You are on page 1of 12

Chemical Engineering Science 62 (2007) 70 – 81

www.elsevier.com/locate/ces

Generalized bubbling–slugging fluidized bed reactor model


J.P. Constantineau a , J.R. Grace a,∗ , C.J. Lim a , G.G. Richards b
a Department of Chemical and Biological Engineering, University of British Columbia, Vancouver, Canada V6T 1Z3
b Teck Cominco Metals Ltd., Trail, British Columbia, Canada V1R 4L8

Available online 22 August 2006

Abstract
A generalized slugging–bubbling fluidized bed reactor model is developed which handles seamlessly the transition from bubbling to slugging
fluidization, using the concept of probabilistic averaging developed in earlier work. The ratio of the bubble diameter to the column diameter
is employed to correlate the probability of each of these fluidization flow regimes. The model gives a good representation of the conversions
within the slugging and bubbling regimes, as well as for the transition between these two regimes.
䉷 2006 Elsevier Ltd. All rights reserved.

Keywords: Fluidization; Chemical reactor; Modelling; Slugging fluidized beds

1. Introduction scale-up. A 1.5-m-deep bed was required to obtain a 90%


yield in a 50-mm-diameter laboratory reactor. For a 300-mm-
Over the years, great success has been achieved in the de- diameter pilot-scale reactor, the same yield required a bed 2.8 m
sign and implementation of new fluidized bed processes. How- high. For a 3-m-diameter industrial reactor, a bed 10 m high was
ever, the reputation of fluidized bed reactors has suffered from required to reach the same yield (Werther, 1980; Wen, 1984).
some failures which occurred even though pilot reactors oper- The strong scale-up effect is primarily due to the growth of bub-
ated successfully. The most notable example (Geldart, 1967) bles and their effect on the gas residence time and interphase
was in the production of gasoline by Fischer–Tropsch synthe- mass transfer.
sis. Pilot-scale reactors (12, 25, 50 and 195 mm diameter) were Scale-up of fluidized bed processes has received considerable
operated successfully with conversions exceeding 95%. With attention in the literature (e.g. Volk et al., 1962; Geldart, 1967;
such encouraging results, a complete industrial plant was built Matsen and Tarmy, 1970; Matsen, 1985, 1996; Glicksman,
with a fluidized bed reactor of approximately 5 m diameter. Re- 1998). Similarity techniques have been developed and used
grettably, conversions of only 40–50% were obtained from the to scale fluidized beds for hydrodynamic studies (Glicksman,
industrial unit. After gaining experience on a 2.4-m-diameter 1998). However, reacting systems often cannot be scaled using
pilot plant, the industrial unit was modified and the conversions these techniques, especially when the reactions are the object
increased to 65–70%. After operating for a few years, the pro- of study. Different reactor models have been formulated for the
cess was uneconomic, and production ceased, highlighting the bubbling and slugging fluidization regimes. No reactor models
difficulty of fluidized bed reactor scale-up. have been formulated to include both bubbling and slugging
One of the main difficulties in scale-up has been associ- fluidization flow regimes with the specific focus of addressing
ated with the use of results from pilot plants operating in the the questions associated with scale-up.
slugging fluidization regime to design large industrial reactors Recently, a generic fluidized bed reactor model has been
operated in the bubbling fluidzation regime. The Shell Chlori- formulated to span the bubbling, turbulent and fast fluidization
nation Process (de Vries et al., 1972), involving catalytic oxi- regimes (Abba et al., 2002, 2003). Using probabilistic aver-
dation of HCl to produce Cl2 , also illustrates the difficulties of aging, this model successfully handles the transitions among
these three flow regimes when the superficial gas velocity is
∗ Corresponding author. Tel.: +1 604 822 3121; fax: +1 604 822 6003. increased. However, it does not cover cases where transitions
E-mail address: jgrace@chml.ubc.ca (J.R. Grace). from bubbling to slugging occurs. This article extends the
0009-2509/$ - see front matter 䉷 2006 Elsevier Ltd. All rights reserved.
doi:10.1016/j.ces.2006.08.011
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 71

probabilistic approach to a new generalized slugging–bubbling 2


fluidized bed reactor model where a single set of differential
equations describes the phenomena occurring within the bub- 1.75
bles and dense-phase, and the parameters are averaged accord-
Zone III
ing to the probability of being in one fluidization flow regime
1.5
or the other. This model is primarily intended for group B par-
ticles (Geldart, 1973) where slug flow is most commonly en-
1.25 P=1
countered.

H (m)
1.1. Bubbling and slugging fluidization regimes 1 Zone II

In a bubbling fluidized bed, bubbles coalesce as they rise 0.75


P=0.5
through the bed causing their average diameter to increase with
Zone I
height. As the bubble diameter approaches the reactor diameter, 0.5
the bubbles can no longer grow, and slugging takes over. As the
bubble size increases, the effect of the walls becomes greater P=0
0.25
and one expects a smooth transition from bubbling to slugging
fluidization. Slugging may therefore be considered as a special
0
case of bubbling where the bubble size is physically constrained 0 0.25 0.5 0.75 1 1.25 1.5 1.75 2
by the walls of the reactor. D (m)
Three conditions are necessary for slugging:
Fig. 1. Influence of column diameter on zones in a slugging fluidized bed,
for incipient slugging, calculated using the Geldart (1972) bubble size corre-
• The bed height (H ) must exceed a minimum height. Baeyens
lation for porous plate distributors. Zone I: freely bubbling, Zone II: slugging
and Geldart (1974) measured (HL ) where bubble coalescence with limited coalescence, Zone III: stable slugging with no further coales-
is complete and stable slug spacing is achieved and proposed cence, based on Baeyens and Geldart (1874). P-lines correspond to slugging
the correlation: probabilities of 0, 0.5 and 1.

