tube: Yo J. Kim et al.

measure pressure drop in the annulus, seven pressure taps were mounted flush with the wall of the column at 0.2 m height intervals from the distributor. Two pressure taps were also mounted at the bottom and the top of draught tube to measure pressure drop across the tube. To measure axial temperature in the annulus, six K-type thermocouples were mounted along the bed height from the distributor. An electric heater (16 kW) was installed at the main reactor wall to heat the reactor to the ignition temperature of coal (-500C). The reactor was insulated with Kaowool to prevent heat loss through the wall. A sight-glass was mounted 1.0 m above the distributor. An ash drain port was located at the bottom of the reactor and an overflow drain port was mounted 1.1 m above the distributor. The freeboard (0.45 m i.d.) section was expanded to reduce particle entrainment from the reactor. The coal was fed from the top of the reactor through a screw feeder connected to a coal hopper and the feed rate (5.3-12.1 kg h -1) was regulated by a DC motor controller. Since coal gasification takes place in the annulus region (moving bed), the coal should be fed from the top of the reactor to provide a longer reaction time in the moving bed. Two cyclones (0.08 m i.d. 0.32 m high) were installed at the outlet of the gasifier. Product gas was cooled through a condenser and fines were collected by a bag filter. Gas sampling probes were installed at the outlet of the condenser. At the beginning of an experiment, only air was fed into the reactor until the bed temperature reached 450-500C. Thereafter, the electric heater was turned off and coal was fed into the gasifier. When the desired reaction temperature was reached, steam was introduced into the gasifier. When the gasifier operation reached a steady state, the gas composition and the amount of particles collected in the cyclone were measured. The sampled gas was analysed by gas chromatography with a thermal conductivity detector and columns of molecular sieve 5A and Porapak Q. To calculate the amount of product gas and gas composition in the annulus region, helium gas as a tracer was injected between the annulus gas outlet and the cyclone. A local mass balance of nitrogen gas was made to determine the amount of product gases from the draught tube by injecting nitrogen as a tracer into the draught tube. The particle size of the bed material (sand) was 390 #m and the static bed height was 0.8 m from the distributor plate. The gasifier reached steady state in a reaction time of 1 h after steam was injected into the gasifier. The particle size of the coal was 1-5 mm; its properties are given in Table 1. RESULTS AND DISCUSSION

~, &

&.

e&

& &l

ia i a

',,
a)

I 1'1
b)

)" Solid flow tl~ Gas flow Figure 1 Fluidized bed with a draught tube: (a) gap height type; (b) orifice type

N2--

~12
20

VI/atcr Out
.=~ Ig

19
Waterout

15

Water in

20 crout
Water

I~
19

He

II
02 Air in Figure 2 Schematic diagram of the internally circulating fluidized bed gasifier. 1, flow meter; 2, steam generator; 3, orifice meter; 4, air plenum; 5, distributor; 6, overflow drain; 7, viewport; 8, draught tube; 9, main body; 10, separator; 11, freeboard; 12, screw feeder; 13, coal hopper; 14, cyclone; 15, condenser; 16, collector; 17, dust filter; 18, condenser; 19, gas sampling bottle; 20, ID fan heater (3 kW) was installed on the outer wall of the plenum chamber. Four equally spaced 30 mm diameter holes were drilled in the wall of the draught tube 40 mm above its base. A gas separator was installed to separate the gas streams emanating from the annulus and draught tube zones. To

Effect of reaction temperature

The reaction temperature is expected to be one of the most important operating variables affecting the performance of the gasifier, since the main gasification reactions (C + H20 --'* CO + H 2 and C + CO2 ---* 2CO) are endothermic. Hence the reaction temperature should be at the highest tolerable level, limited by materials of construction, ash fusion and production of undesirable gases such as NOx ~5. In the present study, the constructional material of the gasifier restricted the maximum operating temperature to 900C. The effect of reaction temperature on composition of the product gas in the annulus region is shown in Figure 3. As can be seen, the composition range (vol.%) is H2 36.7-45.1, CO 19.3-25.5, CO2 15.4-13.4 and CH4 10.3-6.6. The yields of

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Table 1 Typical analysis of Australian coal
Proximate analysis (wt% db) Volatile matter Fixed carbon Ash Ultimate analysis (wt% daf) C H O N S Heating value (MJ k g - J) 26.4 63.9 9.7 68.1 4.58 25.4 1.6 0.3 26.27

