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Mass Transfer
Thomas C. Ho
Lamar University, Beaumont, Texas, U.S.A.
INTRODUCTION
Gassolid fluidized bed reactors are widely used by
industry. Examples include fluid catalytic cracking
(FCC), combustion and gasification, uranium proces-sing,
roasting of sulfide ore, reduction of iron ores, and drying
(Zenz, 1978). Of all the phenomena aecting the
performance of bubbling fluidized beds as chemical
reactors, interphase mass transfer is probably of pri-mary
importance in most cases (Chavarie and Grace, 1996a,b).
The particlegas mass transfer in a gassolid flui-dized
bed has been an essential subject of investigation since
the invention of the fluidized bed technology.
Historically, there have been two approaches in modeling the rate of mass transfer in fluidized bed reactors.
One approach, called the homogeneous bed approach,
considers the fluidized bed reactor to behave like a fixed
bed and correlates the fluidized bed mass transfer
coecient in a manner similar to that in a fixed bed
based on a plug-flow model. The other approach, called
the bubbling bed approach, considers the flui-dized bed to
consist of two phases, a bubble and an emulsion, and the
gas interchange between the two phases constitutes the
rate of mass transfer. The objec-tive of this chapter is to
review the two approaches.
It is essential to point out that the mechanism of mass
transfer, as will be discussed in this chapter, represents
only one of the potential rate controlling steps governing
reactor performance in the system.
dt
g;single ex;single
CAi CA
2 0:6Resph
Sc
D
2
In the above equation, Resph is the particle Reynolds
number defined as
r ud
g
Resph
sph
Sc rgD
Sh
single
dy
g;single p
0:5
2 0:6Rep Sc
rgudp
Rep m
0:333
5
6
dt
Ak
CAi CA
7
However, in this equation, dN A=dt represents the combined mass transfer rate from all the particles in the
segment, kg;bed is the average mass transfer coecient
of the particles, and Sex;particles is the total exterior
surfaces of all individual particles in the bed segment.
It is worth pointing out that the average mass trans-fer
coecient for fixed bed particles may be higher or lower
than that for single spheres at an identical super-ficial gas
velocity. On one hand, the low fixed bed voidage may
enhance the mass transfer coecient owing to the
creation of increased true gas velocities at the gas
particle interphase for fixed bed particles. On the other
hand, the actual particle surfaces involved in the particle
gas mass transfer are smaller for fixed bed particles than
those for well dispersed particles owing to particle
blockage in the fixed bed arrangement. The use of total
exterior surfaces of all individual particles in Eq. 7,
therefore, overestimates the active surfaces involved in
the mass transfer pro-cess. The net eect of this
overestimation is to decrease the average mass transfer
coecient evaluated based on Eq. (7).
g;bed ex;particles
Shbed
dy
g;bed p
D
2 1:8Rep
0:5
Sc
0:333
8
Re
p
m
9
For smaller particles, both Hurt (1943) and Resnick
and White (1949) reported that the particlegas mass
transfer coecient for fixed bed particles can be lower
than that estimated from Eq. (2) for single spheres. Note
that their original results were reported in the form of j Dfactors; those results, however, can be easily converted to
the Sherwood number. The converted Sherwood number
from the above two studies along with those from Eqs.
(2) (for single spheres) and (8) (for large fixed bed
particles) are plotted against parti-cle Reynolds numbers
in Fig. 1. As indicated in the figure, the Sherwood
number for fixed bed particles can be higher or lower
than that estimated by Eq. (2) for well-dispersed single
spheres. For smaller particles, the Sherwood number can
be much lower than the theoretical minimum of the
Sherwood number for single spheres, i.e., Shsingle 2:0.
