CkmicaI Engineering Science. Vol. 42, No. 2. pp. 341-351, 1987. ooo9-2509/87 $3.00+0.

00
Printed in Great Britain. 8 1987. Pergamon Journals Ltd.

POPULATION BALANCE MODELLING OF BUBBLING

FLUIDIZED BED REACTORS-I. WELL-STIRRED DENSE
PHASE
IAN R. SWEET, S. SCOTT GUSTAFSON and DORAISWAMI RAMKRISHNA?
School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, U.S.A.

(Received 21 June 1985; accepted 24 June 1986)

Abstract-A detailed population balance model is presented for a duidized bed reactor incorporating: the
formation of bubbles at the grid plate, their rise with velocities governed by their sizes, random coalescence
between bubbIes, gas exchange between bubbles and the dense phase, and a first order chemical reaction in
the dense phase under well-mixed conditions. Reaction conversion is calculated as a function of
dimensionless parameters relating the rates of various competing processes such as coalescence, dense phase
mixing, mass exchange between bubbles and dense phase and reaction rate. Comparison ofconversions with
those of Davidson et al. (1977) show significant variations indicating that the dynamics of bubble size
distributions could have non-trivial erects on the extent of reaction. Fluctuations in bubble populations did
not seem strong enough to translate to strong fluctuations in reaction conversion.

1. INTRODUCTION The vigorous particle-mixing promotes better heat and

While considerable understanding of the behaviour of
fluidized beds has accumulated in the last two decades,
it has emerged that the system is an extremely complex
one and has attracted many diverse approaches
towards their modelling. The importance of modelling
to design and control of such complex equipment has
been eloquently expressed in the past (Lee and
Weekman, 1976). The issue is one of framing suitably
sophisticated models and, in this regard, the fluidized
bed has presented widely varying perspectives to
modellers with different backgrounds and conse-
quently with rather contrasting directions of emphasis.
This is as it should be in dealing with the many-faced
contraption that the fluidized bed has proved to be.
Indeed, there are excellent reviews of the literature on
fluidized bed reactors. In particular, the compilation
edited by Davidson and Harrison (1963, 1971) brings
together the multifarious efforts addressing different
aspects of fluidized beds.
Of interest to this paper is the subject of aggregatiue
fluidization, characterized by the appearance of gas
bubbles thinly populated by particles as against a
dense ‘emulsion’ phase crowded with particles. The
bubbles promote mixing between particles and in the
gas phase. The subject has been comprehensively
reviewed by Potter (1971). The bubbles, in ascending
through the bed, coalesce to form larger bubbles
before emerging at the top. Indeed bubble-splitting
occurs in conjunction with coalescence although the
net effect is to produce very large bubbles before the
gas phase exits. Detailed photographic captures of
bubble-splitting and coalescence are available in a
review article by Rowe (1971).
The phenomenon of bubbling has complex and
opposing effects on the operation of a fluidized bed
reactor in which the particles are of catalyst material.
+Author to whom correspondence should be addrkssed.
mass transfer to the external particle surface. On the
other hand, back-mixing has the usual negative impli-
cations for non-autocatalytic reactions. Furthermore,
the gas in the bubble phase is denied access to the
catalyst although this is alleviated by some exchange of
gas with the dense phase. The diminished conversion
resulting from the by-pass of gas with the bubbles can
be very substantial.
The modelling of fluidized catalytic reactors has
recognized the existence of the gas (bubble) and
emulsion phases, the former virtually involving no
chemical reaction which is deemed to occur exclusively
in the emulsion phase. The variation in modelling has
consisted in introducing different states of flow in the
two phases. The simplest, but succintly educative
model (Davidson et al., 1977) arises from assuming
that the dense (emulsion) phase is perfectly mixed
while the gas phase describes ‘plug’ flow as bubbles,
ascribed a uniform size. The provision is made here for
exchange between the particle and gas phases. The
model has been discussed in detail by many authors
(Davidson et al., 1977; Orcutt et al., 1962; Calderbank
and Toor, 1971). There have since been varying orders
of sophistication in modelling in’which connection the
many contributions of Amundson and co-workers
deserve special mention (Bukur and Amundson, 1975;
Caram and Amundson, 1979).
A constant and uniform bubble size implied by the
models of Orcutt et al. (1962) is a strong idealization.
As aptly pointed out by Calderbank and Toor (1971)
there is sufficient experimental and theoretical evi-
dence in the literature to make clear that the bubbles,
as they rise through the fluidized bed increase in size
due mostly to coalescence, although there may also
be some increase in size due to influx of gas from
the dense phase. If the reaction rate is relatively fast
and the overall conversion is largely determined by
the rate of interphase gas exchange the assumption
of a constant bubble size for the whole bed