60 50
U d 10 Umr U a = 1.4 Umf U,. r = 0.08 m/s
=

H20/C 0.75 O2/C = 0.25

=

"d 40
"~ 30
..___-v CO

o 20 ~~----~--~t 10
CH 4

. co2

0 750

800

850 Temperature (C)

900

950

Figure 3 Effect of reaction temperature on composition of product gas in annulus region

the chemical reaction rate control under the present experimental conditions, so that yields of H2 and CO increase significantly with reaction temperature since the reaction rate increases about tenfold. In char combustion, the activation energy changes with reaction temperature due to an increase in diffusional resistance, and the kinetics are controlled by the gas film diffusion rate at temperatures above -700C. Therefore the yield of CO2 increases slightly, since the reaction rate increases about 1.14 times with increasing reaction temperature between 780 and 900C. The concentrations of H2 and CO increase with reaction temperature 5'15']7, whereas those of CO2, CH4 and N2 decrease slightly. These results are comparable with those of Judd 9 for a bed with a gap height type of draught tube at higher reaction temperatures than in the present study. Therefore it can be claimed that the draught tube with orifices is superior to the gap height type for producing medium-CV gas in the annulus region. The effect of reaction temperature on the composition of the product gas in the draught tube region is shown in Figure 4. The composition exhibits the same trend as in the annulus region. The increase in yield of H2 and CO may be due to volatile matter released during pyrolysis and the carbon-steam reaction, since steam bypassed from the annulus to the draught tube section. However, the concentration of combustible gases is reduced due to the dilution of the product gas with nitrogen and carbon dioxide. A detailed material balance cannot be constructed, due to the difficulty in estimating tar yield accurately, whereas a carbon balance can easily be determined as shown in Table 3. The carbon content of the solids was determined by chemical analysis and carbon in the product gas was calculated cumulatively from the volume of the gas and its chemical composition. The unaccounted-for carbon may be due to the loss of carbon in the form of tar, liquids and some

Table 2 Kinetic parameters for the reactions

Reaction Gasification Combustion Temperature range (C) 700-850 500-575 575-700 700-800 aRate-determining step

ko
(s - latm - i) 6.47 103 7.58 104 0.44 0.045

E
(kJ tool - i) 167 113 27.6 9.6

RDS ~ chemical reaction chemical reaction pore diffusion gas film diffusion

k780oc

kg~ooc

(s-I)
3.93 10 -5 --1.47 x 10 -2

(s -I)
3.76 10 .4 --1.68 10 -2

H2 and CO increase with increasing reaction temperature since the gasification reactions are endothermic. In a previous study 16, the rate equations for char combustion and steam gasification were determined on the basis of the shrinking-core model as: dX n = Kp02 or
.20( 1 --

X)2/3 (1)

E X)2/3 = koexp ( - R-~)p02 or H20(1 --

where X, K, P02 or PH20, ko, E, R and T are carbon conversion, reaction rate constant, partial pressure of 02 or H20, pre-exponential factor, activation energy of coal combustion or steam gasification, molar gas constant and reaction temperature, respectively. The values of ko and E obtained are shown in Table 2. The kinetics of steam-char gasification are governed by

entrained particles. It is clearly indicated that the increase in gas yield with reaction temperature is partly achieved at the expense of tar and liquids. During gasification, the average carbon content in the bed was in the range 6-10 wt% at a coal feed rate of 5.3-12.1 kg h -1. Calorific values of the product gas from the present and previous studies versus reaction temperature are shown in Figure 5. The CV of the product gas obtained in the annulus region is 11-12 MJ m -3, which is much higher than that in the annulus region (gasification) of an internally circulating fluidized bed with a gap height type of draught tube 1o. The CV of the ~product gas in the draught tube region is 3.34.7 MJ m -e, which is comparable with that for a conventional fluidized bed 6 or spouted bed gasifier 15'18. As the reaction temperature is increased, the H2 and CO concentrations increase whereas high-CV hydrocarbons decrease slightly due to the increase in decomposition reactions, as

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An internally circulating fluidized bed with draught tube: Y. J. Kim et al.