HL = 1.3D 0.175 . (1)


dark lines were derived from an equation proposed by Baeyens
• The superficial gas velocity (U ) must exceed the minimum
and Geldart (1974). The upper line was obtained by fitting the
slugging velocity (Ums ) given (Stewart and Davidson, 1967)
heights observed experimentally when stable slugging was es-
by
 tablished i.e. Eq. (1). The lower dark line was obtained by cal-
Ums = Umf + 0.07 gD (2) culating the height where the bubble diameter from the Geldart
(1972) bubble size correlation is equal to half the bed diame-
Baeyens and Geldart (1974) utilized this criterion for deep ter at the minimum slugging velocity, calculated from Eq. (3).
beds (Hmf > HL ). For shallower beds, they proposed Note that the minimum slugging velocity varies with column
 diameter. While informative, this earlier approach adopts arbi-
Ums = Umf + 0.07 gD + 0.16(HL − Hmf )2 . (3)
trary and sharp boundaries at which there are step changes in
• The maximum stable bubble size (De,max ) must be at least behavior. In reality, the transitions are gradual. This paper mod-
of the order of the column diameter (D). els these gradual transitions using weighting factors which de-
scribe the relative probabilities of bubbling and slugging over
The conditions for stable slugging clearly depend on column the height interval where the transition takes place. The thinner
diameter and bed height. A shallow bed may not experience dashed lines provide these weighting factors or probabilities of
slugging because coalescence may be insufficient for the bub- slugging, as discussed below.
bles to reach the bed diameter. For deeper beds, bubble growth Other correlations can also be used to determine the height
and coalescence may be sufficient to engender slugging. Addi- where free bubbling ends and slugging takes over. For example,
tional criteria for the occurrence of slugging were summarized Darton et al. (1977) used their bubble size correlation to obtain
by Agarwal (1987). a height condition for slugging which depends on distributor
Baeyens and Geldart (1974) divided slugging fluidized beds design.
into three zones:
2. Modelling the transition from bubbling to slugging
• Zone I: Freely bubbling.
• Zone II: Slugging with limited coalescence. Previous slugging fluidized bed reactor models have consid-
• Zone III: Stable slugging with no further coalescence. ered the reactor as a simple one-zone stable slugging bed, or
have split the reactor into freely bubbling and stable slugging
Fig. 1 represents these three zones in a bed at minimum slugging zones. Currently, no model adequately accounts for the tran-
velocity as a function of height and column diameter. The two sition in a slugging fluidized bed. Modelling the transition to
72 J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81

slug flow may be attempted in various ways: ging fluidized beds. Neither considers the effect of the freely
bubbling zone near the gas distributor. Hovmand and David-
• One can use two distinct models, one for bubbling and one
son (1968, 1971) created the first slugging fluidized bed re-
for slugging, applying a bubbling model up to a given height,
actor model by extending the Orcutt et al. (1962) piston-flow
then switching to a slug flow model. This approach has been
fluidized bed model and deriving an interphase mass transfer
used to model slug flow reactors (e.g. Hovmand et al., 1971;
coefficient expression for slugs. Raghuraman and Potter (1978)
Yates and Grégoire, 1980a, b; Yue and Zarifis, 1990; Sadaka
based their slug flow model on the Fryer and Potter (1972)
et al., 2002). A bubbling fluidized bed reactor model is used
countercurrent backmixing model for bubbling fluidized beds,
for the first 1.5–2D where the bed is freely bubbling (Zone
and utilized the analysis of Hovmand et al. (1971) for the gas
I). Above this height, a stable slug-flow model is used (Zone
interphase mass transfer coefficients.
III). However, the transition zone (Zone II) is not accounted
The Orcutt et al. (1962), Hovmand et al. (1971) and
for. The problem with this approach is that there is a dis-
Raghuraman and Potter (1978) models neglect reaction of the
continuity where the switch is made, whereas in practice the
gas in contact with solids suspended in the bubbles or slugs.
transition occurs smoothly. Moreover, there is uncertainty in
Grace (1984, 1986) has shown that this assumption is not valid
predicting the regime transition.
for large effective reaction rate constants. Aoyagi and Kunii
• One could use the results from the two models and interpo-
(1974) have shown experimentally that solids within bubbles
late or average their results. A probabilistic average, based
may play a significant role, even if their concentration is small.
on the weighted sum of the results where the weights are
based on the probability of being in a given regime, would
better characterize the uncertainty of the regime transition.
A problem with this approach is that the interpolated results 3. Extension of the generalized model concept to
are not necessarily consistent with the physics of the system, bubbling/slugging
especially where there are nonlinearities.
• A better method is to combine the two models into a single Our new steady-state fluidized bed reactor model extends
model which approaches the two limiting models outside the generalized bubbling, turbulent and fast fluidization reactor
the transition range. In the transition region between the model of Abba (2002, 2003), which accounts for variable gas
two flow regimes, the model probabilistically averages the density (due to the pressure gradient and changing composition
parameters (not the final predictions) for each regime. This as one or more reactions proceed) and bulk flow in the inter-
approach has been used previously to model the transition phase mass transfer using a probabilistic approach. The model
from bubbling to turbulent fluidization and from turbulent to developed here only considers the bubbling and slugging flow
fast fluidization (Thompson et al., 1999; Grace et al., 1999; regimes. Also, the approach used to model changes in total gas
Abba et al., 2002, 2003). In that case, simple Re vs Ar cor- molar flow differs from that of Abba (2002).
relations were employed to describe the regime transitions Fig. 2 represents the two phases of the model, named the
(Thompson et al., 1999; Abba et al., 2003), with probabilities L- and H-phases for low-density and high-density phases. The
related to rms deviations. These probabilities then provide L-phase represents the bubbles or slugs, while the H-phase
weighting factors for setting the values of key parameters. represents the dense phase or emulsion. Gas enters at the bottom
A somewhat similar approach was employed by Eakman et of the fluidized bed where it is distributed between the L- and
al. (1980) to model a coal gasifier subject to both bubbling H-phases. The gas then rises in each phase and reacts with the
and slugging. However, instead of using the probability of solids present. Mass transfer occurs between the two phases.
being in a given regime, they used an arbitrary function to Axial and radial dispersion could be included within each phase.
interpolate the parameters in the transition interval.
Currently, the transition from bubbling to slugging fluidiza- 3.1. Phase balances
tion is only described by the minimum slugging velocity (Ums )
and the necessary conditions for slugging. The criteria for the As in our previous work (Thompson et al., 1999; Abba et
transition do not quantify the probability of slugging, nor do al., 2002, 2003), the bed volume fractions of phases add up to
they allow for a smooth transition from freely bubbling near unity, i.e.,
the distributor via a smooth transition zone to stable slugging
above. L + H = 1. (4)

Each phase volume is composed of particles and void space.


