ChenucalEngmeermgSclence, 1969,Vol 24,pp 1351-1369 Pergamon Press Prmted m Great Bntam

Bubble assemblage model for fluidized bed catalytic reactors

K KATO and C Y WEN
Department of Chemical Engmeenng, West Vlrgma Umverslty, Morgantown, W V 26505, U S A

(Fwst recewed 20 September 1968, m rewedform 30 December 1968)

Abstract-A new model for catalytic reactlon m flmdlzed beds IS developed Ths model called the
Bubble Assemblage Model IS based on multiple bubbles of varymg sizes with Interchange of gas
takmg place between the bubble phase and the emulsion phase
Smce the model needs no adJustable parameters, It IS beheved that the model IS useful for study m
scale-ups The model proposed 1s also convement for computer slmulatlons Expenmental data from
various mvestlgators were used to test the vah&ty of this model It was found that the conversions
predlcted using this model agree reasonably well with the actual performance of the flm&zed beds

INTRODUCTION Based on the results of these observattons,

EVER SINCE the flurdtzed bed techmque was first
apphed to the makmg of syntheses gas from coal
by the Wmkler generator and to the catalyttc
cracking of petroleum, flmdized beds have been
used for a number of other chenucal processes,
particularly m catalyttc synthesis
Some of the flutdtzed bed catalytic processes
are the catalytic reforming of naphthas, the
phthahc anhydnde production, the catalytic
oxtdatton of ethylene, the productton of alkyl
chlorides, the synthesis of acetomtnle from
acetylene and ammonia, etC Just to mentiOII a
few
However, owing to the complex gas flow and
sohd particle movement within the fluidized bed,
design procedure of catalytic fluidtzed bed reac-
tors has not been well established m spite of the
fact that a number of models for flmdized bed
reactors have been suggested
There have been a number of mvesttgations
on the gas flow behavior m a flmdized bed.
InJectmg a tracer gas mto the bed and exammmg
the behavior of the tracer gas by high speed
photography, comparmg the reactant conversion
m both the fluidtzed bed and the fixed bed under
the same operatmg conditions for well defined
catalytic reactions, and observing bubbles nsmg
m the bed have been some of the techniques
employed to determme the gas flow behavior
1351
Kum~ and Levensptel[22,23] recently proposed
a gas flow model which they called the Bubbling
Bed Model for explanation and predtctlon of
flmdtzed bed behaviors asserting that only the
effective size of bubble 1s needed to supply
adequate descnptlon of the flow of gas through
the bed
Although the concept developed certainly
contnbuted consrderably to the understandmg
of flutdized bed behavior, to use an effective
bubble diameter to represent an assemblage of
bubbles of varying sizes seems to be somewhat
an oversimplification
In this paper we shall present a new model
the Bubble Assemblage Model based on
multiple bubbles of varying sizes for design and
scale-up purposes The Bubble Assemblage
Model contains essentially no adJustable para-
meter and is convenient for computer simulations
The experimental data available m hterature
on first order catalytic reaction systems m
flutdized beds are used to test the vahdity of the
proposed model Unless specified, the equations
appearing m this paper are all based on C.G S.
units
PREVIOUS INVESTIGATIONS
An attempt to find the gas flow behavior m a
flmdized bed usmg tracer technique was first

CES Vol 24 8-K

 K KATO and C Y WEN

made by Gdhland and Mason[9] who measured change coefficient between the two phases Table
the concentratton variation of a tracer gas 1 summartzes the results of mvesttgatron usmg
InJected mto a flurdrzed bed. A model, usually the tracer technique Since the parameters
the drspersron model or the two phase model, determmed by this manner are m a sense adjust-
IS presupposed m the analysrs and the flow able, unless the model selected can descnbe
behavror 1s represented m terms of model para- flow behavior reasonably accurately, the
meters such as drspersron coefficient or mter- mformatron obtained IS of httle use for scale-up

Table 1 Expenmental mvestlgatlon of model parameters (A) Tracer method

Authors Model Expenmental con&tlons Expenmental results

Gdhland Dlsperslon model Steady state method

and Mason[9] gas an
tracer He E, IS affeCted by u,,,,
particle F C C , glass
DR=25- 114cm E, = 1Oe- 101(cm*/sec)

Much1 et al [33] Dispersion model Steady state method EJv = 100{N,,/l -E}O~
gas mr
tracer NH, at 15 < N&l-e < 50
particle sand, glass EJv = 18O{N,,/l -e}oa
DR=5- 15cm at50< NRep/l-~ < 200

Winter[44] Dlsperslon model Residence time curve E, = C* d, p exp(-o *dp O/u)

gas air wherew* = 3 5 x 105
tracer He C* = 3 6x 10
particle glass
DR=20- 13 5cm

Kobayashl et al [ 193 Two phase model Residence time curve F0 = 11/D*

D,=O gas air
tracer He
l&=&f parhcle silica gel
DR=84cm

De Grout [6] Two phase model Residence time curve HK=067DRoPSLo5

De=0 gas air where L = bed height (m)
tracer He Hx = u/F,,, u(m/sec)
ll,=l& particle sihca
DR = 10 - 150 cm

lwasakl et al [ 141 Contact time Residence time curve Converslon of reactant m

drstnbutlon gas ar,Hq fluldlzed bed IS expressed by
tracer I-L, M-L GH,
particle silica-alumna x = 1- Po E(4) exp (-@W/F) d~$
DR=508-763cm
contact time distribution E(6)
IS obtained from residence time
curve of adsorbed and non-
adsorbed tracer gas on solid

Kato et al [15] Two phase model Residence time curve F0 = 5 - 3 llsecfor

up = 0 gas air, Hz, N, ulu*=2- 30
tracer H2~CP& CIHl M=O4-02l/secfor
particle slhca-alumina, u/u,~= 2 - 30
glass
DR= lOcm,D,= 1- 3cm

