Modelling A Circulating Fluidized Bed Riser Reactor With

Gas-Solids Downflow At The Wall

DAVID M. J. PUCHYR, ANIL K. MEHROTRA and LEO A. BEHIE*

Department of Chemical and Petroleum Engineering, The University of Calgary, Calgary, AB T2N 1N4, Canada

and

NICOLAS E. KALOGERAKIS

Department of Chemical Engineering, State University of New York, Buffalo, NY 1422604200, U.S.A.

A predictive model was developed for the fully developed zone of a circulating fluidized bed (CFB) riser reactor oper-
ating in the fast fluidization regime that overcomes limitations of existing models. The model accounts for the upward
flow of gas and solids in the core and downward flow of the two phases in the annulus. Additionally, a numerical solu-
tion methodology for the simulation of a riser reactor employing the hydrodynamic model was devised. A simulation
was performed using the fast, main Claw reaction to demonstrate the effects of backmixing in the fast fluidization
regime. It was found that the molar flow rates of the reactants leaving a fast fluidized CFB riser reactor were signifi-
cantly higher than those leaving an identical reactor operating in the pneumatic transport regime.

Un modele predictif a ete mis au point pour la zone pleinement developpee d’un reacteur a colonne montante et a lit
fluidise circulant fonctionnant dans un regime de fluidisation rapide qui depasse les limites des modeles existants. Le
modele tient compte de I’ecoulement ascendant du gaz et des solides dans l’ecoulement au coeur et I’ecoulement ascen-
dant des deux phases dans I’espace annulaire. De plus, on a conqu une methodologie de resolution numerique pour la
simulation d’un reacteur a colonne montante employant le modele hydrodynamique. On a effectue une simulation a
I’aide de la reaction principale de Claus - qui est rapide - afin de demontrer les effets du retromelange dans le regime
de fluidisation rapide. Les debits molaires des kactifs quittant un reacteur a colonne montante et a lit fluidise circulant
rapide se sont averees plus grands que dans le cas d’un reacteur fonctionnant en regime de transport pneumatique.

Keywords: circulating fluidized bed, predictive model, core-annulus. gassolids downflow.

Contractor et al. (1994) clearly demonstrated that the

S ix distinct hydrodynamic regimes exist when a gas is
passed upward through a bed of Group B particles (Grace,
1986). Varying degrees of solids entrainment occur when the
pneumatic transport regime can justifiably be modelled as a
plug flow reactor (PFR) as a good first approximation. The
gas superficial velocity is greater than the incipient fluidiza- applicability of the PFR model is explained by the cocurrent
tion velocity. If the entrained solids are recirculated back to flow of gas and solids and the large slip factor in a CFB oper-
the bottom of the bed it can be classified as a “circulating flu- ating in this regime. Their experiments, performed on a large
idized bed” (CFB) (Bermti et al., 1995). Throughout this scale pilot plant used to oxidize n-butane to maleic anhy-
study we consider the two cases in which a CFB is operating dride, yielded gas phase residence time distributions which
in either the fast fluidized or pneumatic transport regimes. showed very little gas dispersion at various axial sampling
locations. The lack of axial dispersion indicates near plug
CIRCULATING FLUIDIZED BED RISER REACTORS flow conditions. The use of a pre-reactor particle accelerator,
a proprietary device, resulted in approximately uniform sus-
An advantage of using a conventional fluidized bed over
pension densities for very large solids mass fluxes ranging
a fixed bed reactor is that the excellent axial mixing of solids
from 290 to 690 kg/m2.s. The uniform suspension densities
caused by the bubbles in a fluidized bed allows for near
indicate that the acceleration zone in the reactor, the region
isothermal operation of the reactor when cooling tubes are
at the base of the reactor where the solids are accelerated to
employed. But, the bubbles are also the vehicle for gas by-
their steady-state velocity, which is characterized by chaot-
passing, which reduces the gas-solids contacting, thereby
ic mixing of the two phases, can be effectively eliminated.
reducing conversion. A CFB, which also allows for near
In order to model a CFB as a plug flow reactor, the bed
isothermal operation via the relatively large heat capacity of
density must be calculated so that the reaction rate can be
the recirculated solids, provides outstanding gassolids con-
determined. The bed density is a function of voidage which,
tacting because of the slip factor (w)between the two phases.
in turn, is a hnction of operating conditions and particle
The slip factor is defined as “the ratio of interstitial gas
characteristics. Knowing the overall slip factor, the solids
velocity over the solids velocity”. In the fully developed
mass flux (GJ, particle density (ps), and gas superficial
zone of a tall riser, the overall slip is approximately 2
velocity (ugo), the average “plug flow” voidage in the reac-
(Bermti et al., 1995; Patience et al., 1992; Matsen, 1976).
tor is heuristically determined to be:
Therefore, the problem of gas by-passing present in a con-
ventional fluidized bed is essentially eliminated in a CFB.