70 20

60 .~ 50
,.,..i 0

H20/C = 0.75 O2/C = 0.25

16
E

[]

: This study (orifice type ; annulus) : Jeon (gap height type ; annulus, 1995) : This study (orifice type; draft tube) : Lee (fluidized bed,1995) : Foong et al. (spout bed, 1981)

&
= 0

40

12

30
0 o
~
M

8 #

CO2

20 10
0 750

O "d
4

LI

tq

F1

CO

t
800 850

t cH,
900 950

700

750

800

850

900

950

Temperature (C) Figure 4 Effect of reaction temperature on composition of product gas in draught tube region

Temperature (C) Figure 5 Calorific value of product gas versus reaction temperature, and comparison with previous studies

Table 3 Carbon mass balance in an internally circulating fluidized bed gasifier

T (C) 780 800 850 900 C in coal 98.4 93.9 89.7 85.8 C in cyclone" 2.0 2.2 0.9 2.0 Gasification product (g min -I) C in cyclone b 2.8 1.7 4.8 2.8 C in overflow 44.3 41.8 38.7 36.3

(C in product) X 100%/(C in coal)

C in gas
30.5 28.2 30.5 38.6 80.9 78.7 83.5 92.9

aCyclone located in draught tube gas outlet bCyclone located in annulus gas outlet

can be seen in Table 43'19. Therefore the calorific value of the product gas in the annulus region decreases slightly whereas that in the draught tube increases with increasing reaction temperature. The effects of reaction temperature on gas yield, carbon conversion and cold gas efficiency of the product gas are shown in Figure 6. Gas yield, carbon conversion and cold gas efficiency are defined as: Gas yield--- gas production rate coal feed rate C content of product gas C content of feed coal

reactions increase with reaction temperature, and the cold gas efficiency increases due to an increase in gas yield in both regions.

(2)

C conversion =

(3)

Cold gas efficiency = (CVofgas) (total gas production rate) (coal feed rate) (CV of coal) (4)

The gas yield increases from 0.22 to 0.35 m3kg -l coal in the annulus region and from 0.86 to 1.09 m3kg -l coal in the draught tube region. The gas yield may result from pyrolysis, char ~asification and steam reforming of tar and liquids (Table 3) . Carbon conversion in the two regions increases, since the rates of the carbon-steam and carbon-oxygen

Effect of oxygen/coal ratio The effect of oxygen/coal mass ratio supplied to the draught tube on product gas composition in both regions at a given steam/coal ratio is shown in Figures 7 and 8. In the annulus region, the concentrations of H2, CO and CH4 decrease slightly but the CO: content increases with increasing oxygen/coal ratio from 0.30 to 0.53. In this case, the decrease in H2, CO and CH4 concentrations may be caused by an increase in recombustion of H2 and CH4 owing to the increased amount of oxygen bypassing into the annulus region. The increase in CO2 content arises from the loss of H2 and CH4 as well as from combustion of carbon and CO 1'220 ' . Thus, owing to the reduction of combustible gas by recombustion of the product gas, the calorific value of the product gas in the annulus region decreases from 11.9 to 9.9 MJ m-3. In the draught tube region, concentrations of H2 and C H 4 decrease but the CO2 concentration increases with increasing oxygen/coal ratio. The CO concentration tends to decrease due to recombustion and to increase due to incomplete combustion, but the latter effect predominates so that the net CO concentration increases slightly. The calorific value of the product gas in the draught tube region remains in the range 3.3-3.6 MJ m -3.

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Fuel 1997 Volume 76 Number 11

An internally circulating fluidized bed with draught tube: Y. J. Kim et al.

1.8 ? 1.5 1.2 0.9 0.6 0.3 "7" 0.6
I
Annulus ~_~ H20/C = 0.75 O / C = 0.25 Draft __~

I
-

0.6 7" 0.5 0.4

o

0.5 E ._o 0.4 i

I

;>

0.3-

"_.------1---

0.2 o L)

t
I

0.3 0.~ 0.1

-6 "6
[,.)

0.10,0 750

Mixed (draft + annulus)

I I

800

850
Temperature (C)

900

0.0 950

Figure 6

Effect of reaction temperature on gas yield, carbon conversion and cold gas efficiency of product gas

60
T = 850 - 860 C H20/coal = 0.63 U d = I0 U, = 1.4

7O

50

Umf Umf

f
H2
o >

T = 850 - 860 C
oal = 0.63

.= 40 Q

N2

30
L

:5

t CO2

o 20

O
CO2

E o

30

L
20;
ff--___~
H2 CO I _A I _A I I & CH 4 I

N~

10
CH4
0 I I I I I I

10
v------

0 0.60 0.25

_~ I

0.25

0.30

0.35

0.40

0.45

0.50

0.55

0.30

0.35

0.40 0.45 O2/coal (kg kg~)

0.50

0.55

0.60

O2/coal (kg kg~)

Figure 7 Effect of O2/coal m a s s ratio on composition of product gas in annulus region

Figure 8 Effect of O2/coal mass ratio on composition of product gas in draught tube region

Table 4 Region

Hydrocarbon concentrations (vol.%) at different reaction temperatures T (C) 780

800 850 900 780 800 850 900

C :H4 0.503
0.565 0.494 0.588 1.606 1.674 1.123 1.058

C2H6 0.164
0.178 0.120 0.119 0.460 0.436 0.215 0.150

C 3H6 0.153
0.134 0.057 0.069 0.319 0.294 0.07 0.041

C 3H8

C4 compounds 0.02
0.04 n.d." n.d. 0.037 0.077 n.d. n.d.