1352
 Bubble assemblage model

purposes. In addition d the model mvolves more
than two parameters, the analysis could become
hopelessly difficult
Another technique useful for the search of
flow behavior m a flurdlzed bed is to compare the
conversion obtamed m a flmdlzed bed reactor
wrth that obtamable m a fixed bed reactor under
the same operating conditions. This technique
Initiated by Shen and Johnstone[37] also needs
a presupposed model for evaluation of model
parameters Experimental data are used to com-
pute either the Interchange coefficrent between
the two phases or the fractron of catalyst present
in the bubble phase. The results of studies using
thrs techmque are summarrzed m Table 2.
Although the parameters obtained by this
technique may satisfactorily represent the
mdivrdual experimental results, it IS doubtful
that these parameters have any physical slgmfi-
cance under other operating conditions for
flmdized beds of complex flow patterns.
So far most of the experimental data on

Table 2 Expenmental mvestlgatlon of model parameters (B) Reactlon method

Parameter Parameter and

Authors assumed Expenmental condltlons expenmental results

Shen and Johnstone [37] a=0 Decomposmon of mtrous oxide Parameter F0

U,=U~ DR= 114cm,L,=26-32cm k=006- 005(l/sec)
D,=Oorm dp = 60 - 200 mesh

Masslmda and Johnstone [29] a=0 OxnUon of NH3 Parameter F0

I(,=linf DR= 114,L,=26- 54cm k = 0 071 (l/set)
D,=O dp = 100 - 325 mesh

Mathls and Watson[30] D,=O Decomposltron of cumene Parameter FO,u

1(,=&f DR=5- 102cm,L,=lO- 31cm k=064(1/sec)
dp = 100 - 200 mesh

Lews et al [26] u, = 0 Hydrogenation of ethylene Parameter FO,a

D,=Oorm DR=5 2cm,Lw= ll- 53cm k= 1 1 - 15 6(l/sec)
d,=OOOl- 0003cm a=005 - 0 18,F=04- 08

Orcutt et al [34] a=0 Decomposltlon of ozone k = 0 1 - 3 0 (l/set)

u, = 0 DR=lO- lScm,L,=30- 6Ocm
d,=OOOl- 0003cm

Gomezplata and Shuster [ 101 a=0 Decomposltlon of cumene Parameter FO,a

ll,=I(mf DR=76Lw=38-20cm k=O75(l/sec)
D,=O dp = 100 - 200 mesh

Kobayashl et al [20] l4,=lI* Decomposltlon of ozone Parameter a

D,=O DR=83cm,Llllr=10- 100cm k=O.l - 0 8(l/sec)
dp = 60 - 80 mesh a = 15 (L/Lw- 1)

Kobayashl et al [21] u,=l& Decomposltlon of ozone Parameter a

D,=O D,=20cm,L&=lO- 1OOcm k = 0 2 - 3 5 (l/se@
dp = 60 - 80 mesh a=Ol-03

Ishu and Osberg[ 131 Dlsperslon Packed fluldlzed bed ISO- k=05- 2 l(l/sec)
model menzatlon of cycle-propane
DR=42- 12cm,L,,,,=15- 50cm
dp=lOO-200mesh,Dp=1-25cm

Kato[l6] IA,=&/ Packed flmdlzed bed hydro- Parameter a

D,=O genatlon of ethylene k=l l-33(1/set)
DR=87cm,Lw=10- 30cm a=035 -045
dp= IOO- 200mesh,Dp= 1- 3cm

1353
 K KATO and C Y WEN

kmettc study m fluidized beds were fitted on theof the two phase model by either assuming or
two phase model. A general expression of the estimatmg some of the terms m Eq. (1) and/or
two phase model can be given as (2) In Table 3 the results of the theoretical
development of the two phase model are sum-
martzed.
As has been observed, numerous studies have
+F&b--cC,)+F,y = 0 (1) tried to explam the flow pattern of gas m fluidlzed
beds, the main dtfficulty seems to revolve about
obtaining a sattsfactory flow model which will
fit the observed conversion in fluuhzed beds
+ FdCe-- cd +.6-Y= 0. (2) under a wide range of cot&tons. Thus a new
flow model taking mto account the presence of
Most of the mvestigators used a simplified form an assemblage of bubbles seems to be needed

Table 3 TheoretIcal study of the two-phase model

Parameter
Authors assumed Method aorF, Remarks

Van Deemter[41] a=0 A steady-state analysis of HA&

k Parameter, F,, IS not
I(
u, = 0 gas back-nuxmg and related to the bubble
D,=D, residence time curve and Hk=OS-25 a=0 movement m the bed
first order reaction by two
phase model

Much1 [32] l&=&f A study of effect of Fo, a, No relation between

O<D,<m D,, u, on conversion of a bubble movement and
first order reaction parameters

Mamuro and &.=uw Analysis of a first order

Much1[28] a=0 reaction based on the two-
phase cell model $I = shape factor of bubble

Van Deemter[42] De=0 Analysis of back nuxmg, F0=04- 12(l/sec) Parameters a, F,,, IA,are
residence time curve of not related to the bubble
tracer gas and the first growth m the bed
order reactlons

Kuml and u, = 0 Analysis of vanous phen- Parameter DB

Levensptel[22] omena m fluldlzed beds by model IS characterized by
the bubbling bed model a single effective size of
the bubble
c,,,,Dub %
F,,=678 -
( DB )

Davldson and D,=Ooro: Estunatlon of conversions F = 5 85D12g4 Parameter DB

Harnson[S] a=0 for a first order reactlon II Dp model does not account
for bubble growth m the
; 45und bed
DS

Kobayashl and u, = 0 A study of the effect of Parameters a, FO.D,

Ara1[17] De=0 k, a, D, and F,, on con- are not related to the
version of a first order bubble movement
reaction