2.1. Previous models for the bubbling and slugging
The particle volume fraction () and gas volume fraction ()
fluidization regimes
within each phase also add up to 1, i.e. L + L = 1 and
H + H = 1. The total gas molar flowrate (FT ) through the
Bubbling fluidized bed reactors have received considerable
reactor equals the sum of the phase molar flowrates, i.e.
attention (e.g. see Chavarie and Grace, 1975; Grace, 1986),
whereas slugging fluidized bed reactors have received relatively
little attention. Two basic models have been developed for slug- FT = FLT + FH T . (5)
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 73

 
Freeboard dFH i FLi  FH i FH R
− + kLH aI − L + k r H v i
dz UL H U H UH
FH R FLi
− kr H v = 0. (11)
UH FLT
The interphase mass transfer coefficient (kLH ) is defined as
the volumetric rate of transfer per unit bubble (or slug) surface
area. The interphase mass transfer exchange area (aI ) is the
interfacial bubble area per unit bubble volume. Multiplying the
two gives the volumetric transfer rate per unit bubble volume.
Δz Δz
Bulk interphase mass transfer is required when a change in gas
volume occurs within the H-phase. According to the two-phase
fluidization theory, a flow of gas of Umf A is required for the
H-phase L-phase high-density phase. Any excess gas enters the low-density phase
to create bubbles. In a reacting system, the requirement for the
high-density phase is still present. However, if there is a volume
change, it must be balanced by bulk interphase transfer. The
direction of the bulk flow and the required gas molar fraction
depends on the sign of v. In this case, it is assumed to be
negative. If v were positive, any excess gas produced in the
UH FL UL dense phase would go to the L-phase.
FH
These equations are solved using an initial value solver with
boundary conditions
FT U
FLi = FLi,in = L AUL Ci,in (at z = 0), (12)
Fig. 2. Schematic of two-phase fluidized bed model. FH i = FH i,in = H AUH Ci,in (at z = 0). (13)
The superficial gas velocities (UL and UH ) and the phase vol-
ume fractions (L and H ) are calculated at a series of heights
For ideal gases, the total concentration (CT = PT /RT). The
in the bed beginning at the entrance. The superficial gas ve-
gaseous molar flowrates are related to the superficial gas ve-
locity (U ) is first calculated from the gaseous molar flowrates
locities (U , UL and UH ) by
(FH T and FLT ). The L-phase superficial gas velocity (UL ) is
equal to the void velocity (Uv ), calculated below. This requires
FT = AUCT , (6)
an appropriate bubble size correlation.
The low-density phase volume fraction (L ) is estimated
FHT = H AUH CT and FLT = L AUL CT . (7)
(Clift and Grace, 1985) using
The molar flowrates of gaseous species i in the H- and L-phases U − Umf
L = . (14)
are UL
Since the set of differential equations is solved from the distrib-
FH i = H AUH CH i and FLi = L AUL CLi . (8)
utor (z = 0) to the surface of the expanded bed, the expanded
bed height (H ) must be known, or estimated and then calcu-
Simplifying with the aid of Eq. (5), we obtain lated iteratively. Since only the volume occupied by the bubbles
and slugs (L-phase) contributes to the bed expansion,
U = L UL + H UH . (9)
 H
H − Hmf = L dz. (15)
3.2. Gas mole balances for H- and L-phases 0
With the appropriate choice of parameters, the model can de-
The differential gas mole balance over the control volume scribe a bubbling fluidized bed, a purely slugging bed or a
for the low-density (L) and high-density (H) phases of Fig. 2, bubbling–slugging bed.
for a first-order irreversible reaction assuming steady-state con-
ditions and neglecting axial and radial dispersion, are 3.3. Interphase mass transfer
 
dFLi L F H i FLi FLR
− + kLH aI − + k r  L vi Among the parameters in Eqs. (10) and (11), only kLH and
dz H U H UL UL aI require probabilistic averaging between their bubbling and
FH R FLi slugging values. For bubbling and slugging fluidized beds, L
+ kr H v = 0, (10)
UH FLT and H are usually constant. For a freely bubbling fluidized
74 J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81

Table 1 For freely bubbling beds, the bubble rise velocity (Ub ) is given
Surface integral (I ) for various slug length-to-diameter ratios by
L/D 0.3 0.5 1.0 2.0 3.0 4.0 5.0
Ub = Ub∞ + (U − Umf ). (25)
I 0.13 0.21 0.39 0.71 0.98 1.24 1.48
At minimum fluidization, Eq. (25) predicts a non-zero bubble
rise velocity. As in previous work (Thompson et al., 1999) the
expression for bubble rise velocity is therefore modified so that
bed, the interphase mass transfer coefficient (kLH ,bubbling ) and
Ub → 0 as U → Umf :
area (aI H ,bubbling ) are obtained (Sit and Grace, 1981) from
 