*Author to whom correspondence should be addressed. E-mail address:

behie@acs.ucalgary.ca

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997 317
 Complications, such as the formation of solids clusters, TABLE1
agglomerations of particles with a relatively low interparti- Average Solids Fractions Determined Using The Fully Developed
Zone Pressure Gradient Data of Rhodes et al. ( 1992),
cle voidage, greatly alter the hydrodynamics of the reactor The “Plug Flow” Voidage, and Our Model
and, therefore, necessitate the development of a model more
sophisticated than the PFR model. Experimental work per- us0 [ d s ] G, [kg/m2.s] D [m] ( 1 - E)” ( 1 - E ) ~ ( I - E)‘
taining to clusters is still in its infancy and a complete under- 4 20.0 0.152 0.0073 0.006 0.0065
standing of the hydrodynamics associated with them has not 4 30.7 0.152 0.0112 0.009 0.0099
been presented. Soong et al. (1995) standardized the defini- 4 49.7 0.152 0.0181 0.015 0.0159
tion of a cluster so that effective comparisons between inde- 4 62.7 0.152 0.0228 0.019 0.0200
pendently obtained experimental data could be made. The 5 36.3 0.152 0.0101 0.004 O.OOX9
5 47.8 0.152 0.0139 0.010 0.01 16
focus of our work is on the development of a practical, pre-
5 94.4 0.152 0.0274 0.020 0.0226
dictive model describing the fully developed zone of a CFB 5 111.0 0.152 0.0323 0.023 0.0264
riser reactor operating in the fast fluidization regime. The 4 20.0 0.305 0.0039 0.007 0.0057
presence of clusters is accounted for in our model by using 4 40.0 0.305 0.0078 0.015 0.01 13
average values for the interparticle voidage in the various 4 60.0 0.305 0.0117 0.022 0.0168
regions within the riser reactor. a Average solids fraction determined using the pressure gradient.
A riser with a smooth, rather than abrupt, exit operating b Average solids fraction determined using Equation ( I ) .
in the fast fluidized regime can be divided into three distinct c Average solids fraction determined using our model.
regions based on observed solids behavior: The core, annu-
lus, and acceleration zones. Each region is coupled to the
others by appropriate boundary conditions. The first region, operating conditions and particle characteristics. In a recent
the core, occupies approximately 90% of the riser cross-sec- publication, Patience and Chaouki ( I 995) calculated values
tional area and is characterized by upward flow gas and for the gas (a,) and solids (@J core area fractions for their
solids. It is dilute in terms of suspension density relative to model but used different values for those variables in their
the other regions. Typical voidages in the core range from RTD computations. The resulting RTD match was good
0.95 to 0.999 for laboratory scale circulating fluidized beds, only because of the fitting of the @ and cDS parameters;
but can be lower for industrial scale units which employ therefore, their model is not truly prekctive.
large mass fluxes and pre-reactor particle accelerators Pugsley (1995) developed a predictive model with limited
(Contractor et al., 1994). dependence on empirical correlations that, in theory, would
The region concentrically surrounding the core and bound be sound when used for scale-up purposes. However, under-
by the wall of the CFB is the annulus. The gas and solids lying shortcomings in his model, as in the Patience-Chaouki
flow downward in this region. The suspension density in the model (1993, 1995), are:
annulus is higher than in the core and is highly dependent 1. The gas is assumed to be stagnant in the annulus.