ex;particles
V 1 e a 0
seg
bed
10
is the
pdsph fs
3
pdsph =6
6
11
d f
sph s
where fs is the sphericity of bed particles (f s 1:0 for
spherical particles and 0 < fs < 1:0 for all other par-ticles),
and dsph is the diameter of spherical particles having the
same volume as the bed particles. Equations (10) and (11)
can be combined to yield
S
61 ebed
fd
12
s sph
ex;particles
seg
The sphericity for dierent solids has been calcu-lated
and is given in Table 1. Note that the term
(fsdsph) appearing in Eq (12) is called the eective particle diameter (deff ) and can be estimated according to
the following approximations:
Table 1
Sphericity of Particles
Sphericity
Type of particles
Sphere
Cube
Cylinder
hd
h 5d
h 10d
Disks
h d=3
h d=6
h d=10
Activated carbon and silica gels
Broken solids
Coal
anthracite
bituminous
natural dust
pulverized
Cork
Glass, crushed, jagged
Magnetite, FischerTropsch catalyst
Mica flakes
Sand
round
sharp
old beach
young river
Tungsten powder
Wheat
Source
1.00
0.81
(a)
(a)
0.87
0.70
0.58
(a)
(a)
(a)
0.76
0.60
0.47
0.700.90
0.63
(a)
(a)
(a)
(b)
(c)
0.63
0.63
0.65
0.73
0.69
0.65
0.58
0.28
(e)
(e)
(d)
(d)
(d)
(d)
(e)
(d)
0.86
0.66
as high as 0.86
as low as 0.53
0.89
0.85
(e)
(e)
(f)
(f)
(f)
(d)
(a) From geometric considerations. (b) From Leva (1959). (c) From Uchida
and Fujita (1934). (d) From Carman (1937). (e) From Leva et al. (1948,
1949). (f) From Brown et al. (1949).
Source: Kunii and Levenspiel, 1991.
irregular particles
with no seemingly
longer or shorter
dimension
(hence
isotropic in shape),
d f d
eff
For
s sph
eff
For
f d
s p
irregular particles
with one somewhat
longer dimension, but
with a length ratio not
greater than 2 : 1
(eggs, for example),
d f d
s sph
shorter
dimension,
but with a length ratio
not greater than 1 : 2,
then roughly,
irregular particles
with one somewhat
deff fsdsph fs dp
For very flat or needlelike
particles, estimate the
relationship between
dp and deff from the fs
values
for
the
corresponding disks
and cylinders. An
alternative
method
for these
15
particles is to
conduct the
pressure drop
experi-ments to
determine the
e ective particle
size.
For very small particles
(< 40 mm), there
are two methods to
determine
the
e ective particle
size. One is to use
the scanning of
magnified
photographs
of
particles and the
other is to conduct
sedimentation
experiments
of
particles
in
a
known fluid; the
terminal velocity of
these particles will
give the diameter
of the equiva-lent
sphere.
Method by Carmon
(1941). The method proposed by Carmon (1941) for
the total exterior areas of
fixed bed particles is based
on the equation
ex;particles
SLA
where
S Sa1 X
and
"
Sa 14
Kt
0:5
18
Pp
19
S
S
dp
20
dN A
dt
i
kg;bedSex;particlesCA
CA
Mesh size
1420
2028
2835
3548
4865
Average
r
3
(g=cm )
X
()
Sa
2
3
(cm =cm )
S
2
3
(cm =cm )
dp
Sd
(cm)
()
0.646
0.626
0.615
0.651
0.607
0.629
0.391
0.411
0.422
0.389
0.430
0.409
88.1
106.5
167.7
187.8
262.5
53.65
62.73
96.93
114.75
149.63
0.089
0.073
0.045
0.039
0.028
4.775
4.579
4.362
4.475
4.189
4.476
Table 3
p;m
Investigators
Resnick and White
(1949)
Kettenring et al.
(1950)
Chu et al.
(1953)
Richardson and Szekely
(1961)
Thodos et al.