1354
 Bubble assemblage model
BUBBLE ASSEMBLAGE MODEL
In developing a model for the flow of gas
through a fluidized bed based on an assemblage
of bubbles, the followmg simplifying assumptions
are made
(1) A fluidtzed bed may be represented by n
numbers of compartments m senes The hetght
of each compartment IS equal to the size of each
bubble at the correspondmg bed height This
assumption not only makes it possible for the
mtroduction of bubbles of multiple sizes into
the flow model but also makes It convement for
computer calculations
(2) Each compartment is considered to con-
sist of the bubble phase and the emulsion phase
The gas flowing through the bubble phase and
the emulsion phase is considered to be com-
pletely mixed within each phase
(3) The void space withm the emulsion phase
is considered to be equal to that of the bed at
mctpient fluidizmg condttions. The upward
velocity of the gas m the emulston phase IS at
U,
(4) The bubble phase IS assumed to consist of
spherical bubbles surrounded by spherical
clouds. The diameter of the bubbles and that
of cloud are given by Davidson [4] as
Rc 3= ub + k&n.f
(3)
( R1,> ub- kn.fknf
ub 3 hnfknf
Under normal operating comhtions, &, is much
larger than u,&~ In this region cloud forma-
tion around the bubble can be observed How-
ever, when large particles are used for fluidiza-
non, umf is correspondmgly large and therefore,
the bubble velocity can become smaller than
I(,,&~ The calculation presented here based on
the proposed model would not be apphcable to
this range of operation. The voidage withm the
cloud is assumed to be the same as that m the
emulsion phase
(5) The total volume of the gas bubbles wtthm
the bed may be expressed as (L - L,) S
(6) Gas interchange takes place between the
1355
two phases. Overall interchange coefficient per
umt volume of gas bubbles is given by
Fd = F,+KM (4)
(7) The bubbles are considered to grow con-
tmuously while passing through the bed until
they reach the maximum stable size or reach
the diameter of the bed column Harrison et al.
[l l] showed that the maximum stable bubble
diameter is attamed when the upward flowing
velocity becomes the termmal velocity of
particles The maximum stable bubble diameter,
&, can be found from
(5)
(8) Smce the effective thermal ddfusivny and
the heat transfer coefficient [43] m a fluidized
bed have been shown to be very large, the bed
is assumed to be operating under isothermal
condrttons The maJonty of experimental data
reported are also obtained under isothermal
conditions
Bubble me
The studres on bubble growth are numerous,
among them the works of Yasm and Johanson
[45], Toei et a1.[39], Hu-ski, Yoshida and Kunu
[ 121, Kobayasht, Arai and Shiba[ 181 and
Baugarten and Ptgford[2] are noteworthy Their
expenmental data are plotted m Fig. 1, followmg
Kobayashi ef a/.[ 181, m terms of D,/ppdp(u/u,)
and the bed height, h In this figure some addi-
tional data were Incorporated mto the ongmal
plot of Kobayshi et al.[ 181 Although some
scattenng of the data IS seen, the bubble diameter
and the distance from the distributor can be
approximately related by the correlation equa-
tion of Kobayashi et al [ 181 as
h
Exammation of Fig 1 reveals that the bubble
diameter IS not necessarily proportional to the
 K KATO and C Y WEN

CormlotIonequatlon of Kobayoshl et al I

IO2
.
6

22 2 4 6 6 IO 20 40 606OKx) 200

h,cm

Fig 1 Correlation of Bubble diameter along the bed axis for crowd of bubbles

Symbol Authors Matenal d&m)

Hnxkletal[12] F C C catalyst 0 015

Kobayashl et al [ 181 Sihca gel 0 0194
Toe] et al 1391 Glass 0 0137
Yasm and Glass 0 0041 - 0 0267
Johanson [45]
Ohvme 0 0042 - 0 015
Coal 0 0692
Magetlte 0 0072
V 0 P catalyst 0 0078
Tanaka[38] Sihca gel 0 0213
Winter [44] Glass 0 011 - 0 025
Baugarten and Glass 0 0074
Plgford [2]
Romero[35] Glass 0 0071

first power of the bed height. In fact several sets
of the data indicate the power on the bed height
to be somewhat smaller than umty. However,
before more accurate measurement of bubble
diameter with respect to bed height becomes
possible, there 1s at present no Justification of
using more sophlstlcated correlation beyond
that of Kobayashl et al [ 181.
Stnctly speaking, the bubble diameter also
should vary slightly with the bed dla DR under
the same fluldlzatlon condltlons There IS an
1356
expenmental evidence mdlcatmg that the bubble
diameters are shghtly smaller when the bed
diameter becomes larger. However, the relatlon-
ship between the bubble velocity and the bubble
diameter 1s also affected by the change m bed
diameter. In other words, for a larger bed, the
velocity of the bubble having the same diameter
will become shghtly larger due to the reduced
fnctlon along the wall of the bed Just how great
the wall effect on the bubble velocity is not very
clear at present Hence, until additional research
 Bubble assemblage model

is made to provrde more refined relattonshtp
between the bubble veloctty and the bed dta-
meter, Eqs. (6) and (8) are believed to be most
reliable today.
The above correlation IS based on the data
obtained using porous plates as the distributor.
For perforated plates the size of bubbles at the
surface of the dtstnbutor are substantial and
therefore must be taken mto constderatton.
According to Cooke et a/.[31 the bubble srze
at the surface of a perforated plate havmg no
number of holes, can be calculated from (SC/W)4/
g 2 based on the work of Davidson and Harrison
[5] where G = (U-U&/Q,. Therefore, m general,
the diameter of bubbles m a fluidized bed can be
approxtmated by
of Fan, Lee and Baihe[8] m&cate the voidage
up to the bed height corresponding to L, can
be considered approxnnately umform and that
the votdage above L, increases along the bed
height. For an approxrmatlon, rt is assumed that
above the bed height correspondmg to Lw,
(1 -E) decreases linearly wtth respect to the
bed height. It is further assumed that the average
bed height reported m the experiments can be
considered as an arithmetic average of the maxi-
mum bed height correspondmg to E = 1 and Lw.
Following Davidson and Harnson[5], the
velocity of nse of a crowd of bubbles through a
fluidtzed bed can be calculated by
u;, = ~~--/.++0~711(gD~)~. (8)