341
342 IAN R. SWEET
becomes inappropriate. It is of interest, therefore, to
estimate the variations in bubble sizes and to modify
appropriately the equations of bubble motion.
Calderbank and Toor provide ample references to
substantiate their arguments. Unfortunately, however,
the accounting for bubble coalescence as presented by
them does not address directly the issue of coalescence.
Indeed a direct attack must draw on the framework of
population balances (Hulburt and Katz, 1964). There
have been no instances of such an approach except for
a paper due to Argyriou et al. (1971) subsequently
examined under a more general stochastic framework
by Shah et al. (1977a) in view of the fact that the bubble
population dwindles to a small number.? Neither of
these papers, however, consider chemical reaction in
the bed.
There have been detailed simulative approaches to
predicting bubble size distributions such as by Nguyen
et al. (1976) in which care was taken to follow the
location of every individual bubble in the bed and
coalescing those in suitable proximity of one another.
Based on the argument that such simulation pro-
cedures can be very time consuming, Mori et al. (1984)
have considered a very simple steady-state formulation
in which the variation in the number of bubbles along
the vertical and radial directions caused by coalescence
is described by a simple first-order partial differential
equation. While this modei appears to have parameters
that can allow reasonable agreement with experimen-
tal data its adaptation to handle chemical reactions is
unclear.
The objective of this paper is to model the fluidized
bed reactor within the framework of population
balances so that we may account for the effects of
bubbling on reactor conversion in a rational manner.
More specifically, it will be our endeavour to determine
the multivariate number density function associated
with bubble populations in the fluidized bed whose
evolution is a result of bubble coalescence and split-
ting. We will be only concerned with a first-order
isothermal reaction since a number of past models will
be available for comparison; besides, the effect of
bubble by-passing on conversion may be evaluated
with a minimum of additional computational burden.
The technique to be employed, however, is indeed
capable of handling non-linear kinetic and non-
isothermal effects if computational constraints are not
severe.
It is emphasized here that very little quantitative
information concerning the actual break-up and
coalescence rates of bubbles is available. In this regard,
the objective of this paper is to evaluate the effects of
bubble break-up and coalescence rates on reaction
conversion using characteristic dimensionless par-
ameters. Even more importantly, it will serve the
purpose of establishing that the methodology for
* More recently,Matsuura and Fan (1984) have reported
experimental measurements of bubble size distributions in
gas-liquid-solid fluid&d beds.
et al.
Gas exit
9
Z-H
. . .
.
. -a.
_+IBubbCtS
.
-10.
Dense
0 cj”“”
Q Q
Grid plate .___(2.___~___O________~.G
fi
Gos inLet
Fig. 1. Schematic of fluidized bed reactor.
analysing such complex phenomena does indeed exist
and that quantitative experimental work towards
determination of coalescence and break-up rates in
fluidized beds would be a valuable undertaking.
2. THE POPULATION BALANCE MODEL
We consider a fluidized bed reactor (see Fig. 1 for a
schematic diagram) in which catalyst particles are
fluidized and essentially confined to a dense phase
while the reactant (A) in the gas phase exists both in the
dense phase where the reaction occurs and in the
bubble phase which promotes no reaction. The chemi-
cal reaction
Ak+ products
occurs isothermally in the dense phase.
We assume that bubbles are formed at the grid, rise
through the bed at velocities characteristic of their size,
coalesce with other bubbles or break up into smaller
bubbles, and eventually emerge at the top. While in
flight the bubbles exchange gas with the dense phase at
rates that have been investigated by Davidson et al.
(1977). In addition, mass transfer of the reactant occurs
between the bubbles and the dense phase at rates
determined by a suitable mass transfer coefficient.
The choice of particle coordinates in a general
particulate system has been discussed by Ramkrishna
(1978). In the present case, the bubble coordinates
must include its size (as determined by bubble volume),
its locution and the concentration of reactant (assumed
to be uniform). The location of the bubble in the bed is
taken to be the vertical distance of its centre of mass
measured from the grid plate. This implies that the
bubble location on any plane perpendicular to the
 Population balance modelling of bubbling fluid&d
vertical axis is adjudged immaterial. It is assumed that
transverse motion is random and that ‘coalescable
bubbles’ are determined only by their proximity with
respect to the vertical coordinate.
Thus we let the expected number of bubbles with
volume between v and v + dv, at height between z and
z +dz, and possessing reactant at a concentration
between c and c + dc be given by
fr (v, z, c) du dz dc.