  0.71 
Umf Dg mf Ub∞ 1/2 Ub = (U − Umf ) 1 + gDe . (26)
kLH ,bubbling = +2 , (16) U
3 De
This change makes negligible difference in the overall predic-
6 tions, but facilitates the use of the probabilities as weighting
aI,bubbling = . (17)
De factors below.
Since the velocity of bubbles depends on their size, the effec-
The interphase mass transfer coefficient (kLH ) and area (aI ) tive bubble size (De ) must be calculated as a function of height.
for slugging fluidization can be expressed in similar form Numerous correlations are available (e.g. Mori and Wen, 1975;
(Hovmand and Davidson, 1971), giving Darton et al., 1977; Horio and Nonaka, 1987). Since particles
 1/2  of Geldart Group A behave differently from Group B particles,
16mf I Dg g 1/4
kLH ,slugging = Umf + , (18) especially with respect to the maximum bubble size, the bubble
1 + mf  D size correlation must be chosen carefully.
The velocity of a single slug (Us∞ ) is given by
1
aI,slugging = . (19) 
Dfs Us∞ = 0.35 gD. (27)
The surface integral (I ) (see Table 1) and slug shape fac- For a continuously slugging bed, the slug velocity (Us ) is
tor (fs ) are functions of the slug length-to-diameter ratio
(Hovmand and Davidson, 1971) with Us = Us∞ + (U − Umf ). (28)
   1/2 In order to bridge the bubbling and slugging fluidization
4V L L
fs = = − 0.495 + 0.061. (20) regimes, the void (bubble or slug) rise velocities (Uv∞ ) are
D 3 D D
described in dimensionless form
The slug length-to-diameter ratio can be obtained (Hovmand et Uv∞
al., 1971) by solving the quadratic equation Fr = √ (subscript  = b or s) (29)
gD
 1/2  
L L U − Umf Eqs. (24) and (27) may then be written as
− 0.495 1+ √
D D 0.35 gD
Bubbling Fr = 0.71, (30)
(T /D − 0.061)(U − Umf )
+ 0.061 − √ = 0, (21)
0.35 gD Slugging Fr = 0.35, (31)

where T is the slug-to-slug (tail-to-nose) separation distance. where  is the ratio of square root of diameter, De /D.
The generalized interphase mass transfer coefficient and area Allahwala and Potter (1979) measured isolated bubble and
are calculated by weighting factors analogous to those obtained slug rise velocities in a gas–solid fluidized bed and correlated
in previous work by probabilistic averaging, i.e. the results by
ktransition = (1 − Pslugging )kLH ,bubbling + (Pslugging )kLH ,slugging , Fr = 0.35 tanh1/1.8 [3.6()1.8 ]. (32)
(22)
Instead of using this relatively complex equation to calculate
atransition = (1 − Pslugging )aI,bubbling + (Pslugging )aI,slugging . the velocities and evaluate the probabilities, a simpler fitting
(23) approach is employed here. Fig. 3 presents the velocities in an
air–water system. The transition between the limits of single
3.4. Void velocities and weighting factors for isolated bubbles and single isolated slugs given by Eqs. (30)
bubbling/slugging and (31) is smooth and occurs for  between about 0.38 and
0.7 (Hovmand and Davidson, 1971). The behavior at each end
For the bubbling fluidization regime, the isolated bubble rise of the transition interval clearly approaches the two limiting
velocity is cases, with the slopes equal to each of the limiting values.
 We require an interpolation between the two limits which
Ub∞ = 0.71 gDe . (24) fits the experimental data and gives the proper limiting slopes.
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 75

1
Fr = 0.35
0.35
0.9

0.3

ζ
0.8

.71
=0
0.7
Fr
0.25

0.6
0.2

Pslugging
Fr

0.5

0.15
0.4

0.1 0.3

0.2
0.05
No wall effect Transition Slug
0.1
0.319 0.493 0.714
0 0.493
0 0.2 0.4 0.6 0.8 1 0
0 0.2 0.4 0.6 0.8 1
ζ
ζ
Fig. 3. Bubble rising velocity in water in the presence of wall effects. √
Fig. 4. Probability of slugging as a function of  = De /D.
Experimental points from Hovmand and Davidson (1971).

for details) as
A fit in the intermediate region (between pure bubbling and
pure slugging) was obtained by a transformation of variables. Pslugging = 0 ( 0.319), (37)
The resulting piecewise fit is
Pslugging = 2.794X 2 − 0.491X 3 (0.319 <  0.493), (38)
Fr = 0.71 (0.319), (33)
Pslugging = −0.813 + 4.116X − 2.794X 2 + 0.491X 3
Fr = 0.2265 + 0.2805X − 0.1904X + 0.0334X 2 3
(0.493 <  < 0.714), (39)
(0.319 <  < 0.714), (34)
Pslugging = 1 ( 0.714), (40)
Fr = 0.35 (0.714), (35)
The gas velocity is assumed to be low enough that we are only
where considering bubbling and slugging. Hence

 − 0.319 Pbubbling = 1 − Pslugging . (41)


X= . (36)
0.395 Fig. 4 presents the resulting weighting factor for slugging
This piecewise fit is shown in Fig. 3. as a function of . This procedure allows a smooth transi-
Outside the transition interval, the weighting assigned to tion between pure bubbling (Pbubbling = 1) and pure slugging
slugging is taken as 0 for 0.319 and 1 for  0.714. (Pslugging = 1) as  increases from 0.319 to 0.714. While this
In the transition interval, the slugging weighting factor in- approach is conceptually similar to the probabilistic transitions
creases smoothly from 0 to 1. A reasonable estimate of in the generalized fluidized bed reactor model (Abba et al.,
in the intermediate region, 0.319 <  < 0.714, was obtained 2002, 2003), in the current case, the transition takes place over
by considering the growing deviation of the corresponding height as  grows due to coalescence, whereas in the bub-
void velocity (Eq. (34)) from the corresponding wall-effect- bling/turbulent/fast fluidization transitions of the generalized
independent bubble rise velocity (Eq. (33)) in the lower part fluidized bed reactor model, the transitions are taken to be only
of the transition interval, and then the shrinking difference functions of the superficial gas velocity.
between the void velocity and the slug flow (Eq. (35)) limit
in the upper section of the transition interval. The condition 3.5. Transition to slugging
( = 0.35/0.71 = 0.493) when the two limiting velocities are
equal defines the point where the weighting factors for slug- According to the equations presented in the preceding sec-
ging and bubbling are equal, i.e., Pbubbling =Pslugging =0.5. The tion, slug flow is dominant for  0.714, i.e for De 0.51D,
weighting factors are then assigned (see Constantineau, 2004 while wall effects are negligible for  0.319, i.e., for
76 J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81