(1961, 69, 72)
dt
Lm
Gas
Air
H2
CO2
Air
Process
s. naphthalene
Particles
Naphthalene
(mm)
2101700
(cm) (cm)
2.2 1.32.5
4.4
v. water
3601000
5.9 1015
Air
s. naphthalene
Silica gel
Alumina
Glass
Lead
Rape seed
Active carbon
Silica gel
Alumina
Celite
7101980
10.2 0.39.2
Air
H
Air
s.=sublimation,
v.=vaporization,
Source: Kunii and Levenspiel, 1991.
a. CCl4
a. water
s. dichlorobenzene
v. water
v. nitrobenzene
n-decane
882580
18003100
3.0
5dp
3.8 0.67.0
9.5
11.3
a.=adsorption.
Shbed 0:200 Re
Rep < 90
for 30 <
21
Shbed 0:274 Re
Rep < 80
for 15 <
22
Shbed 0:773 Re
Rep < 60
for 8 <
23
Shbed 0:071 Re
Rep < 40
for 6 <
24
Shbed 0:041 Re
Rep < 15
for 4 <
25
0:33
Sha 0:117Ar Sc
26
with an expression suggested by Avedesian (1972) for the
limiting Sherwood number, i.e.,
Sh
limit
to become
k dy
g;a p
2emf
0:39
27
0:33
28
29
Ar gdp n rg
The authors reported that Eq. (28) describes the
experimental results of their own and those from other
research groups well. The Sherwood number esti-mated
from Eq. (28) is plotted against Rep in Fig. 4
C C
g;bed ex;particles
dNA
dt
u V
b
bubble
dC
A;b
dz
K V
GB
bubble
A;c
With the assumption that fresh gas enters the bed only as
bubbles, Eq. (7) can be rewritten as
dNA
C C
g;bed ex;particles
A
A;b
31
dt
where CA;b is the concentration of A in the bubble phase.
Equation (31) can then be rewritten as
dV
bubble A;b
Ci
A;b
g;bed ex;particles
dt
A
The above equation can be rearranged to become
dCA
V
or
C C
g;bed ex;particles
dC
ex;particles
dt
dC
bubble
dC
dNA=dt
A;b
bubble
A;b
dt
C
A;b
ub
A;b
dz kg;bed
ex;particles
bubble
segment
38
where the terms Sex,particles and Vbubble in the bed segment
can be formulated respectively by
33
g;bed
bubble CA
dt
Note that Eq. (32) implies that
or
A;b
dNA
dC
A;b
37
i
CA CA;b
dt
bubble
dC
dt
32
dt ub
Inserting Eq. (37) into Eq. (34) yields
34
A;b
dt
35
36
Sex;particles A dz1 ef a
and
39
Vbubble A dz d
40
0
In the above equations, a is
the ratio of particle
surface to particle volume defined previously as
surface of a particle
a volume of a particle
0
pdp fs
pdp3=6
11
df
p s
Figure 7 Nomenclature used in developing the model of Kunii and Levenspiel. (From Kunii and Levenspiel, 1991.)
ex;particles
bubble segment
1 ef
dN=dt
V
bubble
dC
kg;bed1 ef a
A;b
dz
C
A;b
43
41
d
i
CA
Inserting Eq. (41) into Eq. (38) yields
dt
dz
b
d
dC
dC
k
A;b
A;b
g;bed
1 e fa
CA;b
With the assumption that equilibrium is rapidly established between CA at the gasparticle interphase and its
i
surroundings, i.e., CA CA;e CA;c, Eq. (43) can be
expressed as
dN
dt ubVbubble
dC
A;b
g;bed
42
and upon combining this with Eq. (36), the equation
becomes
bubble
ef a
dz
A;c
C
A;b
44
kg;bed1 ef a
45
d
Note that Eq. (45) implies that
GB
1 ef a GB
Combining with Eq. (11) the equation yields
g;bed
d y
6D1 ef
46
48
where Kbc is the bubble-cloud interchange coecient
derived by Davidson and Harrison (1963), i.e.,
GB
Shbed g;bed p
d= 1 ef a
D
D
2
yfsdp d
KGBdpy
bc
47
GB
Kbc
4:5
0:5 0:25
5:85 D g
mf
49
db
db1:25
K qk S
bc
bc ex;bubble
where
3p
q 4
and
50
U d
51
mf b
g
0:5
kbc 0:975D
db0:25
Inserting Eq. (48) into Eq. (47) yields
52
yfsdp d
Shbed 6D1 ef bc
53
The above equation provides a correlation for estimating Shbed (or kg;bed) based on particle and fluidization
properties, which then can be used to determine the
rate of mass transfer employing Eq. (7) based on the
homogeneous bed approach. In the application, the
following equations provided by Kunii and Levenspiel
(1991) are needed for calculating fluidiza-tion properties
appearing in Eq. (53)
U Umf
ub
d
54
ub U Umf ubr
0:5
ubr 0:711g db
55
56
1 ef 1 emf 1 d
57
The above equations indicate that, besides gas and
particle properties, the fluidization properties are a
function of bubble size only.