D, = 14ppdp h+D,, (7) Now, rf the charactenstrc bubble diameter 1s

taken as that correspondmg to the bubble
where situated at L,,,,/2, from Eqs. (7) and (8) and
assumption (5), the bed expansion ratio can be
expressed as

The validity of Eq (7) IS tested usmg the expen- (L-L,)/L,= (u-u~)/{0~711(g~~)~~} (9)
mental data of Cooke et a1.[3] and 1s shown m
Table 4. where & is an average bubble dtameter of the
Equation (7) can be used to compute local bed given by
average bubble diameter along the axis of the
flmdtzed bed. & = 14ppdp - u T+
Lmf DO.
(10)
(k >
Voidage dmtrlbutlon and bubble velocity
In developing the gas flow model, rt is neces- In Fig 2, the bed expansions calculated from
sary to know the votdage distribution within the Eq (9) are compared with the experimental data
flmdlzed bed The study of Bakker[l] and that of Leva et al [25], Lewis, Gilhland and Bauer

Table 4 Companson of expenmental bubble diameter with calculated values usmg Eq (7)

Dsobst DB Cal
Condltlon (cmkec) ulu, h (cm) (cm) (cm)

ud = 5 cm/set 36 72 20 15 16 2
36 72 40 24 27 4
24 48 20 12 5 11 5
pp= 14&c 24 48 40 21 0 19 3
perforated plate 18 36 20 98 91
n, = 0 l/cm* 18 36 40 160 14 8
18 36 60 22 20 4
DR=30cmX12cm 18 36 80 27 26 0

tBased on data from Cooke et al [3]

1357
 K KATO and C Y WEN

Fig 2 Companson of expenmental bed expansion with calculated bed expansion

Symbol Authors Matenal & (cm) D&m)

Leva et al [25] Round sand 0 0063 - 0 0381 6 3.5

Round and 0 00775 6 35 - 10 15
sharp sand
Fisher-Tropsch Cat 0 00705 - 0 0385 10 15
Lewis et al 1271 Glass-beads 0 0102 - 0 056 635- 114
Tanaka[38] Sihca gel 0 021 20 0

[27], and Tanaka[38] As seen from the figure,
the ratios of calculated bed herght to expen-
mental bed he&t are wtthm + 10 per cent of 1 0
mdtcatmg a favorable agreement. Thus, m model
development, Eq (9) may be used to compute
the bed he&t with reasonable accuracy Once
the bed expansion ratio 1s known, the votdage
from the distributor up to a height correspond-
mg to Ld and that from Lti to the top of the bed
can be computed, respectively, as
for large U/U&, U, 1s neghgrbly small This 1s a
reasonable assumptron m vtew of the fact that
the experimental findmgs of May [3 l] and Kunu
and Levensptel[22] mdtcate the emulston gas
may reverse its dtrectton m vtgorously bubbhng
beds According to Kunn and Levensptel[22],
the velocity of gas flowmg m the emulsion phase
m the axial direction can be expressed as

I--E=+(l-eti) for h< Lti (11)

and
where (Y 1s the ratio of the volume of emulsion
transported upward behind a bubble (1 e volume
of wake) to the volume of a bubble. The value of
, (Y is approx 0.2 - O-3 according to the expen-
for mental study of Rowe and Partndge[36] There-
Lmfs h =s L,+2(L-LL,) fore, under normal expenmental condrtrons, Eq
(13) yields u,/umf = 0 5 for u/uW = 3, and u,/
Gas velocity m emulsion phase umf = 0 for U/Q= 5 - 6 Latham, Hamilton
Since the knowledge of the upward velocrty and Potter[24] also studied using a tracer gas to
of the gas flowmg in the emulsion phase, u,, IS locate the velocity at which the emulsion gas
still a controversial subJect, we shall assume that will reverse its dlrectton (u, = 0) and found that
1358
 Bubble assemblage model

u, = 0 when u/uW= 2.7 - 6-O. Based on the CALCULATION PROCEDURE BASED ON

above expenmental findings and the argument BUBBLE ASSEMBLAGE MODEL

presented by Levensplel and Kunn[23], it Let the height of n-th compartment be Ah,,
would be reasonable to assume u, = 0 under where n = 1, 2, 3,. Based on an anthmetlc
most of the normal operating condltlons average of bubble size, the height of mltlal com-
partment immediately above the dlstnbutor
Interchange coeficlent becomes
The gas interchange between the bubble phase
and emulsion phase mvolves direct interchange Ah 1
= Do+(*hl+DO) or

of gas m bubbles and m emulsion, and mdu-ect 2

interchange due to adsorbed gas on the surface
of mterchangmg particles Since no expen-
mental data are available for the particle mter- where I?Z= 1 4pPdP (u/u~) , a proportlonahty
change rate, M, and adsorption equlhbrmm constant relating the bubble diameter for a given
constant, K, for the reacting gas on particle operating con&tlon The height of the second
surfaces, the analysis presented here will neglect compartment then becomes,
gas interchange due to adsorbed gas on mter-
changing particles. Therefore, Eq (4) 1s reduced
to Fd = F0 As to the direct gas interchange,
semi-theoretical studies by Zenz [46], Davidson
and Harnson[S] and Kuml and Levensplel[22] and that of n-th compartment becomes,
as well as an analysis based on the stlmulus-
response curve from tracer data using the two
Ah, = 2Do (;;f-$; (15)
phase model by Kobayashl, Aral and Sunagawa
[19] are available Most of these studies agree
on one point that the interchange coefficient, The number of bubbles m the n-th compartment
FO, IS approximately inversely proportional to becomes,
the bubble diameter Therefore, the followmg
equation based on the expenmental work of
(16)
Kobayashl et al [ 191 will be used