De 0.1D. Combining a correlation√ for bubble diameter with In general, the predictions for the bubbling fluidized bed
the definition of , i.e.,  = De /D, and Eqs. (37)–(41) al- models are higher than for the slugging models. Note that the
lows one to predict lines of constant probability of slugging for fluidized bed models are applied without any allowance for
fluidized beds operated in the bubbling and slug flow regimes slugging, even when the bubble size exceeds the reactor diame-
as plotted in Fig. 1. Since Baeyens and Geldart (1974) used ter. For this reason, the predictions for small column diameters
the Geldart (1972) bubble size correlation, the same correlation must be considered with caution.
has been employed in this figure to calculate the probability of When the weighting factor for slugging is 1, the results of
slugging. Note that the superficial gas velocity in Fig. 1 varies the Hovmand et al. (1971) slugging model and the GSBM
with column diameter. The location of the line with a proba- model are indistinguishable in Fig. 5. The GSBM therefore
bility of slugging of 1 is virtually equal to that calculated by essentially reduces to the Hovmand et al. slugging model
Baeyens and Geldart (1974) for the transition from freely bub- in the  0.714, Pslugging = 1 limit. When considering pure
bling to slugging with limited coalescence. An important fea- bubbling behavior (Pbubbling = 1), the GSBM is seen to cal-
ture of this figure is that the transition range of the probabilities culate similar conversions to the bubbling bed models con-
(i.e. 0 < Pslugging < 1) falls within Zone I, closer to bubbling for sidered, though with small differences due to variations in
Pslugging 0.5 and approaching slug flow for Pslugging > 0.5. assumptions.

4. Reactor model predictions 4.2. Influence of effective reaction rate constant

With the weighting factors for the two flow regimes now de- The influence of the effective reaction rate constant, kr , on
fined, the generalized bubbling–slugging fluidized bed reactor the gas conversion is presented in Fig. 6 for different reactor
model proceeds in an analogous manner to the generalized bub- diameters with some solids in the low-density phase, L =
bling turbulent model (Thompson et al., 1999). The probabili- 0.005 and neglecting any solids within the bubbles or low-
ties are used as weighting factors to adjust and interpolate such density phase (i.e., L =0). The figure presents the results of the
factors as the interphase mass transfer coefficients in the range complete generalized slugging–bubbling model, as well as the
(0.319 <  < 0.714) between pure bubbling and pure slugging. predictions when the probabilities of bubbling and slugging are
equal to one (entirely slugging or bubbling). When Pslugging =
1, no bubbling region is considered prior to slugging. When
4.1. Comparison with previous models Pbubbling = 1, the model either calculates a given bubble size for
each height or uses a constant average bubble size calculated
Previous models in the literature have assumed either pure at 40% of the expanded bed height (z = 0.4H ). The model
bubbling or pure slugging in any given zone. Fig. 5 presents parameters and conditions are again as given in Table 2.
conversions calculated from the Hovmand et al. (1971) slug- For slugging beds (Figs. 6a and b), bubbling bed models tend
ging bed model, the Orcutt et al. (1962) mixed-flow and plug- to overpredict the conversions. For small kr , the generalized
flow models, the Grace (1984) two-phase bubbling bed reactor slugging–bubbling fluidized bed model predicts conversions
model and our generalized slugging–bubbling model (GSBM) similar to those for pure slugging (where Pslugging =1) since the
for pure slugging and pure bubbling with constant average bub- conversion is primarily reaction-controlled. For higher kr , the
ble size and variable bubble size for a first order chemical re- generalized slugging–bubbling fluidized bed model predictions
action, with the operating conditions as given in Table 2. The diverge from the pure slugging predictions due to the increas-
constant average bubble size case is considered because both ing importance of interphase mass transfer from the bubbles
the Orcutt and Grace models use an average bubble size. Since and slugs to the dense phase. For such conditions, the bubbling
previous models do not consider changes in gas volumetric flow region at the base of the bed before the onset of slugging is of
due to variations in hydrostatic pressure and total molar flow, critical importance to the conversion. The presence of particles
the comparisons here are for constant total volumetric and mo- within the bubbles (L ) significantly augments the predicted
lar flow. conversions for large kr by compensating for limited interphase
mass transfer.
Table 2 For large vessels where slugging does not occur (Figs. 6e
Model parameters used to compare the generalized bubbling slugging model and f), the GSBM model predicts the same conversions as for
to earlier slugging and bubbling models pure bubbling (Pbubbling =1). The use of an average bubble size
Figs. 5, 6 and 7 Fig. 8 results in reduced gas conversions for large reaction rate con-
stants. For large kr , mass transfer from the bubbles to the dense
U 0.5 m/s 0.5 m/s
phase is rate-controlling. There is then a significant beneficial
Umf 0.02 m/s 0.02 m/s
H 1.0 m Calculated effect on interphase mass transfer from the small bubbles near
Hmf Calculated 1.0 m the distributor, which disappears when a single average bub-
mf 0.45 0.45 ble size is adopted. As for slugging beds, accounting for the
Gas diffusivity: Dg 1.0 × 10−4 m2 /s 1.0 × 10−4 m2 /s presence of particles within the bubbles (L ) is significant for
Bubble correlation Mori and Wen (1975) Mori and Wen (1975)
large kr . For fluidized beds of intermediate sizes (Figs. 6c
Initial bubble size: Deo 0.01 m 0.01 m
and d), the GSBM model predictions diverge slightly from the
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 77

0.5 0.5
Slug flow models, kr = 1 s-1 Bubbling bed models, kr = 1 s-1
0.4 0.4

Conversion (-)

Conversion (-)
0.3 0.3

0.2 0.2
Orcutt, Plug Flow
Orcutt, Mixed
0.1 0.1 GSBM, PBubbling=1, Constant De
Hovmand
Grace 2-phase
GSBM, PSlugging=1 GSBM, PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

1 1
Slug flow models, kr = 10 s-1 Bubbling bed models, kr = 10 s-1

0.8 0.8
Conversion (-)

0.6 Conversion (-) 0.6

0.4 0.4
Orcutt, Plug Flow
Orcutt, Mixed
0.2 0.2 GSBM, PBubbling=1, Constant De
Hovmand Grace 2-phase
GSBM, PSlugging=1 GSBM, PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

Fig. 5. Comparison of the GSBM model to the Hovmand et al. (1971) slugging model and to the Orcutt et al. (1962) and Grace (1984) bubbling bed models.
For conditions, see Table 2.