We emphasize here that since the bubble distri-
bution is deemed to be independent of location along a
given cross-section the number density fi may be
regarded as integrated over the cross-section of the
bed. Time does not appear in the trivariate number
density function above because the bed is assumed to
be at steady state. It appears to be well established that
there exists a maximum bubble size v,,, both theoreti-
cally (Davidson and Harrison, 197 1; Rice and Wilhelm,
1958) and experimentally (Matsen, 1973). If the feed
concentration of the reactant is co, then clearly the
domain of the density function fr is given by 0 < v
< “Inax*0 < z < H, and 0 < c < co. The population
balance equation is an equation in the number density
functionf, (v, z, c). Before identifying this equation we
dispense with some preliminaries which have to do
with how the volume u of a bubble, its location z, and
concentration c can vary for a single bubble as it
ascends through the bed.
Volume change of bubble and bubble velocity
The volume of a bubble may vary because of varying
net gas exchange with the particle phase and because of
the diminishing pressure encountered by the rising
bubble. While any available information on gas ex-
change with the particle phase is easily incorporated,
we will neglect any net exchange. Note that the volume
changes envisaged here are continuous changes in
which the identity of the bubble concerned is pre-
served. Thus coalescence, which changes the volume of
a bubble but also destroys its identity (and those of the
other bubbles with which coalescence occurs), is not
included in this consideration.
The rate of change of volume of a bubble of volume
u at location z (the reactant concentration being
virtually immaterial) will be denoted V(v, z). Further,
we let u(u) be the velocity of the bubble of volume v and
the pressure at the top of the bed be pa. Then based on
ideal behaviour it is readily established that
Mv)
V(v, z) = far as such an event can be approximated by a rapid
(H -z + P,/P,z)
where p, is the density of the particle phase and H is the
height of the fluid bed. The bubble velocity U(V)is not
an entirely well-characterized and accessible quantity
particularly because it should be influenced by its
fellow bubbles. Without some simplifications, this
problem becomes exceedingly complex. There are also
other complications to which Davidson et al. (1977)
allude that make this issue even more difficult.
Following these authors,,we will accept for the present
bed reactors-1 343
the estimate based on
6v “6
u(u) = U-U&+0.71
0 n
where V is the prevailing superficial velocity and iJmf
that at incipient fluidization. Some further discussion
on this issue appears in the work of Argyriou et al.
(1971).
(1) Concentration change in bubble
The rate of change of reactant concentration in the
ascending bubble, denoted C(v, z, c), may be obtained
from Davidson et al. (1977). Thus
vC(u, z, c) = (q + &a) (cP -c) (4)
where we have accounted for change due to bulk
exchange rate q and due to mass transfer via the mass
transfer coefficient times the interfacial area, K, a. The
z dependence of C may be inherited from that of the
local dense phase concentration, cP. In this paper, we
make the assumption that the dense phase is well-
mixed so that c,,, and hence C, are independent of z.
The exchange rate 4 has been the subject of discussion
by Davidson et al. (1977). It results from a remarkable
two-phase hydrodynamic model. For other than slugs
it is given by
/?..\213
q = 3x 2 v,,.
\ )
Bubble break-up and coalescence
Quantitative information on the rates of break-up
and coalescence of bubbles is virtually non-existent. In
view of the fact that maximum bubble sizes have been
found, bubble break-up does indeed occur. Rowe
(1971) seems to suggest that splitting is essentially
binary with the daughter bubble sizes distributed
asymmetrically. It is possible to model the break-up
phenomenon along the lines of Narsimhan et al.
(1984). However, in the absence of any real quantitat-
ive information and, in view of the fact that coalescence
is indeed the overwhelming phenomenon leading to
the progressive increase in bubble sizes observed, we
neglect the contribution of break-up to the bubble size
distribution. It is emphasized that the techniques of
this paper are just as easily used to include both break-
up and coalescence. Further considerations will be
restricted to coalescence rates and bubbles only.
Coalescence must involve two or more bubbles. The
problem of accounting for coalescence featuring more
than two bubbles becomes very complicated but in so
succession of binary coalescence events, it may be
reasonable to assume that coalescence may occur only
between two bubbles at a time. Argyriou ef al. (1971)
assume that the coalescence rate is proportional to the
mean projected area of the coalescible pair (which
must necessarily be at the same bed height). Yoshida et
al. (1978) introduce a slight variation over the coalesc-
ence rate of Argyriou et al. (1971) based on the
argument that coalescence is consequent upon relative
motion between the two bubbles.
344 IAN R. SWEET et 01.