F,, = 11/I&. (14) The volume of cloud m the n-th compartment can
be computed from Eq (3) as,
In a recent study, Toe1 et al [40] injected a
single CO, bubble mto a fluldlzed bed and V = Nr(AU3
measured the vanatlon of CO, concentration cn 6 (17)
within the bubble They calculated the gas mter-
change coefficient based on these measurements where,
and found that F,, which IS somewhat affected &, = 0*711(gAh,)2.
by the particle diameter, can be approximated
by 310~ - 6/DB Since their study pet-tams to The total volume of the bubble phase and that of
a single bubble, the effects of bubble colhslons the emulsion phase m the n-th compartment are,
and coalescence are not taken into conslderatlon respectively,
It IS therefore not unreasonable to assume that
m a vigorously fluldlzmg bed, the interchange v = N~@hd3 ub+2hfhf
bn 6 (18)
ub - kfknf >
coefficient IS more closely represented by Eq
(14) v,,, = SAh, - v,, (19)
1359

The drstance from the distributor
compartment is
h, = 2 Ahf
f=l
The gas interchange coefficient based on unit
volume of bubbles from Eq. (3) can be shown as
tub - &&mf)
= Fan (&, + 2&&Q)
Hence, the matenal balance for the gaseous
reactant around the n-th compartment becomes,
for the bubble phase,
(sucb)n-I = {F;,vb(cb - c,> )n
+ (rbvc)n+
and for the emulsion phase,
{F:,Vb(Cb- C,)), = (rev,),,
where rb and r, are the reaction rates per unit
volume for the bubble phase and emulston phase
respectively For example, tf the rate of reaction
1s a first order with respect to reactant gas, they
become; rb = kc,, and r, = kc,
The computattonal procedure for converston
and concentration profile m a flutdtzed reactor
is gtven below when the operatmg conditions
such as particle size, d,, parttcle denstty, pP,
mtmmum flutdtzatlon veloctty, umf, gas velaclty,
u, dtstnbutor arrangement, column diameter,
DR, mctptent bed height, LW, the reaction rate
constant, k, and order of reactton are known.
Note that this model requues no adjustable
parameter
First, Eqs. (8) and (9) are used to calculate
the expanded bed height, L Next, Eq (15) 1s
used to compute the size of the n-th com-
partment. Using Eqs. (17-19), the volume of
cloud, that of the bubble phase, and the emulsion
phase for the n-th compartment are then calcu-
lated Cbn and C,, are computed from (Cb),_,
and (C,)._l usmg Eqs (22) and (23) The cal-
culations are repeated from the dlstnbutor unttl
the bed height equivalent to Lw IS reached For
K KATO and C Y WEN
to the n-th bed height above Lw, the voulage IS adjusted by
Eq. ( 12) and Vm, vb, and V,, are obtamed using
the same procedure as that shown for the height
(20)
smaller than Lw The calculatton 1s repeated
until the bed height reaches L,+ 2(L- L,,J. A
computer logtc dtagram based on thrs procedure
1s shown m Table 5.
RESULTS OF CALCULATIONS
(21)
* Smce most of the experimental data were
obtained using porous plates, the bubble size
at the surface is very dtfficult to estimate There-
fore, the height of mmal compartment, Ah1, 1s
assumed. It becomes necessary to test the effect
of size of Ah, on the conversion m order to show
the soundness of this assumption. For a com-
(such), (22) paratively small flurdtzed bed reactor, say
column dia. of 5 cm - 20 cm and bed height of
less than 100 cm, we should expect the sizes of
bubbles formmg on the surface of a porous plate
(23) to be quite small. It 1s therefore logical to assume
that the height of the first compartment would
be no more than a few centtmeters. In Fig. 3, the
effect of Ah, on conversion 1s exammed for
cases where reaction rate is comparatively fast
(1 e for large k). It 1s quote obvious that for slow
reactions, the size of compartment 1s of httle
significance on overall converston and 1s there-
fore not examined. As can be seen from the
figure, the mmal height of the compartment,
Ah,, does not affect greatly on overall conversion
even for fast reactions In actual calculation
therefore, Ah, = 1 0 cm 1s used
For a large fluubzed bed reactor which has a
perforated plate distributor, Eq (15) together
with mformatton on the number and the size of
holes must be used to calculate the he&t of
initial compartment
In order to demonstrate the vahdtty of the
proposed model, conversions m flutdtzed beds
based on the kmettc mformatlon given m Table 2
are calculated. The results of calculatton are then
compared with actual expenmental converstons
In Figs. 4-6 the extent of conversion along the
bed height are shown for three sets of data; those
of Lewis, Gllhland and Glass[26] for compara-
tively large reaction rates, those of Kobayashl
1360
 Bubble assemblage model

Table 5 Logic diagram for computer slmulahon

Read dP.pP, u+ DR.

Start r k,Co.u.L,,,,
Calc L from Eq (9)

No

No

& End

and Arai [20] for intermediate reactton rates and
those of Massmnlla and Johnstone[29] for small
reactron rates, respectrvely.
As can be seen from these figures, when the
rate of reactron 1s small, the concentratton of gas
m the emulston phase 1s not too much different
from that in the bubble phase However, when
the rate of reactron IS large, the difference m
concentratrons between the two phases become
very stgmficant For a fast reaction, a great deal
of gaseous reactant m the emulston phase 1s
seen to be converted m the rmmedrate vrcmtty
of the drstnbutor These observations imply
that for fast reacttons the gas interchange between
1361
the two phases IS of prtmary importance whereas
for slow reactions the gas interchange between
the two phases does not affect stgntficantly on
the converston.
To examme the gas velocity effect, a compar-
lson of the conversron predrcted by the model
and that from actual expenments IS shown m
Fig. 7. In Fig 8, the calculated conversion IS
compared with the expenmental converston
based on nearly all the data presented in the
studres listed m Table 2 Consrdenng the dlf-
ticultres m obtarmng accurate kinetic mformatton
from tied bed expenmentatlon and the posstble
vanatron of catalyst acttvtttes dunng the flutdrzed
 K KATO and C Y WEN