K g a 0k
GB
df k
K g
g;single
bc
p s
g;single
bc
Sh
single
KGB gb dpfs
single
Sh
single
60
fsdp2y
6 Sh
Sh
bed
6D1 ef
single
gb
fsdp y
g Sh
single
63
g;single p;mean
64
65
fd
s p
a
Note that, in Eq. (64), m is the adsorption equilibrium
constant defined as
Kbc
yfsdp d
6k
Kbc
dpy
#
gbShsingleZd fsd6p y Kbc
ef
Zd 1 a=m
and
gb
59
Sh
"
bed
where
dpy
Equation (58) can be rearranged to become
g;single
Sh
58
CAs mCA
bc
fsdp y Kbc
61
66
0,
and
Eq.
and d
(63) reduces
to Eq. (53). For
highly adsorbing particles, m is on the order of thousands, in which case Zd ! 1:0 and Eq. (63) becomes Eq.
(61). For porous but nonadsorbing particles,
m ep, and Eq. (63) can be used to estimate Shbed. In
demonstrating the eect of the particle adsorbing
property on the mass interchange coecient,
Wakabayashi and Kunii (1971) reported that the K GB can
be greatly enhanced even with a small value of (g bZd).
Their reported values are shown in Table 4. Rietema and
Hoebink (1975) also reported that their measured gas
interchange coecients increase in bub-ble size and
commented that this was just the reverse of the prediction
of Eq. (49) for Kbc. According to Kunii and Levenspiel
(1991), this is because the first term of Eq. (63)
dominates for large bubbles, caused by more vigorous
splitting and coalescing of bubbles.
3.2 Model of Partridge and Rowe (1966)
In this class of models, the cloud surrounding the bub-ble
is considered the primary mass transfer boundary, and the
bubble and the cloud phases are considered a perfectly
mixed single phase, as indicated in Fig. 6(b). The mass
transfer equation then has the form
Table 4
db;m (m)
1
KGB;measured (s )
calculated, with gbZd 0
K
0.04
0.06
0.08
0.11
1116
5
918
3
814
2
711
1.6
13
12
12
11
GB
dNA
dt
7
w
h
mf
e u
mf b
kgt p
Copyright 2003 by Taylor & Francis Group LLC
pdb
Table 5 Interphase Mass Transfer Models and Coefficients for Ozone Exchange in an Air-Fluidized Two-Dimensional Bed
k
Model
Coecient
Reference
1. Penetration
Chavarie
(1973)
Walker
equivalent
k
4Demf ub
k
gc
gc
(1970)
dc
0:93
gt
gc
dc
mf
e U
gc
gc
(1970)
Kunii and Levenspiel
0:33
" k
sc
0:6
0:26DRec
Sc
dc
4Demf uba 1
gc
1=2g=db 1=4
q 2Umf dbw
7. Murray through-flow,
Murray (1965)
no diusion
Empirical value (from Charvarie and Grace, 1976a)