Shah et al. (1977a) have argued that bubble popu- reflects the fact that all entering bubbles contain gas of
lations may become so small that fluctuations could, in reactant concentration c0 _
some circumstances, play a considerable role. Thus the
more general stochastic framework presented by The population balance equation
Ramkrishna and co-workers (1973, 1976) may be The population balance model is now complete and
necessary for such analysis. In this connection, the the relevant equation for the expected number density
simulation technique of Shah et al. (1977b) based on fi (u, .z, c) is readily identified. Under steady-state con-
the method of the interval of quiescence, automatically ditions, we have
accounts for any fluctuations that may be important.
In this paper we will use the coalescence model of $c V(U,Z)f 1(~TG41+~[u(o)f, (u,z,c)l
Argyriou et al. (1971), slightly modified by Shah ef al.
(1977a) (to account for the fact that coalescable
bubble-pairs may not necessarily be exactly at the same
bed height), to analyse the effect of bubble coalescence
and interactions with dense phase on reaction conver-
sion. Thus the coalescence frequency is taken to be

0 Iz -2’1 > d(u, u’)

Q(u,.z; u’,z’) = 113 + u’ 1’3)2/k;/3, (6)
kz(u I2 --‘I sz d(u, u’)

where

is the least distance of separation between the two

bubbles beyond which coalescence between them is
+ E$)]
($)“” Tf2(”- u~,z~,c~;u~,z,
impossible; k3 is a shape factor relating to vertical
‘diameter’ of the bubble to its volume, determined
experimentally by Argyriou et nl. (1971). The coalesc-
ence rate constant k2, which may be expected to
depend on the dimensions of the fluidized bed, particle
properties and the rate of gas flow, is a quantity to be
obtained from experimental observations of bubble in which the function f2(u,z,c; u’,z’,c’) is the second-
size distributions of various heights. order product density (see Ramkrishna and
Following Shah et ul. (1977a) we stipulate that the Borwanker, 1973; Ramkrishna et al., 1976). Equation
coalesced bubble is instantaneously at the location of (9) is subject to the ‘initial’condition (8). Consideration
the larger bubble. of the second-order product density leads to a closure
problem since an equation forfi would containf, and
Bubble sizes at the grid so on (Ramkrishna and Borwanker, 1973). However,
The bubbles which appear in the bed are formed at since the actual solution to the problem can be
the grid. Experimental data are available on the sizes of obtained by an artificial realization of the process from
such bubbles (see, for example, Harrison and Leung, an initial condition, the closure problem need not
1961; Yates et al., 1984). There are also theoretical concern us here. We shall return to this problem later.
predictions of such bubble formation (see Kumar and It is convenient to characterize the dynamic effects
Kuloor (1970). We assume here that the bubbles which of bubble coalescence by suitable dimensionless
enter the bed are all of uniform volume u,,. For a groups. Accordingly, we non-dimensionalize the popu-
superficial velocity U we may then write for No, the lation balance equation using the following dimen-
number density of bubbles entering the bed over the sionless quantities
entire cross-section S

S(U - Urn,)
(7)
N =

0 9 ug = u(uo).
uouo
The condition that the entering bubbles are all of
uniform volume u0 translates to

fi (r,O,c) = Noh(r - 00) h(c - co) (8)

where 6 is the Dirac delta function and c0 is the
reactant concentration in the feed gas. Equation (8)
 Population balance modelling of bubbling fluid&d bed reactors-I 345
where we have permuted the arguments in c$~ and & general. In this paper we will assume that the dense
merely for alphabetical sequencing. The foregoing phase is thoroughly mixed and may be modelled as a
non-dimensionalization leads to the coalescence rate perfectly stirred tank reactor. In Part II we relax this
parameter assumption and instead use an axial dispersion model
for the dense phase.
(10) If the dense phase is perfectly mixed, mass balance
on the reactant leads to
which compares the characteristic coalescence rate (for
the feed bubbles) to the rate of their ascent through the If
su,,,, (co - cp) - kSf&cp = umar&,, &
bed. Small values of w relative to unity will imply that
s0 s 0
coalescence does not occur much in the bed.
The balance equation (9) may be rewritten in
dimensionless form as
X
s
“dc u&(v,z,c)f, (o,z,c)
0
where H is the height of the fluidized bed. Substituting
(13)