predictions for pure bubbling due to the effect of the walls as part from pure slugging for reactor diameters larger than about
bubbles grow with height, causing Pslugging to increase, and 0.1 m. The departure from pure slugging at the higher reaction
hence the interphase mass transfer to decrease. rate constant results from the bubbling region near the distrib-
If one chooses a regime-specific model (either pure bubbling utor. In the calculations leading to Fig. 7, as shown in Table 2,
of pure slugging) for cases where there are zones of Pslugging the expanded bed depth, H, was fixed, consistent with the in-
between 0 and 1, there can be substantial errors. For reactions dustrial equipment related to the modelling, for which there
with large values of the effective reaction rate constant (kr ), the was a weir, limiting the bed expansion. In Fig. 8, on the other
model should not use an average bubble size to characterize hand, as in most comparisons in the literature, the bed inven-
the entire reactor and should include the effect of solids within tory, and hence Hmf is fixed. In the latter case, we observe the
the bubbles. The generalized slugging–bubbling fluidized bed usual overall trend of decreasing conversion with increasing
model allows the modelling of fluidized systems where a transi- column diameter. In both cases the model smoothly interpolates
tion from bubbling to slugging occurs within the bed, or where between the two limiting cases of pure slugging and pure bub-
there are appreciable wall effects. bling as D increases. The minimum in the conversion predicted
in Fig. 8 for D ≈ 0.3 m is not expected, and it is not known
4.3. Effect of reactor diameter whether there are any experimental results which would confirm
such a trend.
The predicted effect of scale-up of a reactor for different re- In the predictions of Figs. 5–8, the bubble diameters have
actor diameters and different rate constants is shown graphi- been based on the correlation of Mori and Wen (1975). Other
cally in Fig. 7. The GSBM model is seen to approach the slug- bubble diameter correlations would result in somewhat different
ging limit for small columns and then to approach the bubbling predictions. For the conditions studied, the predictions of the
bed limit with increasing column diameter, giving a smooth GSBM model converge to pure bubbling at column diameters
transition between these limits in the intervening region. For close to 1 m. This is the minimum reactor diameter for the
the conditions considered, the GSBM model predictions de- system to be modelled as pure bubbling. Note that results from
78 J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81

1 1
PBubbling=1, Variable De PBubbling=1, Variable De
GSBM GSBM
0.8 PBubbling=1, Constant De 0.8 PBubbling=1, Constant De
PSlugging=1
PSlugging=1

Conversion (-)
Conversion (-) D = 0.1 m
0.6 D = 0.1 m 0.6
φL = 0 φL = 0.005

0.4 0.4

0.2 0.2

0 0
10-2 100 102 10-2 100 102
(a) kr, s-1 (b) kr, s-1

1 1
PBubbling=1, Variable De PBubbling=1, Variable De
GSBM GSBM
0.8 PBubbling=1, Constant De 0.8 PBubbling=1, Constant De
PSlugging=1 PSlugging=1

Conversion (-)
Conversion (-)

0.6 D = 0.5 m
0.6 D = 0.5 m
φL = 0 φL = 0.005

0.4 0.4

0.2 0.2

0 0
10-2 100 102 10-2 100 102
(c) kr, s-1 (d) kr, s-1

1 1
PBubbling=1, Variable De PBubbling=1, Variable De
GSBM GSBM
0.8 PBubbling=1, Constant De 0.8 PBubbling=1, Constant De
PSlugging=1
PSlugging=1
Conversion (-)
Conversion (-)

0.6 D=1m 0.6 D=1m


φL = 0 φL = 0.005

0.4 0.4

0.2 0.2

0 0
10-2 100 102 10-2 100 102
(e) kr, s-1 (f) kr, s-1

Fig. 6. Comparison of conversions predicted by GSBM model and its limiting models as a function of reaction rate constant and column diameter. For
operating conditions see Table 2.

small and large industrial fluidized beds must be compared with model developed here has the same structure as the generic
care. In the transition region, the generalized model predicts fluidized bed reactor model formulated to span the bubbling,
conversions intermediate between those for pure bubbling and turbulent and fast fluidization regimes (Abba et al., 2002,
for pure slugging. 2003). To construct a model useful for both diameter and
velocity scale-up, one must account for the transition from
5. Discussion slugging to turbulent fluidization. Since the superficial gas
velocity where the transition to the turbulent regime occurs
For reactions where interphase mass transfer is rate-limiting, (Uc ) varies with bed diameter (Bi et al., 2000), a generalized
the size of bubbles has a critical effect on the conversion. The slugging–bubbling–turbulent regime probability model which
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 79

0.6 kr = 1 s-1, φL = 0 0.6 kr = 1 s-1, φL = 0.005

0.5 0.5

Conversion (-)

Conversion (-)
0.4 0.4

0.3 0.3

0.2 0.2
GSBM GSBM
0.1 PSlugging=1 0.1 PSlugging=1
PBubbling=1, Variable De PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

1 1
kr = 10 s-1,φL =0 kr = 10 s-1,φL = 0.005
0.8 0.8
Conversion (-)

Conversion (-)
0.6 0.6

0.4 0.4

0.2 GSBM 0.2 GSBM


PSlugging=1 PSlugging=1
PBubbling=1, Variable De PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

Fig. 7. Comparison of the conversions calculated using GSBM model and its limiting cases as a function of bed diameter for different gas reaction rate
constants with constant expanded bed depth. For conditions, see Table 2.

kr = 1 s-1, φL = 0 kr = 1 s-1, φL = 0.005


0.6 0.6

0.5 0.5
Conversion (-)
Conversion (-)

0.4 0.4

0.3 0.3

0.2 0.2
GSBM GSBM
0.1 PSlugging=1 0.1 PSlugging=1
PBubbling=1, Variable De PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

1 1
kr = 10 s-1, φL = 0 kr = 10 s-1, φL = 0.005

0.8 0.8
Conversion (-)

Conversion (-)

0.6 0.6

0.4 0.4

0.2 GSBM 0.2 GSBM


PSlugging=1 PSlugging=1
PBubbling=1, Variable De PBubbling=1, Variable De
0 0
10-1 100 10-1 100
Bed Diameter (m) Bed Diameter (m)

