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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
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
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
1352
Bubble assemblage model
purposes. In addition d the model mvolves more pute either the Interchange coefficrent between
than two parameters, the analysis could become the two phases or the fractron of catalyst present
hopelessly difficult in the bubble phase. The results of studies using
Another technique useful for the search of thrs techmque are summarrzed m Table 2.
flow behavior m a flurdlzed bed is to compare the Although the parameters obtained by this
conversion obtamed m a flmdlzed bed reactor technique may satisfactorily represent the
wrth that obtamable m a fixed bed reactor under mdivrdual experimental results, it IS doubtful
the same operating conditions. This technique that these parameters have any physical slgmfi-
Initiated by Shen and Johnstone[37] also needs cance under other operating conditions for
a presupposed model for evaluation of model flmdized beds of complex flow patterns.
parameters Experimental data are used to com- So far most of the experimental data on
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
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
Parameter
Authors assumed Method aorF, Remarks
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
1354
Bubble assemblage model
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
first power of the bed height. In fact several sets expenmental evidence mdlcatmg that the bubble
of the data indicate the power on the bed height diameters are shghtly smaller when the bed
to be somewhat smaller than umty. However, diameter becomes larger. However, the relatlon-
before more accurate measurement of bubble ship between the bubble velocity and the bubble
diameter with respect to bed height becomes diameter 1s also affected by the change m bed
possible, there 1s at present no Justification of diameter. In other words, for a larger bed, the
using more sophlstlcated correlation beyond velocity of the bubble having the same diameter
that of Kobayashl et al [ 181. will become shghtly larger due to the reduced
Stnctly speaking, the bubble diameter also fnctlon along the wall of the bed Just how great
should vary slightly with the bed dla DR under the wall effect on the bubble velocity is not very
the same fluldlzatlon condltlons There IS an clear at present Hence, until additional research
1356
Bubble assemblage model
is made to provrde more refined relattonshtp of Fan, Lee and Baihe[8] m&cate the voidage
between the bubble veloctty and the bed dta- up to the bed height corresponding to L, can
meter, Eqs. (6) and (8) are believed to be most be considered approxnnately umform and that
reliable today. the votdage above L, increases along the bed
The above correlation IS based on the data height. For an approxrmatlon, rt is assumed that
obtained using porous plates as the distributor. above the bed height correspondmg to Lw,
For perforated plates the size of bubbles at the (1 -E) decreases linearly wtth respect to the
surface of the dtstnbutor are substantial and bed height. It is further assumed that the average
therefore must be taken mto constderatton. bed height reported m the experiments can be
According to Cooke et a/.[31 the bubble srze considered as an arithmetic average of the maxi-
at the surface of a perforated plate havmg no mum bed height correspondmg to E = 1 and Lw.
number of holes, can be calculated from (SC/W)4/ Following Davidson and Harnson[5], the
g 2 based on the work of Davidson and Harrison velocity of nse of a crowd of bubbles through a
[5] where G = (U-U&/Q,. Therefore, m general, fluidtzed bed can be calculated by
the diameter of bubbles m a fluidized bed can be
approxtmated by u;, = ~~--/.++0~711(gD~)~. (8)
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
1357
K KATO and C Y WEN
[27], and Tanaka[38] As seen from the figure, for large U/U&, U, 1s neghgrbly small This 1s a
the ratios of calculated bed herght to expen- reasonable assumptron m vtew of the fact that
mental bed he&t are wtthm + 10 per cent of 1 0 the experimental findmgs of May [3 l] and Kunu
mdtcatmg a favorable agreement. Thus, m model and Levensptel[22] mdtcate the emulston gas
development, Eq (9) may be used to compute may reverse its dtrectton m vtgorously bubbhng
the bed he&t with reasonable accuracy Once beds According to Kunn and Levensptel[22],
the bed expansion ratio 1s known, the votdage the velocity of gas flowmg m the emulsion phase
from the distributor up to a height correspond- m the axial direction can be expressed as
mg to Ld and that from Lti to the top of the bed
can be computed, respectively, as
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
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
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
K KATO and C Y WEN
The drstance from the distributor to the n-th bed height above Lw, the voulage IS adjusted by
compartment is Eq. ( 12) and Vm, vb, and V,, are obtamed using
the same procedure as that shown for the height
h, = 2 Ahf (20)
f=l smaller than Lw The calculatton 1s repeated
until the bed height reaches L,+ 2(L- L,,J. A
The gas interchange coefficient based on unit
computer logtc dtagram based on thrs procedure
volume of bubbles from Eq. (3) can be shown as
1s shown m Table 5.
No
No
& End
and Arai [20] for intermediate reactton rates and the two phases IS of prtmary importance whereas
those of Massmnlla and Johnstone[29] for small for slow reactions the gas interchange between
reactron rates, respectrvely. the two phases does not affect stgntficantly on
As can be seen from these figures, when the the converston.
rate of reactron 1s small, the concentratton of gas To examme the gas velocity effect, a compar-
m the emulston phase 1s not too much different lson of the conversron predrcted by the model
from that in the bubble phase However, when and that from actual expenments IS shown m
the rate of reactron IS large, the difference m Fig. 7. In Fig 8, the calculated conversion IS
concentratrons between the two phases become compared with the expenmental converston
very stgmficant For a fast reaction, a great deal based on nearly all the data presented in the
of gaseous reactant m the emulston phase 1s studres listed m Table 2 Consrdenng the dlf-
seen to be converted m the rmmedrate vrcmtty ticultres m obtarmng accurate kinetic mformatton
of the drstnbutor These observations imply from tied bed expenmentatlon and the posstble
that for fast reacttons the gas interchange between vanatron of catalyst acttvtttes dunng the flutdrzed
1361
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
1362
Bubble assemblage model
-Bubble phosr
-- - - - - Emulrlon phaw
Pornmeter =u/u,
----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
agam seems to be remarkable. Notice that the computer stmulatlon and can handle rather
reaction progresses very rapidly just above the easily even cases involving complex reaction
distributor. The profile calculated from a model rate expressions One of the weaknesses of this
characterized by a smgle effective bubble size model as m any other model is the uncertainty
IS unlikely to exhibit such a trend of knowledge of gas velocity m the emulsion
The foundation of the proposed Bubble phase, u, It can be shown that the conversion
Assemblage Model lies on the knowledge of calculated based on this model is rather m-
variation m bubble diameters along the bed sensitive to the value of u,, nevertheless, further
axis Hence more accurate measurement of mvestlgatton on this subject is needed The
bubble growth is necessary to ascertain the model can be extended to include solid parttcle
bubble diameter correlation presented here mixing pattern which may be used to develop
In addition the knowledge of gas interchange a flmdtzed bed reactor model for a non-catalytic
between the two phases is also a very important solid-gas reacting system. This ~111be presented
factor particularly for fast reactions and there- m another paper
fore should be further mvestlgated The charac-
teristics of the proposed model is its versatlhty CONCLUSION
and adaptability for varying situations. This The catalytic conversion measured by expen-
is believed to be due to the fact that the model ments of others can be predicted by the Bubble
is developed based on an assemblage of multiple Assemblage Model in terms of the reported
bubbles which grow as they nse through the kinetic constants and the operating condl-
bed The scale-up constderation is now possible ttons The model needs no adJustable parameters
with fair amount of confidence m the accuracy and 1s useful for design and scale-up of the
of the results The model is also convenient for flutdized bed reactor The correct grasp of the
1364
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
-
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
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
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