upon the operating conditions and particle characteristics. 2. Equation (1) is used for determining the average
For example, Pugsley (1 995) measured the interparticle interparticle voidage ( E ) in the fully developed zone.
voidage in the annulus (E,) at 0.62 1 with a solids mass flux The use of Equation (1) for the determination of the aver-
of 240 kg/m2.s and a gas superficial velocity of 5 m/s . For age voidage in the fully developed zone of the riser is the
the same superficial velocity, Hartge et al. ( 1 988) measured key to the predictive nature of the models. However, the
E, at 0.965 with a solids mass flux of 75 kg/m2.s. internal reflux of gas and solids influence the voidage, or,
The third region in a CFB operating in the fast fluidiza- equivalently, solids fraction ( 1 - E ) , in the riser by conser-
tion regime is the acceleration zone. It is located at the base vation of mass. Therefore, using Equation ( I ) , the “plug
of the reactor and is due to the re-injection of solids from the flow” voidage, to calculate the average voidage in the fully
standpipe and the internal refluxing of the solids from the developed zone is suspect because it neglects the influence
annulus to the core. The length of this region can be mini- of the gas and solids refluxed into the core from the annulus.
mized with the use of a pre-reactor particle accelerator. Table 1 shows the average solids fractions in a riser deter-
Moreover, in industrial scale risers, typically greater than mined by using pressure gradient data and by using
15 m tall, the acceleration zone can be a small fraction of the Equation (I). Agreement between the two solids fractions is
total reactor height. good, but misleading. If the gas is assumed to be stagnant in
the annulus, the voidage in the core must be less than the
SHORTCOMINGS OF EXlSTlNG CFB RISER MODELS voidage predicted by Equation ( I ) due to the internal reflux-
ing of solids. Therefore, the assumptions of stagnant gas in
Patience and Chaouki (1995, 1993) developed a model the annulus and voidage being calculated from Equation ( I )
that simulates both the gas and solids phases in the fully are contradictory.
developed zone of a CFB riser operating in the fast fluidiza- The fact that the average solids fraction in the fully devel-
tion regime. The gas phase modelling is based on the work oped zone is close to the solids fraction calculated using
of Brereton et al. (1988) and the solids phase modelling was Equation (1) is because the gas in the annulus is not stag-
developed using the data of Rhodes et al. (1992) and Zhang nant. In certain instances the gas is also reintroduced into the
et al. (1991). The Patience-Chaouki model (1992, 1995) core at the base of the riser, thereby increasing the gas flow
matches experimental gas and solids RTD data very well. in the core (Kruse et al., 1995): The last three entries at the
So, it must be asked, “Why develop a new model?”. The bottom of Table I , those obtained from a 30.5 cm diameter
answer is simply because the Patience-Chaouki model riser, provide clear evidence of gas refluxing since the mea-
(1993, 1995) is unrealistic in describing the hydrodynamics sured solids fractions, 0.0039, 0.0078 and 0.01 17, are all
in the annulus and is, in fact, not predictive. A predictive significantly less than the “plug flow” solids fractions of
model for a CFB can accurately simulate a process given the 0.007,0.015, and 0.022. Assuming a constant molar volume