(4) into (13) and solving for cp we obtain

If&, is the average concentration of the reactant in the

outgoing bubbles

The mean concentration cH of the reactant in the entire

gas phase leaving the bed is obtained from

c” = (=$!+bH+(+)Cp. (16)

Letting cH/co 3 c’ be the dimensionless exit concen-

tration in the efIIuent gas we get

where A = d/H,,. The dimensionless version of the

initial condition (8) is where

91 (th,O) = w7 - l)b(S - 1). (12) H

(q-C&&a), i=;, k’=kmf.
u
The dense phase equation must be identified to mf

complete the formulation of the problem.
3. DENSE PHASE MODEL
The balance equation (9) [or its dimensionless form
(1 I)] is written without regard to the state of mixing in
the dense phase and to this extent eq. (9) is quite
The quantitative analysis of the model consists in
solving eq. (9) simultaneously with eq. (13). Before we
address this issue it is instructive to see how the present
model degenerates into the more elementary models of
the past. Suppose, for example, the entering bubbles
leave without any coalescence between bubbles.
346 IAN R. SWEET et al.

Assume further that the bubble volume does not to the population balance framework has been dis-
change as it ascends through the bed. Then the present cussed by Ramkrishna (198 1). The simulation not only
model must simplify to the one presented by Davidson produces average values but also computes fluctu-
et al. (1977) which assumes that the dense phase is well ations about the average values.
mixed and that the bubble phase consists of identical Shah et al. (1977a) have employed their simulation
non-coalescing bubbles. When no coalescence occurs technique to predict bubble size distributions in a
we must set o = 0 in eq. (II) to obtain fluidized bed without chemical reaction. The inclusion
of chemical reaction is conveniently made in the
foregoing simulations. The technique, being essentially
transient in nature, requires an initial condition stipu-
For constant bubble volume, q = 0. Further if 4 is lating the state of the entire population (that is the
independent of < (but dependent on v) then the above bubble trivariate distribution in size, location and
equation becomes reactant concentration in this case) and evolves to the
steady-state distribution. With chemical reaction to be
accounted for, since the concentration change in each
bubble depends upon the dense phase concentration
(not at first available because of the coupling between
The foregoing equation is readily solved subject to
the population balance and the dense phase equations),
condition (12) yielding
the bubble population can be simulated only for
assumed values of the dense phase concentrations, c~.
9, (S,rl.i) = exp [ “‘y&I i 1-t6 5, - (<, - 0 For each such assumed value of cp, the simulation