mf
ubD 1
1:02emf
k
gc 1
0.0030
kgcQ
0.0051
kgcSb Q
Q q kgbSb
4Demf ub
k
gc
pdc
6. Toei et al.
gc
pd a
kgb 0:6D
(1969)
0.0020
mf gc
0.0051
0.0017
2k
a 1
mf
Calculated
kgt (m/s)
2 =
da
a 1
k k
gc
q=S
gs
0.0056
0.0160
kgb 0
0.0160
q Umf dbw
dC
dN
A;b
pdb
75
4
U
e u
mf
4 mf b 0:5
KGT db gt
1:5Umf
76
12 Demf ub
0:5
1:5
pdb
db db
The corresponding mass transfer equation for K GT
appearing in Eq. (76) is
dt Vbubble
A;e
dt KGTVbubble
77
C
A;b
r
e
ue
b mf
0:33 0:33
kgt 0:127D
0:22
w
h
Cor
r
T
h
T
h
e u
mf b;m
pd
kgt;m 0:4Umf
b;m
Since bubbles are also smaller near the grid, they concluded that favorable gassolid contacting occurs in this
region primarily because of convective outflow followed
by recapture.
Qor uor 4 or
83
and kbe1 represents the diusive mechanism, which can
be predicted by the penetration theory expression, i.e.,
k
4 Demf
0:5
84
ptf
be1
Their results indicated that the convective mechanism
has a greater eect on the grid region mass transfer.
a01
mf
1 0:67m
be
1 emf
1:5
0:5
85
Umf
u e
86
b mf
0:5
0:333
Nubed kg 2 1:8Rep Pr
87
Pr g
88
Note that the corresponding equation for the Sherwood
number has the form
dy
g;bed p
Shbed
2 1:8Rep
0:5
Sc
0:333
89
The above discussion implies that the correlation equa-tions derived for Nu bed based on heat transfer experi-ments can
also be converted to the Sherwood number for estimating kg;particles.
CONCLUDING REMARKS FROM KUNII AND LEVENSPIEL (1991)
It is worth bringing up the concluding remarks of Kunii and Levenspiel (1991) at this point to conclude the chapter
regarding particlegas mass transfer in a fluidized bed. Three points were made: first, particles dispersed in bubbles
should be taken into account when kinetic processes, such as mass transfer, are car-ried out in fluidized beds; second,
when dealing with a gaseous component that is adsorbed or somewhat cap-tured by the bed solids (or else desorbed),
Kbc should be used carefully to represent the movement of these adsorbed gaseous components; third, the mass transfer
coecient measured for the bed as a whole, kg;bed, is model dependent. For large-particle cloudless bubble
beds, the plug flow model closely matches the flow conditions in the bed, and the kg;bed should match
the single particle coecient, i.e., k g;single. However, for fine-particle clouded bubble beds, the k g;bed may be well
below that of kg;single.
EXAMPLE CALCULATIONS
Two examples are given here to demonstrate the eects of d b and gb on the prediction of the particlegas mass transfer
coecient based on Eq. (61). The calculated results are then compared with the experimental data of Resnick and
White (1949).
Example 1 Effect of db on Shbed based on Eq. (61)
3
Determine. The relation between Shbed and Rep based on Eq. (61) with db 0:1, 0.2, 0.37, 0.5, and 1 cm.
Solution. Equation (61) has the form
Shbed
g Sh
d
1
ef
single
fsdp2y !