Draught tube

0.037
0.022 0.012 0.012 0.044 0.032 n.d. n.d.

Annulus

Fuel 1997 Volume 76 Number 11

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An internally circulating fluidized bed with draught tube: Y. J. Kim et al.

1.4
1.2 --~ "-" 1.0
o
"7

60
T = 860 C H20/coal = 0.63

50

T = 870 C H 2 0 / O z = 2.5

U a = 10 Umf U a = 1.4 Umf

.~ 40
o

0.s

Draft tube

~E
-~ 0.6

:~ 30
o

~ 20
10

0.4
Annulus

:
I I I

CO2 Ctt 4 N2

0.2 0.0 0.2~

I I I I I I

0.30

0.35

0.40

0.45

0.50

0.55

0.60

12

15

O2/coal (kg kg"1) Figure 9 Effect of OJcoal mass ratio on yield of product gas in both regions The effect of oxygen/coal ratio on gas yield in both regions is shown in Figure 9. As the oxygen/coal ratio increases, the following two processes occur simultaneously: H2, CO and CH 4 production decreases due to recombustion and CO2 production increases due to combustion. These two opposing reactions compensate each other to maintain an almost constant gas yield. Carbon conversion increases with increasing oxygen/coal ratio, whereas cold gas efficiency decreases slightly due to a decrease in calorific value of the product gas.

Coal feeding rate (kg h"l) Figure 10 Effect of coal feed rate on composition of product gas in annulus region

Effect of steam/coal ratio

The effect of steam/coal mass ratio supplied to the annulus region on the composition of the product gas at a coal feed rate of 7.56 kg h - ' and a O2/C mass ratio of 0.30 is shown in Figure 12. Since the reaction temperature decreases with increasing steam/coal ratio 1, it was maintained by an electric heater. As can be seen, the product gas composition in the annulus region is insensitive to changes in steam/coal ratio z5'17, since equilibrium of the water-gas shift reaction favours H2 production and the residence time of steam in the annulus region decreases with increasing steam/coal ratio. The calorific value of the product gas in the annulus region remains in the range 11.0-11.5 MJ m-3 and the gas yield, carbon conversion and cold gas efficiency of the product gas in the annulus region remain roughly constant.

Effect of coal feed rate

The effect of coal feed rate on composition of the product gas in the annulus region at a constant steam/oxygen ratio is shown in Figure 10. As can be seen, the percentages of H2, CO, and CH4 increase with increasing coal feed rate from 5,3 to 12.1 kg h -1 due to an increase in supply of volatile matter, whereas the CO2 concentration remains almost constant 1'2'15'17'18. Thus the calorific value of the product gas in the annulus region increases from 8.56 to 13.22MJm -3 since combustible gases increase with increasing coal feed rate. The composition of the product gas in the draught tube follows the same trend as that in the annulus region. The range of product gas composition (vol.% db) in the draught tube region is: H2 10.1-19.7, CO 6.7-13.1, CO2 18.9-29.0 and CH4 1.9-4.4%, and the calorific value is 3.3-5.9 MJ m -3. The effect of coal feed rate on gas yield, carbon conversion and cold gas efficiency of the product gas is shown in Figure 11. Although the amount of product gas increases slightly with coal feed rate due to an increase in pyrolysis products, the gas yield decreases. Since the oxygen/coal ratio decreases with increasing coal feed rate, carbon conversion decreases 17. The cold gas efficiency tends to increase with increasing calorific value of the product gas but to decrease due to the decrease in gas yield in the annulus region. These two effects compensate each other and the cold gas efficiency does not exhibit any noticeable variation.