318 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75. APRIL, 1997

Figure I - Schematic diagram of our model for the h l l y devel-
oped zone of a circulating fluidized bed riser reactor operating in
the fast fluidized regime.
for the gas, the only means by which the solids fraction in
the fully developed zone could be less than the “plug flow”
solids fraction is by the internal refluxing of the gas. The
internal refluxing of the gas in a CFB riser reactor is of par-
ticular significance because it represents backmixing which
can have catastrophic effects on conversion by reducing
reaction rates (Ouyang et al., 1995).
Ouyang et al. (1 995) modelled a fast fluidized CFB riser
reactor incorporating the downward flow of the gas in the
annulus. Their model was a major improvement over the
models presented above in terms of realism, but was not
totally predictive. For their particular simulation, the solids
velocity in the annulus was assumed to be -1.0 d s . The
non-predictive nature of their model makes its application
limited to risers where the downflow of solids in the annu-
lus can be determined.
Additionally, the analytical solution Ouyang et al. (1995)
obtained for their reaction modelling cannot be applied gen-
erally since only a single reaction was taken into account.
When multiple reactions with highly non-linear kinetics
occur an analytical solution is not likely to be found.
The three main goals in the development of our model for
the fully developed zone of a CFB riser reactor operating in
the fast fluidization regime are to:
1. Make our hydrodynamic model predictive and practical.
2. Account for the downward flow of gas and solids in
the annulus.
3. Devise a general, numerical solution methodology for
the modelling of a CFB as a chemical reactor with
highly non-linear intrinsic reaction kinetics.
THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997
Fully developed zone model
It is assumed that the CFB has a smooth exit so that the
hydrodynamics are not influenced by the exit geometry. A
schematic diagram of our model is shown in Figure I . Unlike
the Patience-Chaouki model ( 1993, 1995) and the Pugsley
model (1995), our predictive model for the fully developed
zone of a CFB riser reactor accounts for the observed down-
ward flow of both the gas and solids in the annulus.
HYDRODYNAMIC
MODEL
The radius of the core
The core and annulus regions are in the fully developed
zone of the riser and are the focus of this study. For a con-
stant flow rate, neither the gas nor the solids undergo accel-
eration in these regions as indicated by the constant pressure
gradient (Bodelin et al., 1994, Rhodes et al., 1992). In our
model, the radius of the core is taken as constant throughout
the filly developed length of the reactor. It is calculated
using an averaged form of Werther’s ( 1994) equation:
Equation (2) was chosen to determine the radius of the
core because the correlation is state-of-the-art and is based
upon a pool of data that consisted of both laboratory and
industrial scale units. Also, it is not based upon the fitting of
RTD data. Rather, it was determined by the actual physical
radial location of zero net solids velocity which, by defini-
tion, is the radius of the core.
Beside maintaining simplicity, there are two other rea-
sons for using the averaged form of the correlation present-
ed by Werther (1994):
I . The radius of the core varies with solids mass flux
when the gas superficial velocity is held constant.
2. The radius of the core is not zero at the exit of the
riser.
Equation (2) does not account for the effect of the solids
mass flux on the radius of the core. Data given by Rhodes
et al. (1992) show up to a 10% variance in the radius of the
core when the gas superficial velocity was held constant and
the solids loading was increased. In their experiments, the
variation of the solids mass flux was quite large (2 to
11 1 kg/m2.s). The deviation in the radius of the core with
varying solids mass fluxes decreases significantly if only
fluxes with the same order of magnitude are considered and
with increased reactor radius.
Furthermore, data presented by Werther (1994) show that
the radius of the core is not equal to the riser radius at the
top of the column.
Gas and solids profiles
The model developed in this study applies to risers in
which the gas flows upward in the core and downward in the
annulus. Our model assumes that plug flow of the gas occurs
in both regions. On the other hand, the solids mass flux pro-
file and solids velocity profile are not linear.
Rhodes et al. (1992) assumed a solids mass flux profile of
the form:
(3)
319
 They found that a value of m = 5 fit their extensive pool
of data most effectively. Only the form and exponent value