IO-
6 15 bed operation, the agreement must be regarded
-I2 6 to be quite remarkable.
194
06 -256
470 DISCUSSION
06
D,=52an The computation using the Bubble Assem-
x Ld24cm blage Model Indicates that for most of the
k-87 I/bet expenmental condmons tested, the number of
04 hf= 0 73cmAec
Parameter *U/Q compartments are usually greater than ten. This
means, m terms of the flow pattern, the gas
passing through the bubble phase IS close to
plug flow This IS probably a reasonable con-
I I I I I I clusion. The flow pattern of gas m the emulsion
IO 14 18 22 26 30
phase may be also regarded to be close to plug
Ah,, cm flow although m the actual computatton, because
u, = 0 IS used, tt turns out to be a dead space
mterchangmg gas with the bubble phase This
may invite an argument since some investigators
regard the flow m this phase to be close to com-
06
plete nuxmg However, as Lewis et al [26] and
x
73 Muclu[32] pointed out that under normal
operattons, the calculation of converston m a
flutdtzed bed reactor based on the two phase
model IS not affected stgmficantly by the flow
patterns m the emulston phase, whether tt IS
assumed to be plug flow or completely mixed.
The important aspect of a flow model for a flutd-
IO 14 I8 22 26 30 tzed bed IS to correctly account for the bubbhng
Ah, ,cm phenomena and assoctatmg gas interchange
Fig 3 Effect of AhI on the converslon between the two phases. Using probes, Tanaka

- Bubble phase
-- - - - Emulrlon phase
Parameter = u/u,, (6-j

Fig 4 Relation between the concentration profile and bed height

when the reaction rate constant 1s large Lews et al [26] (DR =
52cm,L,=242cm,k=87sec-)

1362
 Bubble assemblage model

-Bubble phosr
-- - - - - Emulrlon phaw
Pornmeter =u/u,

Fig 5 Relation between the concentration profile and bed height

for an mte.rme&ate rate constant Kobayasb et al [21] (& =
20 cm, LW = 67 cm, k = 0 7 se0

----c-Em&ion phone

QL,
Rg 6 Relation between the concentration profile and bed hetght
when the reaction rate constant IS small Massmulla et al [29]
(& = 11 4 cm, 15~ = 54 3 cm, k = 0 0707 l/set)

[38], recently measured the concentration pro- tlons predxted by the model usmg the followmg
file along axial dlrectlon in a 20 cm dla column relation.
for the decomposlhon of ozone Since the con-
&L--L,
centration obtained by the probe IS an average C*++ for h s L, (24)
between the emulsron phase and the bubble LLf
phase, It may be compared with the concentra- Frgure 9 shows this companson. The agreement
1363
 K KATO and C Y WEN

^^I0 2 4

k L&l
6 6 IO 20 40 60

Fig 7 Companson of expenmental conversion with calculated

results 0 - Lewrs et al [26] k = 8 7 l/set, Lw = 24 2 cm, DR = 5 2
cm, 0 - Kobayashl et al [2 l] k = 0 7 llsec, Lti = 67 cm, DR = 20 0
cm, A - Massrmdla and Johnstone[29] k = 0 0707 llsec, Lti = 54 3
cm,D,= 114cm

agam seems to be remarkable. Notice that the
reaction progresses very rapidly just above the
distributor. The profile calculated from a model
characterized by a smgle effective bubble size
IS unlikely to exhibit such a trend
The foundation of the proposed Bubble
Assemblage Model lies on the knowledge of
variation m bubble diameters along the bed
axis Hence more accurate measurement of
bubble growth is necessary to ascertain the
bubble diameter correlation presented here
In addition the knowledge of gas interchange
between the two phases is also a very important
factor particularly for fast reactions and there-
fore should be further mvestlgated The charac-
teristics of the proposed model is its versatlhty
and adaptability for varying situations. This
is believed to be due to the fact that the model
is developed based on an assemblage of multiple
bubbles which grow as they nse through the
bed The scale-up constderation is now possible
with fair amount of confidence m the accuracy
of the results The model is also convenient for
1364
computer stmulatlon and can handle rather
easily even cases involving complex reaction
rate expressions One of the weaknesses of this
model as m any other model is the uncertainty
of knowledge of gas velocity m the emulsion
phase, u, It can be shown that the conversion
calculated based on this model is rather m-
sensitive to the value of u,, nevertheless, further
mvestlgatton on this subject is needed The
model can be extended to include solid parttcle
mixing pattern which may be used to develop
a flmdtzed bed reactor model for a non-catalytic
solid-gas reacting system. This ~111be presented
m another paper
CONCLUSION
The catalytic conversion measured by expen-
ments of others can be predicted by the Bubble
Assemblage Model in terms of the reported
kinetic constants and the operating condl-
ttons The model needs no adJustable parameters
and 1s useful for design and scale-up of the
flutdized bed reactor The correct grasp of the
 IO-

08-

06-

OS-
x_

04-

;E , , , ,,,,,
01 02 03 04 0506 08 IO

Experlmtntol conversion, x
Fig 8 Companson of expenmental converslon with calculated converslon
3
Symbol Author d&m) PPkfW D&m) L&m) k( llsec) 8

Lewis et al [26] 0 0122 0 93 52 24 - 46 14-87

: Kobayashl et al [20] 0 0194 1 25 83 19- loo 08-02
A Massmulla and 0 0105 206 114 18 1 - 54 0 0707
Johnstone [29]
0 Shen and 000806 1 91 11 4 27 - 54 0 022 - 0 0068
Johnstone[37]
0 Kobayashl et al [21] 0 0194 1 25 20 0 34 - 67 02- 14
v Ofcutt et al [34] 00038- 00042 1 14 15 25 - 10 15 61 - 29 4 02-30
A Mathls and 0 0103 12 8 07 10 - 50 0 65
Watson[30]
0 Echlgoya et al [7] 0 0122 1 15 53 5- 17 40-8
n Gomezplata and 0 0105 0 98 76 4 - 20 0 775
Shuster[lO]
V Ishu and Osberg[l3] 0 0088 1 65 15 2 45-26 031- 15