(18)
yields the number density fi, which on substitution
xexp
[ rli(rl)P
1>
“(‘1!(1-, -1 b(q- 1)
into eq. (14) will produce a new value of c,, generally at
variance with the assumed
used in a successive
one. While
approximation
this could be
scheme for the
where we have set 5, E c,/cO and p = (U - U,,)/U.
assumed and calculated dense phase concentrations to
Substitution of (18) into the dimensionless version of
agree within specified limits, another approach, which
(14) gives after some algebra
has some computational advantages, is as follows.
1 --fieeX Because the bubble coalescence rate has been assumed
tl, = (19)
to be independent of reactant concentration (and thus
1 +k’-flepX
where the dense phase concentration) the dynamics of the
x ~ K(l)(l -8) 4 bubble size distribution in the bed is unaffected by the
reactant concentration in the bubbles. Thus the mul-
B
tiple simulations do not have to be repeated for each
the right-hand side of which is readily shown to be the assumed cp if, in the simulations, the updating of
same as (4 + KGa)H/u,u(v,), an expression used by bubble concentrations during a quiescence interval is
Davidson et al. (1977). When eq. (18) is plugged into performed for each cp. The calculated values of cp for
the dimensionless form of (15), denoting cbH/cO by <bH different assumed values of it are obtained from a
we get single set of sample paths. By plotting the calculated cp
<,(l -e-x)+e-x. vs the assumed value the intersection of the curve with
<bH = (20)
the line representing equal values of the ordinate and
When (19) and (20) are employed in (17) abscissa the correct steady-state value of c,, is obtained.
This value of the dense phase concentration may again
l-z++z
c’=Peb,,+(l-B)&,= 1_z+-t, , Z=PepX be used for a simulation as a second check and to
obtain the actual number density function fi. Once the
which is the expression derived by Davidson et al. number density function is calculated the fraction
(1977). Thus we have shown that the coalescence model unconverted in the gas leaving the bed, c’, is obtained
here simplifies appropriately in the limit of vanishing from eq. (17).
coalescence. Computations were made on a Cyber-205 at the
Purdue University facility. The simulation times re-
quired varied from 30 s to 9 min of CPU time to
4. COMPUTATIONS compile and run. Naturally, smaller coalescence rates
The numerical solution of eqs (11) and the dimen- needed the greatest amount of computer time since
sionless form of (13) is a very formidable task because larger numbers of bubbles are encountered in this case.
of the trivariate nature of 4, and the possibility of
statistical correlation between bubble states (which
presents a closure problem). However, a very effective 5. RESULTS AND DISCUSSION
alternative is available in a simulative approach due to At the level of analysis in this paper we are
Shah et al. (1977b) which consists in artificially realiz- examining effects not quantitatively studied in exper-
ing the process by Monte Carlo simulations. The imental works on fluidized bed reactors. Hence the
mathematical relationship of the simulation technique computations made in this paper have generally been
 Population balance modelling of bubbling fluidized bed reactors-I 347
with a view towards establishing the major directions Table 2. Heights and thicknesses of
in which the reactor behaviour changes with the bed slices
phenomena for which account has been made. In this
Slice no. Height (in.)
connection the experimental data of Argyriou er 02.
(1971) provide a useful starting point for our compu- 1 o-1.54
tations. Table 1 lists the dimensions of the bed, 2 1.54-3.08
operating conditions, the feed bubble size, and values 3 3.084.62
4 4.62-6.16
of the parameters in the coalescence model. Table 2 5 &l&7.70
shows a discrete partition of the fluidized bed with 20 6 7.70-9.24
slices within which the events occurring in the bed will 7 9.24-10.78
be viewed. The calculations include not only average 8 10.78-12.32
values of various quantities but also fluctuations about 9 12.32-13.86
10 13.8~L15.40
the mean. 11 15.4CLl6.94
The main parameters whose effects are to be 12 16.94-18.48
evaluated are the dimensionless coalescence rate w, the 13 18.48S20.02
dimensionless reaction rate k’, and the dimensionless 14 20.02-21.56
15 21.5C23.10
constant Z which contains the exchange rate of 16 23.10-24.64
reactant between the dense phase and the bubbles. 17 24.626.18
First, we examine the bubble number distribution in 18 26.18-27.72
the bed. Since the model does not account for any 19 27.72 29.26
20 29.2C30.8
dependence of coalescence rate upon either reaction or
gas exchange the only relevant parameter which can
alter the bubble number and size distribution in the increased coalescence rates. For the lowest coalescence
bed is the coalescence parameter. Figure 2 shows the rate the standard deviation about the average number
mean value of the cumulative number of bubbles and of bubbles increases progressively throughout the bed.
its fluctuations as a function of bed height for three This follows from the fact that at the entrance of the
different coalescence rates. The figure clearly reflects bed the number of bubbles is assumed to be known
the drastic reduction in the number of bubbles with exactly (i.e. zero standard deviation) and thereafter
random coalescence leads to an increasing standard
Table 1. Values of fluidized bed parameters used in the deviation about a smaller average. If the bed were high
simulations enough this standard deviation would eventually drop
since the mathematical limit of the process is a single
u mf 0.042 in. s ’ bubble with zero standard deviation. Although this
u 0.08652 in. s 1
14.0 in.“’ s- ’ does not occur with the low coalescence rate the drop
k,
kz 0.364, 1.5, 3.64 in.-‘s-l in standard deviation at higher rates is apparent from
ks 0.125 Fig. 2. Figure 3 illustrates the number of bubbles in
H 30.8 in. each slice and the standard deviation for the low
DR 11.5 in.
coalescence rate. Table 3 reinforces the above
VO 0.037 in.3
conclusions.

I
0.:0,87 0.186410
I 0.322634
I 0.458857
I 0.5930W
I 0.731303
I 0.867527
I I. 00373
I

Fig. 2. Cumulative average number of bubbles vs dimensionless reactor height for all three coalescence rates.
348 IAN R. SWEET ef al.

24.0

z
I’
* Number of bubbles
2
12.0
0 2 x standard deviation
z t

O.&W37 0 195410 0.322534 0.459957 0.595090 0.731303 0.957527 1.00375

Fig. 3. Averagenumber of bubbles and twice the standard deviation about the averages vs dimensionless bed
height for w = 291.3.

Table 3. Results of the hydrodynamic model

Ave. no. SD ave. no. Ave. no. in SD ave. no.