Fig. 8. Comparison of the conversions calculated using GSBM model and its limiting cases as a function of bed diameter for different gas reaction rate
constants with constant bed depth at minimum fluidization. For conditions, see Table 2.
80 J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81

accounts for superficial gas velocity, bed diameter and height, HL limiting bed height where coalescence is com-
as well as gas and particle properties, must first be developed plete and stable slug spacing achieved, m
before adding the slugging fluidization flow regime into the Hmf bed height at minimum fluidization, m
generic fluidized bed reactor model. Once a consistent descrip- I slug surface integral function,dimensionless
tion of the probabilities is available, adding the slugging regime kLH interphase mass transfer coefficient, m/s
to the generic fluidized bed reactor model should be straight- kr reaction rate constant, s−1
forward. L slug length, m
Pbubbling weighting factor analogous to probability of
bubbling,dimensionless
Pslugging weighting factor analogous to probability of
6. Conclusion slugging,dimensionless
PT total reactor pressure, Pa
A new model is proposed to predict the performance of flu- R universal gas constant, 8.314 J/(mol K)
idized bed reactors operated wholly or partially in the slug flow T slug-to-slug (tail-to-nose) distance, m
regime. This model simulates the transition from bubbling to U reactor superficial gas velocity, m/s
slugging within a given reactor as operating variables such as Ub bubble rise velocity, m/s
superficial gas velocity, bed inventory and height change. It Ub∞ isolated bubble rise velocity, m/s
interpolates smoothly between the limits where the bed oper- UH H-phase superficial gas velocity, m/s
ates entirely in the bubbling bed flow regime and the slug flow UL L-phase superficial gas velocity, m/s
regime as height increases within a given reactor, or as the col- Umf superficial gas velocity at minimum fluidization,
umn diameter is varied. m/s
Ums superficial gas velocity at minimum slugging,
m/s
Us slug velocity, m/s
Notation
Us,∞ slug velocity of a single slug in a bed at
minimum fluidization, m/s
A bed cross-sectional area, m2 Ut• terminal velocity of spherical particles of
Ad distributor area per orifice, m2 diameter 2.7dp , m/s
aI interphase mass transfer exchange area, m−1 Uv void (bubble or slug) rise velocity, m/s
CH i molar concentration of species i in H-phase, Uv∞ free void (bubble or slug) velocity, m/s
mol/m3 z height coordinate, m
Ci,in inlet molar concentration of species i, mol/m3
CLi molar concentration of species i in L-phase, Greek letters
mol/m3
CT total gaseous molar concentration v difference in gas total stoichiometric coefficient
(CT = PT /RT), mol/m3 due to reaction, dimensionless
D reactor diameter, m z finite height in bed (control volume), m
De effective bubble diameter, m H H-phase gas volume fraction, m3 /m3
De,0 initial effective bubble diameter, m L L-phase gas volume fraction, m3 /m3
De,∞ maximum bubble diameter due to coalescence mf bed voidage at incipient fluidization, m3 /m3
and growth, m  square root
√ of bubble-to-column diameter
Dg gas diffusivity, m2 /s ratio = De /D, dimensionless
FH i molar gas flowrate of species i in H-phase, I Stoichiometric coefficient of reactant i, dimen-
mol/s sionless
FH i,in inlet gas molar flowrate of species i in H-phase, H H-phase solids volume fraction, m3 /m3
mol/s L L-phase solids volume fraction, m3 /m3
FH T total gas molar flowrate in H-phase, mol/s H H-phase volume fraction, m3 /m3
FLi molar gas flowrate of species i in L L-phase volume fraction, m3 /m3
L-phase, mol/s
FLi,in inlet gas molar flowrate of species i in L-phase,
mol/s Acknowledgments
FLT total gas molar flowrate in √L-phase, mol/s
Fr Froude number = U∞ / gD, dimensionless The authors thank Teck Cominco Metals Ltd. and the Nat-
FT total gas molar flowrate in reactor, mol/s ural Science and Engineering Research Council of Canada
fs slug shape factor, m3 /m3 (NSERC) for financial contribution and the Science Council
g acceleration due to gravity, m/s2 of British Columbia for supporting J. Pierre Constantineau
H expanded bed height, m through a GREAT Scholarship.
J.P. Constantineau et al. / Chemical Engineering Science 62 (2007) 70 – 81 81