-
 K KATO and C Y WEN

I%- 1,,=345cm
=237 Vsec
/q&l 9

00 I I I L I
00 02 04 06 06 IO

Fig 9 Companson of expenmental concentration profile with calculated

values - Bubble phase concentration, ----- Average concentration
based on Eq (24), ------Emulsion phase concentration, 0 Expenmental
daia[38]

bubbling phenomena together with the knowl- concentration of reactant in emulsion

edge of bed expanston, votdage dtstnbutton, phase, g-mol /cc
gas interchange between bubbles and the concentratron of reactant m bubble phase
emulston phase, are the key to the success of at n-th compartment g-mol./cc
the development of this model It IS hoped that concentration of reactant in emulsion
models devoloped will promote further mvestt- phase at n-th compartment, g-mol./cc
gattons so that a more accurate and versattle average concentratron of reactant defined
model can be developed in Eq (23), g-mol./cc
Acknowledgments-The authors express then gratitude to
D dtffustvtty of reactant gas, cm2/sec
the Office of Coal Research, Department of the Intenor, & bubble diameter at surface of dtstrtbutor,
Washmgton, DC for financial support The authors also cm
wish to acknowledge the help of L Y WeI on the computer
calculations Db axial dispersion coefficient of reactant m
bubble phase, cm2/sec
NOTATION D, axial dispersion coefficient of reactant m
a fraction of flutdtzed parttcles m bubble emulsion phase, cm2/sec
phase DIJ effective bubble diameter, cm
C concentration of reactant, g-mol./cc DP packing diameter m packed flutdtzed bed,
cb concentratron of reactant m bubble phase, cm
g-mol./cc DR bed diameter, cm
1366
 Bubble assemblage model

DS axial solid drspersron coefficrent in emul- N number of bubbles m n-th compartment

sion phase, cm%ec NRCP particle Reynolds number
DT maximum stable bubble diameter, cm n0 number of holes per unit surface area of
4 fluidized particle diameter, cm drstributor, l/cm2
ES axial gas drspersron coefficient m the bed, RC radms of cloud, cm
cm2/sec & radms of bubble, cm
F volumetnc fractron of gas in the bubble r reaction rate per unit volume of catalyst,
phase g-molelsec cc
Fd overall gas interchange coefficient per rb reaction rate m bubble phase per umt
unit volume of gas bubble, llsec volume of cloud, g-mole/set cc
FO gas interchange coefficient per unit re reactron rate m emulsion phase per umt
volume of gas bubble, l/set volume of cloud, g-molelsec cc
F on gas Interchange coefficient at the n-th s cross sectional area of the bed, cm2
compartment, l/set t time, set
Fon gas interchange coefficient at the n-th u superficial gas velocny, cm/set
compartment based on the unit volume ub bubble nsmg velocrty, cm/set
of bubbles, llsec 4 bubble nsing velocrty based on fixed axls,
F8 volumetric fractron of sohd m bubble cmlsec
phase, llsec super&la1 gas velocrty at muumum flmd-
f volumetric fraction of gas in emulsron izatron velocity, cm/set
phase, llsec UC? superfictal gas velocity m the emulsion
f, volumetnc fraction of solids m emulsion phase, cmAec
phase, l/set uT termmal velocrty of flurdlzed partrcles,
g gravitational acceleration, cm/sec2 cmlsec
h distance from the dlstnbutor, cm Vbn volume of the bubble phase at the n-th
Ah length of the n-th compartment, cm compartment, cc
h, drstance between the distributor and n-th VC, volume of the cloud at the n-th compart-
compartment, cm ment, cc
K absorption equrhbrmm constant V en volume of the emulsron phase at the n-th
k reaction rate constant, l/set compartment, cc
L bed height, cm X conversion of the reactant gas
Lti bed height at nnmmum flurdlzed velocity, i-x ratio of the volume of wake to volume of
cm bubble
L Cal bed height calculated from Eq (9), cm E void fraction
Lob observed bed height m the flutdrzed bed, EP vord fraction of fixed packing
cm %f void fraction at umf
M solid interchange coefficient between the ZJ kmematrc vrscoslty
bubble phase and the emulsron phase PP particle density, cm2/sec
per umt volume of bubble, l/set

REFERENCES
[l] BAKKER P J , Chem Engng Scr 1960 12 260
[2] BAUGARTEN P K. and PIGFORD R L ,A I Ch E .I1 19606 115
131 COOKE M J , HARRIS W , HIGHLEY J and WILLIAMS D F , TrrpartrteChem Engng Conf, Symp on Flurdts-
atzon I. pp 14-20, Montreal 1968
[4] DAVIDSON J F , Trans Instn them Engrs 196139 230
[5] DAVIDSON J F and HARRISON D , Flurdrzed Part&es Cambndge Umverslty Press 1967
[6] DEGROOTJ H ,Proc lnt Symp on Flurdzzatron,pp 348-361 1967
[73 ECHIGOYA E , IWASAKI M , KANETOMO T and NIYAMA H , Chem Engng, Tokyo 196832 571