‘0 in bed in bed top slice top slice

291.3 101.8 4.5 0.87 0.70

1200.4 35.5 3.4 0.34 0.48
2913.0 21.6 2.4 0.42 0.50

Figure 4 shows the bubble volume distribution on a
cumulative basis at three chosen bed heights, one at the
bottom region, another in the middle and the third at
the top. At the bottom of the bed the cumulative
number fraction rises quickly to unity for small bubble
volumes (since the bubbles there are small). For the
middle section the rise to unity is gradual as one should
expect. Near the top of the bed the existence of large
sized bubbles leads to a steep rise of the cumulative
distribution to unity for a large bubble volume as it
should.
Next, we examine the model predictions for re-
action conversion. The conversion (or c’ which is the
result of deducting the conversion from unity) depends
upon the parameters, o, k’and Z. Figure 5 shows c’, the
unreacted gas fraction, as a function of k’ for various
coalescence rates for a fixed Z (representing a fixed gas
exchange rate). Alongside is also plotted the result
from the model of Davidson et al. (1977). Each of the
curves in Fig. 5 shows the obvious increase in conver-
sion at higher reaction rates while higher coalescence
rates show diminished conversion as a result of by-

w = 291.3 . Bottom region

k’ - 5.0 0 Middle region
D - 0.02232 in2 /s 0 Top region

0 I I I I
1.0 5.0 9.0 l3..0 17.0 21.0

T)

Fig. 4. Cumulativefraction of bubbles withindifferentvolume ranges at the lowest coalescence rate in the
bottom, middle and top regions of the bed.
 e
Population balance modelling of bubbling fluid&d bed reactors-1 349
I .o

A w = 291.3

0 w = 1200.4 o Z - 2.26 x lO-4

0.6 . w -2913.0
q Z-3.16 xIO-~
C’ 0 Predicted by Davidson el (II.
(1977) C’
0.4 for well-stirred dense phases
06

I I I I 1
8.0 16.0 24.0 32.0 400
k’
k’
Fig. 5. Unreacted gas fraction vs dimensionless first-order
reaction rate constant for three coalescence rates and Fig. 6. Unreacted gas fraction vs dimensionless first-order
D = 0.02232 in. s-‘. reaction rate constant at w = 2913.0 with varying transport.

passing of the reactant with bubbles with inadequate
exchange between the dense phase and the bubbles. As
the coalescence rate drops the conversion curve ap-
proaches that of Davidson et al. (1977), a result that
was established also analytically earlier in the paper.
Figure 6 shows the effect of exchange rate as
measured by 2 on the conversion. Lower exchange
rates reduce conversion significantly because the by-
passed reactant transfers less efficiently to the dense
phase to which the reaction is confined. The higher
exchange rates produce conversion curves which ap-
preach that of Davidson et al. (1977) in the infinite
limit. Table 4 gives the numerical results of the
computations represented in Figs 5 and 6. In par-
ticular, fluctuations in conversion were found to be
negligible even at the highest coalescence rate used.
Figure 7 is a graph of the cumulative number
fraction of bubbles vs the dimensionless concentration,
5, for the top, middle and bottom regions of the bed.
Bubbles near the grid plate have concentrations dis-
tributed almost evenly from 65 to 100% of the feed
concentration. However, by the time bubbles reach the

TabIe 4. Results of the well-stirred dense phase model

w Z k C’ 5, hi C’ (Davidson) SD C’ x lo3

291.3 2.26 x 1O-4 1.0 0.511 0.494 0.525 0.500 1.70

2.0 0.351 0.328 0.370 0.333 2.01
5.0 0.191 0.162 0.214 0.167 2.15
11.0 0.113 0.083 0.138 0.084 2.14
19.0 0.080 0.049 0.107 0.050 2.13
30.0 0.064 0.03 1 0.090 0.032 2.13

1200.4 2.26 x 1O-4 1.0 0.525 0.480 0.567 0.500 1.52

2.0 0.375 0.318 0.429 0.333 1.37
5.0 0.228 0.156 0.294 0.167 0.81
11.0 0.158 0.079 0.232 0.084 0.40
19.0 0.128 0.047 0.204 0.050 0.29
30.0 0.113 0.030 0.190 0.032 0.30

2913.0 2.26 x lO-4 1.0 0.527 0.473 0.581 0.500 1.64

2.0 0.380 0.311 0.449 0.333 1.55
5.0 0.238 0.152 0.321 0.167 1.30
11.0 0.170 0.076 0.263 0.084 0.83
19.0 0.143 0.045 0.238 0.050 0.73
30.0 0.128 0.029 0.225 0.032 0.67