CONCLUSIONS Coal gasification in an internally circulating fluidized bed with an orifice-type draught tube and a gas separator over the draught tube allows low-CV gas in the draught tube region and medium-CV gas in the annulus region to be obtained. In the annulus zone, the composition (vol.% db) of the product gas is in the range 31.8-46.2 Hz, 18.8-25.6 CO, 13.2-20.4 CO2 and 5.3-10.4 CH4, and the calorific value is 8.6-13.2 MJ m -3, which is higher than is obtained from conventional fluidized bed, spouted bed or other types of internally circulating fluidized bed gasifiers. In the draught tube zone, the composition (vol.% db) of the product gas is 8.3-19.7 H2, 6.7-13.1 CO, 18.9-35.3 C O z a n d 1.9-4.4 C H 4 , and the calorific value is 3.3-5.9 MJ m -3, which is comparable with that from conventional fluidized bed or spouted bed gasifiers. ACKNOWLEDGEMENTS The authors acknowledge a grant-in-aid for research from the Ministry of Trade, Commerce and Energy, Korea.

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Fuel 1997 V o l u m e 76 N u m b e r 11

An internally circulating fluidized bed with draught tube: Y. J. Kim et al.

1.4 o 1.2 o, 1.0 ~E 0.8
~

Draft tube

T = 870 C H20/O2 = 2.5

0.6 Annulus
I I I

;, 0.4 (3 0.2 0.0 0.5

~0

0.5

"~ .o %)
r~o

=" 0.4 0.3

o
o %) = o ,,.0

04
o

0.3 s> 0.2 -0.1

0.2 0.1 0.0 3

i i i

12

0.0 15

Coal feeding rate (kg h "l)

F i g u r e 11

Effect of coal feed rate on gas yield, carbon conversion and cold gas efficiency of product gas

60 T = 880 C O2/C = 0.30 Ua= 10 Umf Umf= 0.08 rrl/s

5 6 7

50

40
0

H2

8 9

30
v
0 o

10
CO

11

20
D

0 10
D &--

-~D

A I 0.4

A J 0.6

CO2 o N2 .o. CH4 I 0.8

12 13

0 0.2

1.0

14 15 16 17 18

Steam/coal (kg kgl ) Figure 12 Effect of steam/coal mass ratio on composition of product gas in annulus region

REFERENCES 1 2 3 4 Gutierrez, L. A. and Watkinson, A. P., Fuel, 1982, 61, 133. Watkinson, A. P., Cheng, G. and Prakash, C. B., Canadian Journal of Chemical Engineering, 1983, 61, 468. Neogi, D., Chang, C. C., Walawender, W. P. and Fan, L. T., AIChEJournal, 1986, 32, 17. Saffer, M., Ocampo, A. and Laguerie, C., International Chemical Engineering, 1988, 28, 46.

19

20

Chatterjee, P. K., Datta, A. B. and Kundu, K. M., Canadian Journal of Chemical Engineering, 1995, 73, 204. Lee, W. J., Ph.D. dissertation, Korea Advanced Institute of Science and Technology, 1995. Herguido, J., Corella, J. and Gonzalez-Saiz, J., Industrial & Engineering Chemistry Research, 1992, 31, 1274. Corella, J., Aznar, M. P., Delgado, J. and Aldea, E., Industrial & Engineering Chemistry Research, 1991, 30, 2252. Judd, M. R., in 2nd International Coal & Gas Conversion Conference, Pretoria. 1987, p. 23. Jeon, S. K., Lee, W. J. and Kim, S. D., in Preprints 8th International Conference on Fluidization, Tours. 1995, p. 879. Berggren, J. C., Bjerle, I., Eklund, H., Karlsson, H. and Svensson, O., Chemical Engineering Science, 1980, 35, 446. Riley, R. K. and Judd, M. R., Chemical Engineering Communications, 1987, 62, 151. Judd. M. R. and Rudolph, V., in Proceedings of the 5th International Conference on Fluidization, ed. K. Ostergaard and A. Sorensen. Elsinore, 1986, p. 505. Ahn, H. S., M.S. thesis, Korea Advanced Institute of Science and Technology, 1995. Foong, S. K., Lim, C. J. and Watkinson, A. P., Canadian Journal of Chemical Engineering, 1980, 58, 84. Lee, J. M., Kim, Y. J., Lee, W. J. and Kim, S. D., Theories and Applications of Chemical Engineering, 1996, 2, 829. Kikuchi, K., Suzuki, A., Mochizuki, T., Endo, S., Imai, E. and Tanji, Y., Fuel, 1985, 64, 368. Foong, S. K., Cheng, G. and Watkinson, A. P., Canadian Journal of Chemical Engineering, 1981, 59, 625. Bjerle, I., Eklund, H. and Svensson, O., Industrial & Engineering Chemistry Process Design & Development, 1980, 19, 345. Sue-A-Quan, T. A., Watkinson, A. P., Gaikward, R. P., Lim, C. J. and Ferris, B. R., Fuel Processing Technology, 1991, 27, 67.

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