1367

CES Vol 24 8-L

 K KATO and C Y WEN

;z; FAN L T , LEE C J and BAILIER C ,A I Ch E Jll962 8 239

GILLILAND E R and MASON E A , Ind Engng Chem 1949 416,119l
HOI GOMEZPLATA A and SHUSTER W W ,A I Ch E Jll960 6 454
1111 HARRISON D , DAVIDSON J F and KOCK J W , Tram Znstn them Enars 196139 202
WI HIRAKI I , YOSHIDA K and KUNII D , Chem Engng, Tokyo 1965 29 11, ii46
1131 ISHII T and OSBERG G L .A I CH E Jll965 11279
[I41 IWASAKI M , FURUOYA I , SUEYOSHI H , SHIRASAKI T and ECHIGOYA E , Chem Engng, Tokyo 1965
29 892
WI KATO K ,IMAFUKU K and KUBOTA H , Chem Engng, Tokyo 196731 10,967
[161 KATO K , Ph D Thesis, Tokyo Institute of Technology 1967
u71 KOBAYASHI H and ARAI F , Chem Engng, Tokyo 1965 29 885
[181 KOBAYASHI H , ARAI F and SHIBAT , Chem Engng, Tokyo 1965 29 858.
u91 KOBAYASHI H , ARAI F and SUNAGAWA T , Chem Engng, Tokyo 1967 31239
WI KOBAYASHI H , ARAI F , ISAWA S , SUNAGAWA T and MIYA K , Chem Engng, Tokyo 196630 656
@II KOBAYASHI H , ARAI F , TANAKA T , SAKAGUCHI Y , SAGAWA N , SUNAGAWA T , SHIBA T and
TAKAHASHI K ,6th Reactron Engng Symp p 13 1966
WI KUNII D and LEVENSPIEL 0 , Znd Engng Chem Fundls 1968 7 3,446
WI KUNII D and LEVENSPIEL 0 , Flurdlzatlon Engrneenng Wdey 1969
t241 LATHAM R , HAMILTON C andPOTTER 0 E , Br them Engng 1968 13 666
WI LEVA M , WEINTRAUB M , GRUMMER M , POLLCHIK M and STORCH H H , Bull US Bur Mmes No 504
1949
LX1 LEWIS W K , GILLILAND E R and GLASS W ,A I Ch E Jll959 5 419
P71 LEWIS W K ,GILLILANDE K andBAUERW C .Znd EnanaChem 194941 1104
MAMURO T. and MUCH1 I , J md Chem 1965 68 126 - -
E MASSIMILLA L and JOHNSTONE H F , Chem Engng Scr 196116 105
r301 MATHISJ F andWATSONC C,A Z Ch E J119562518
1311 MAY W G , Chem Engng Prog 1959 55 49
MUCH1 I , Mem Fat Engng Nagoya Umv 1965 17 1,79
,::z MUCH1 I , MAMURO T and SASAKI K , Chem Engng, Tokyo 196125 747
ORCUTTJ C , DAVIDSON J E and PIGFORD R L , Chem Engng Prog Symp Ser 1962 58 38,1
gz; ROMERO J B ,A I Ch E Jll965 11595
[W ROWE P N and PARTRIDGE B A, Truns Znstn them Engrs 1965 43 T157
[371 SHEN C Y andJOHNSTONE H F ,A Z Ch E Jll955 1349
[38] TANAKA T , M S Thesis, Hokkado Umverslty 1967
[39] TOE1 R , MATSUNO R , KOJIMA H , NAGAI Y and NAKAGAWA K ,Chem Engng, Tokyo 1965 29 851
[40] TOE1 R , MATSUNO R , MIYAKAWA H , NISHIYA K and KOMAGAWA Y , Chem Engng, Tokyo 1968 32 565
[41] VAN DEEMTER J J , Chem Engng Scr ,196113 143
[42] VAN DEEMTER J J , Proc Znt Symp on Flwdrzatron, p 334 1967 Eldenhoven, Netherland
[43] WEN C Y and CHANG T M Proc Znt Symp on Fludrzatlon, p 491 1967 Eldenhoven, Netherland
[44] WINTER 0 H , Paper presented at Symposium on fundamental and apphed flus&zation I, Fifty-Eighth NatIonal
Meetmg, Dallas, Texas, Feb 6 ( 1966)
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APPENDIX
In the above &scusslon, the height of each compartment
was selected based on the average diameter of bubbles at where
a gven bed he&t Since a portion of the cloud associated
with the bubble was excluded, the volume of cloud must be and &, = 0 711 (gD,,)
adjusted to include the small segments of cloud situated at
the top and the bottom of the bubbles mto that compartment The number of bubbles m the n-th compartment becomes
Because the choice of the size of compartment 1s rather
arbitrary, it makes httle ddference whether one bubble &a- N_6S(L
meter, or one cloud diameter 1s used as a umt height of the sLDj,
compartment Selection of the compartment height based on
the bubble diameter excludmg the cloud gave a neat expres- The volume of cloud, and the volume of the bubble phase are
sion of the height of n-th compartmept as shown by Eq (15) gven by Eqs (17) and (18), respectively, except that Ah,
On the other hand, If the unit height 1s based on the diameter appeanng m these expressions are replaced by Dgn The
of the cloud, the height of the n-th compartment becomes converslons calculated based on the he& on bubble and
those based on the height of cloud are practically the same
Ub + 2&J&f 13 (The maximum tierence 1s 1 5 per cent for all the expen-
Ah. = De,
Ubn - %k,,, > mental data tested )

1368
 Bubble assemblage model

R&um& Un nouveau modble de r6actlon catalytique sur couches flmd~s&s est dCveloppC Le prmclpe
de ce mod&le, appelC le ModBle dassemblage de bulles, repose sur une multitude de bulles de
ddT&entes grosseurs, un tchange de gaz ayant lem entre la phase bulle et la phase Cmulslon
Le modkle de demandent aucun parambtre r&&e, 11apparait pmcuh&ement utde pour 16tude
des crolssances dtchelles Le mod&le proposC convlent aussl pour les slmulatlons de calcul La
vabQtC de ce mod&le a Ctt test& & partlr des don&es expknmentales de ddfirents chercheurs On a
trouvC que les converstons prkvues utdlsant ce modtle saccordent assez blen avec la performance
actuelle des couches flm&sbes

Zusammenfassung-Es wlrd em neues Model1 fur die katalytlsche Reaktion m der Wlrbelschlcht
entwrckelt Dleses als Blasenaufbaumodell bezelchnete Model1 baslert auf emer Vlelzahl von
Blasen verschledener Grosse, wobel zwlschen der Blasenphase und der Emulslonsphase Gasau-
stausch stattfindet
Da&eses Model1 keme veranderhchen Parameter benotlgt, wlrd angenommen, dass es zur Unter-
suchung massstabhcher Vergrosserungen geelgnet 1st Das vorgeschlagene Model1 1st femer fur
Slmuherung auf Rechnem verwendbar Es wurden Versuchsergebmsse emer Relhe von Forschern
herangezogen urn &e Gultq$elt &eses Modelles nachzuwelsen Es wurde festgestellt, dass der unter
Anwendung des Modelles vorausgesagte Umsatz recht gut mlt der tatsachhchen Lelstung der Wlrbel-
schlcht uberemstlmmt

1369