2913.0 9.43 x 10-3 1.0 0.562 0.439 0.684 0.502 1.66

2.0 0.438 0.276 0.59 1 0.338 1.45
5.0 0.326 0.135 0.511 0.173 1.02
11.0 0.273 0.066 0.470 0.093 0.80
19.0 0.252 0.039 0.453 0.059 0.74
30.0 0.241 0.025 0.449 0.041 0.72

2913.0 3.16 x 1O-6 1.0 0.514 0.49 1 0.532 0.500 1.49

2.0 0.353 0.325 0.380 0.333 1.48
5.0 0.197 0.162 0.232 0.167 1.10
11.0 0.119 0.079 0.159 0.083 0.75
19.0 0.088 0.048 0.128 0.050 0.59
30.0 0.072 0.031 0.114 0.032 0.51
350 IAN R. SWEET er al.
Fig. 7. Cumulative fraction of bubbles within different concentration ranges in the top, middle and bottom
regions of the bed: well-stirred dense phase model.
middle of the bed a vast majority have concentrations
less than 30% of the feed concentration. As might be
expected, at high transport rates and low coalescence
rates bubble phase concentrations tend to decrease.
6. CONCLUSiONS
We have been able to incorporate the population
balance framework to account for the effect of by-
passing of reactant with bubbles which coalesce ran-
domly and individually exchange gas with the dense
phase on the reaction conversion. The conversions
predicted can vary substantially from those of
Davidson et al. (1977) depending upon the values of
the coalescence rate and the exchange rate parameters.
The fluctuations in conversion were negligible for the
most part, at least in the range of parameter values
included in this work. The superficial velocities used in
this work were relatively low, being twice the minimum
fluidization velocity. It is likely that for higher fluidiz-
ation velocities the volume fraction of reactants in the
bubble phase may be substantial enough to lead to
fluctuations in the conversion. Such computations
were not pursued in this work because of limited
availability of data to serve as a guide. It is essential
that efforts be made to determine coalescence rates
before a sound quantitative understanding of fluidized
bed reactors can emerge.
We have emphasized that one of the objectives of
this work is to show that the facility now exists to
analyze rather complex features of fluidized bed
reactors and their effects on conversion. The demon-
stration was confined to a first-order isothermal reac-
tion and in the absence of bubble break-up. It is
possible to incorporate bubble break-up into the
analysis without any special strain on the computation
provided, however, quantitative information is
available. Non-isothermal reactions and complicated
kinetics introduce no conceptual problems although
the computational burden is increased enormously.
Acknowledgements-The authorsgratefullyacknowledgethe
National Science Foundation for an InternationalGrant
INT-8206424 which made this researchpossible. One of us
(D. Ramkrishna)is also grateful to the Indian Instituteof
Science, Bangalore where part of this research was ac-
complished for a Visiting Professorship sponsored by the
University Grants Commission of India.
NOTATION
a interfacial area of bubble
C concentration of reactant in bubble
C’ dimensionless exit concentration of reactant
in the efhuent gas phase
=H exit concentration of reactant in the gas
phase
‘hi average reactant concentration in the bubble
phase at reactor exit
CO reactant concentration in feed gas
CP reactant concentration in well-mixed dense
phase
c rate of change of reactant concentration in
bubble
H height of fluid bed
Hmf height of bed at incipient fluidization
k rate constant of reaction
k dimensionless reaction rate
k2 constant in coalescence frequency governing
coalescence rate
k, shape factor for non-spherical bubbles
KG mass transfer coefficient for bubble for ex-
change of reactant with dense phase
fl average number density function (product
density of order 1); average number of pairs
of bubbles (product density of order 2)
NO number of bubbles per unit volume in feed
Pa pressure at bed top
4 gas exchange rate between bubble and dense
phase
Q coalescence frequency
S cross-sectional area of fluidized bed
U bubble velocity
u superficial velocity of fluidization
u mf superfTcia1velocity at incipient fluidization
0 bubble volume
 Population balance modelling of bubbling fluid&d
v.max maximum bubble volume
V rate of change of bubble volume
X dimensionless parameter defined below eq.
(19)
Z height measured from grid plate
Z dimensionless parameter defined below eq.
(20)
Greek letters
B dimensionless parameter defined below eq.
(18)
6 Dirac a-function
41 dimensionless number density function
PP
dimensionless coalescence rate parameter
w dimensionless exchange rate for bubble
K dimensionless exchange rate for bubble
r dimensionless concentration of reactant in
bubble
5,
dimensionless dense phase concentration of
reactant
dimesionless version of c
4
dimensionless bubble volume
T dimensionless bubble velocity
r dimensionless height of bubble location
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