References Grace, J.R., 1986. Fluid beds as chemical reactors. In: Geldart, D. (Ed.), Gas
Fluidization Technology. Wiley, New York, pp. 285–339.
Abba, I.A., Grace, J.R., Bi, H.T., 2002. Variable-gas-density fluidized bed Grace, J.R., Abba, I.A., Bi, H.T., Thompson, M.L., 1999. Fluidized bed
reactor model for catalytic processes. Chemical Engineering Science 57, catalytic reactor modeling across the flow regimes. Canadian Journal of
4797–4807. Chemical Engineering 77, 305–311.
Abba, I.A., Grace, J.R., Bi, H.T., Thompson, M.L., 2003. Spanning the Horio, M., Nonaka, A., 1987. A generalized bubble diameter correlation for
flow regimes: generic fluidized-bed reactor model. A.I.Ch.E. Journal 49, gas–solid fluidized beds. A.I.Ch.E. Journal 33, 1865–1872.
1838–1848. Hovmand, S., Davidson, J.F., 1968. Chemical conversion in a slugging
Agarwal, P.K., 1987. Effect of bed diameter on bubble growth and incipient fluidised bed. Transactions of the Institution of Chemical Engineers 46,
slugging in gas fluidised beds. Chemical Engineering Research and Design 190–203.
65, 345–354. Hovmand, S., Davidson, J.F., 1971. Pilot plant and laboratory scale fluidized
Allahwala, S.A., Potter, O.E., 1979. Rise velocity equation for isolated reactors at high gas velocities: the relevance of slug flow. In: Davidson,
bubbles and for isolated slugs in fluidized beds. Industrial and Engineering J.F., Harrison, D. (Eds.), Fluidization, first ed. Academic Press, London
Chemistry Fundamentals 18, 112–116. and New York, pp. 193–259.
Aoyagi, M., Kunii, D., 1974. Importance of dispersed solids in bubbles Hovmand, S., Freedman, W., Davidson, J.F., 1971. Chemical reaction in
for exothermic reactions in fluidized beds. Chemical Engineering a pilot-scale fluidized bed. Transactions of the Institution of Chemical
Communications 1, 191–197. Engineers 49, 149–162.
Baeyens, J., Geldart, D., 1974. An investigation into slugging fluidized beds. Matsen, J.M., 1985. Fluidized beds. In: Bisio, A., Kabel, R.L. (Eds.), Scale-
Chemical Engineering Science 29, 255–265. up of Chemical Processes. Wiley, New York, pp. 347–405.
Bi, H.T., Ellis, N., Abba, I.A., Grace, J.R., 2000. A state-of-the-art review of Matsen, J.M., 1996. Scale-up of fluidized bed processes: principle and
gas–solid turbulent fluidization. Chemical Engineering Science 55, 1–37. practice. Powder Technology 88, 237–244.
Chavarie, C., Grace, J.R., 1975. Performance analysis of a fluidized bed Matsen, J.M., Tarmy, B.L., 1970. Scale-up of laboratory fluid-bed data: the
reactor. Industrial and Engineering Chemistry Fundamentals 14, 75–91. significance of slug flow. A.I.Ch.E. Symposium Series 66 (101), 1–7.
Clift, R., Grace, J.R., 1985. Continuous bubbling and slugging. In: Davidson, Mori, S., Wen, C.Y., 1975. Estimation of bubble diameter in gaseous fluidized
J.F., Clift, R., Harrison, D. (Eds.), Fluidization, second ed. Academic Press, beds. A.I.Ch.E. Journal 21, 109–115.
London, pp. 73–132. Orcutt, J.C., Davidson, J.F., Pigford, R.L., 1962. Reaction time distributions
Constantineau, J.P., 2004. Fluidized bed roasting of zinc sulfide concentrate: in fluidized catalytic reactors. Chemical Engineering Progress Symposium
factors affecting the particle size distribution, Ph.D. Thesis, University of Series 58 (38), 1–15.
British, Columbia. Raghuraman, J., Potter, O.E., 1978. Countercurrent backmixing model for
Darton, R.C., LaNauze, R.D., Davidson, J.F., Harrison, D., 1977. Bubble slugging fluidized-bed reactors. A.I.Ch.E. Journal 24, 698–704.
growth due to coalescence in fluidized beds. Transactions of the Institution Sadaka, S.S., Ghaly, A.E., Sabbah, M.A., 2002. Two phase biomass air–steam
of Chemical Engineers 55, 274–280. gasification model for fluidized bed reactors. Biomass and Bioenergy 22,
de Vries, R.F., van Swaaij, W.P.M., Mantovani, C., Heijkoop, A., 1972. 439–487.
Design criteria and performance of the commercial reactor for the shell Sit, S.P., Grace, J.R., 1981. Effect of bubble interaction on interphase mass
chlorine process. Proceedings of the Fifth European Second International transfer in gas fluidized beds. Chemical Engineering Science 36, 327–335.
Symposium on Chemical Reaction Engineering. Elsevier, Amsterdam, Stewart, P.S.B., Davidson, J.F., 1967. Slug flow in fluidised beds. Powder
pp. B9:59–69. Technology 1, 61–80.
Eakman, J.M., Wesselhoft, R.D., Dunkleman, J.J., Vadovic, C.J., 1980. Gasifier Thompson, M.L., Bi, H.T., Grace, J.R., 1999. A generalized bubbling/
operation and modeling in the Exxon catalytic coal gasification process. turbulent fluidized-bed reactor model. Chemical Engineering Science 54,
Coal Processing Technology 6, 146–158. 2175–2185.
Fryer, C., Potter, O.E., 1972. Countercurrent backmixing model for fluidized Volk, W., Johnson, C.A., Stotler, H.H., 1962. Effect of reactor internals on
bed catalytic reactors. Applicability of simplified solutions. Industrial and quality of fluidization. Chemical Engineering Progress 58 (3), 44–47.
Engineering Chemistry Fundamentals 11, 338–344. Wen, C.Y., 1984. Flow regimes and flow models for fluidized bed reactors.
Geldart, D., 1967. The fluidized bed as a chemical reactor: a critical review In: Doraiswamy, L.K. (Ed.), Recent Advances in the Engineering Analysis
of the first 25 years. Chemistry and Industry 1474–1481. of Chemically Reacting Systems. Wiley Eastern, New Delhi, pp. 256–290.
Geldart, D., 1972. The effect of particle size and size distribution on the Werther, J., 1980. Mathematical modeling of fluidized bed reactors.
behavior of gas-fluidised beds. Powder Technology 6, 201–215. International Chemical Engineering 20, 529–541.
Geldart, D., 1973. Types of gas fluidization. Powder Technology 7, 285–292. Yates, J.G., Grégoire, J.-Y., 1980a. An experimental test of slugging-bed
Glicksman, L.R., 1998. Fluidized bed scale-up. In: Yang, W.-C. (Ed.), reactor models. In: Grace, J.R., Matsen, J.M. (Eds.), Fluidization. Plenum
Fluidization, Solids Handling, and Processing: Industrial Applications. Press, New York, pp. 581–588.
Noyes, Westwood, NJ, pp. 1–110. Yates, J.G., Grégroire, J.-Y., 1980b. Catalytic oxidation of o-xylene in a
Grace, J.R., 1984. Generalized models for isothermal fluidized bed reactors. slugging fluidized bed. Chemical Engineering Science 35, 380–385.
In: Doraiswamy, L.K. (Ed.), Recent Advances in the Engineering Analysis Yue, P.L., Zarifis, N., 1990. Catalytic dehydration of ethanol in a fluidized
of Chemically Reacting Systems. Wiley Eastern, New Delhi, pp. 237–255. bed reactor. A.I.Ch.E. Symposium Series 86 (276), 119–125.

You might also like