Kbc
6
D
From Eq. (6)
rgudp
Rep
At ut 69 cm=s;
r ud
Re
g t p
p;t
m
Then Eq. (2) gives
0:00118690:028 12:66
0:00018
0:5
0:33
4:84
db
1:21
db1:25
0:065
0:5
980
0:25
4:5
5:85
0:37
0:37 1:25
43:63 s
Combining Eqs. (54) through (57), i.e.,
U Umf
ub
d
ub U Umf ubr
ubr 0:711gdb
0:5
1 ef 1 emf 1 d
we obtain
U Umf
1 ef ubr1 emf
U 1:21
0:5
6:77
Also
2
fd y
s p
0:4 0:028 1
10 4
8:04
6D
6 0:065
Combining (A) through (D) yields
d
g Sh
b
single
Shbed 1 ef
U 1:21
fsdp y
6D
bc
0:0088U
0:011
Then, since
Re
rgUdp
0:028U0:00118
0:184U
p
0:00018
m
Combining expressions (E) and (F) gives
Note that the above equation is generated based on d b 0:37 cm. This calculation procedure can be easily repeated for
dierent bubble sizes at 0.1, 0.2, 0.5, and 1.0 cm. The generated equations for these dierent bubble sizes are plotted in
Fig. 9 along with the experi-mentally observed data of Resnick and White (1949). The results indicate that the
correlation based on db 0:37 cm describes the experimental data best. The results in Fig. 9, however, indicate that the
Sherwood number is sensitive to the bubble size selected; a smal-ler bubble size generates a higher Sherwood number,
i.e., a higher mass transfer coecient.
Example 2. Effect of cb on Shbed based on Eq. (61)
Data. Same as Example 1; but, with db 0:37 cm.
and Rep
Figure 10
Determine.
based on Eq. (61) with db 0:37 cm and gb 0:001, 0.005, and 0.01.
Solution. The identical procedure as is demon-strated in Example 1 can be used to evaluate Sh bed at different gb. The
results are shown in Fig. 10 where, as expected, a higher g b will generate a higher Sher-wood number. The results in
Fig. 10 clearly indicate that, in addition to bubble size, the selection of g b is also essential in the estimation of the
particlegas mass transfer coeffficient based on Eq. (61) proposed by Kunii and Levenspiel (1991).
NOMENCLATURE
2
m1
= concentration of A in bulk gas phase, kg-mol/
CA
C
m3
A;b
A;c
p;a pi
p;m
A;e
be
sph
As
Cp
d
db
b;m
dc
eff
or
dp
dp
bc
dt g
be1
hh
kg
0
Kbe
g;a
bc
GB
GC
K
K
GT
GT;m
Kt
g;bed
g;single
gc
gt
gt;m
je
K1
Lm
Sh
Sha
Sh
bed
Sh
Sh
limit
single
d y=D
g;single p
= time, s
= bubble formation time, s
t
p;mean
= mean particle residence time staying in bubble
phase, s
= superficial gas velocity, m/s
tf
=
=
=
=
mf
u
ub
u
b;m
br
uc
ue
=
=
=
=
=
=
=
or
uR
ut
V
bubble
V
cloud
seg
a0
gb
bed
ef
e
mf
rg
r
fs
= kinematic viscosity, m /s 3
= density of gas, kg/m
3
= density of particle, kg/m
= dispersion parameter defined in Eq. (64)
= sphericity of a particle
= constant, 3:1416
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coal particle: a review of drying, devolatilization and mass
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Avedesian MM. Combustion of char in fluidized beds. PhD
dissertation: University of Cambridge, 1972.
Bauer W, Werther J. Proceedings of 2nd World Congress
Chemical Engineering, 1981, p 69.
Behie LA, Kehoe P. The grid region in a fluidized bed reac-tor.
AIChE J 19:10701072, 1973.
Behie LA, Bergougnou MA, Baker CGJ. Mass transfer from a
grid jet in a large gas fluidized bed. In: Keairns DL, ed.
Fluidization Technology, Vol 1. Washington DC:
Hemisphere, 1976, pp 261278.
Bohle H, Van Swaaij WPM. In: Davidson JF, Keairns DL, eds.
Fluidization. London: Cambridge University Press, 1978, p
167.
Brown GG. Unit Operations. New York: John Wiley, 1950.
Carmon PC. Fluid flow through granular beds. Trans Inst
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