of Equation (3) are common between our model and that of
Rhodes et al. ( 1 992). The parameters a and b are calculated
with different methodologies.
It is also assumed that the solids velocity profile is para-
bolic (Pugsley, 1995; Miller and Gidaspow, 1992) and is of
the form:
The interparticle voidage profile in the fully developed
zone of the reactor varies radially as well because it is deter-
mined by combining Equations (3) and (4) appropriately:
E(r)=l-- G,si r ) . . . . . . . . . . . . . . . . . . . . . . . . . . .
P s u.7 ( r )
Obviously, Equation (5) is not applicable at the boundary
of the core and annulus ( r = rc) where both the solids mass
flux and velocity are zero.
The parameters a, b, c, and d, as well as the gas velocity
in the annulus (u ) and core (ugc)must be calculated. (The
explanation of w%y uga and ugc are included in the list of
unknowns is forthcoming.) Therefore, six equations govem-
ing the CFB system must be known.
The first two equations are derived from the fact that the
solids mass flux and velocity at the radius of the core are, by
definition, zero. That is,
........................
and
The third equation comes from the following assumption
of our model: The solids velocity at the wall is equal to the
terminal velocity of a single particle relative to the gas
velocity in the annulus. Therefore, with the upward direc-
tion being positive, at r = R,
k + u , = d ..............................
1' r= R
The fourth equation comes from another assumption of
our model: The slip velocity at the centerline of the reactor
is equal to the terminal velocity of a single particle.
Expressed mathematically this assumption is:
k + u , =c+d.. ..........................
E(r=o
The final two equations are based upon conservation
equations for both the gas and solids phases. For the gas
(assuming that the ideal gas law is applicable):
320
For the solids:
..........
Note that the local slip factor can be calculated once tiRL
and the constants c and d have been determined by dividing
u by us at r. The overall slip factor can be calculated by
$C
dividing unC by the average of u , ~ .
Solids interchange between the core and the annulus is
(4)
not considered in our model. Hence, its application is
restricted to systems in which catalyst deactivation does not
occur on a single pass basis.
Pressure drop
Frictional losses in the fully developed zone are negligi-
ble (Pugsley, 1995; Louge and Chang, 1990). Hence, the
pressure drop through the fully developed zone is due to the
(5) hydrostatic head of solids in the riser. The average differen-
tial pressure drop is:
.....................
dz
REACTION MODEL
Modelling the core
Both the gas and the solids flow upward in the core.
Similar to many other models (Ouyang et al., 1995; Pugsley,
1995; Patience and Chaouki, 1993; Brereton et al., 1988).
our model assumes plug flow of the gas phase in the core.
Consequently, the differential mass balance on species i is:
(6)
.................................... (13)
Equation (13) shows that the gas phase of the core and
annular regions are coupled by means of a cross-flow coef-
ficient (k ). It accounts for equimolar exchange between the
core a n 8 annulus driven by the concentration gradients
between the two regions. Several values for the cross-flow
coefficient have been reported and are shown in Table 2 .
Pugsley (1992) used a modified form of the Higbie
Penetration Theory (Higbie, 1935) to estimate k so that the
predictive nature of his model would be mainjained. The
result was that the cross-flow coefficient was of the order of
lop2 m / s . Recently, Ouyang et al. (1 995) performed experi-
(8)
ments using ozone decomposition in a CFB and fit kK to best
match their data. Table 2 shows that the values obtained by
Ouyang et al. ( 1 995) are similar to those obtained by using
the modified Higbie Penetration Theory. The results of
Ouyang et al. (1995) are significant to this study because
their non-predictive model incorporated downward flowing
gas in the annulus (as in our model). Hence, the modified
Higbie Penetration Theory presented by Pugsley ( 1992) can
(9) be justified for calculating kg and is used in our model.
Modelling the annulus
The differential mass balance on species i in the annulus is:
.......................................... (14)
T H E CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997
 TABLE2
Calculated Cross-Flow Coefficients ( k ) Reproduced From 2.0
Ouyang et al. (1 9 9 8
ugo [ d s l 2 3 4 6 8
1.5
G, [kg/m2,s] 100 150 200 300 400
Method of
van der Ham et al.
G
‘ 1.0
( 1994) 0.0066 0.0105 0.0148 0.0237 0.0332 0-
Method of
PugsIey et aI. kg [ d s ]
-$
LL
0.5
(1 992) 0.0083 0.01 15 0.0144 0.0200 0.0251 v1

Method of 5
Ouyang et al. 4
2 0.0
( 1 995) 0.0100 0.0150 0.0200 0.0300 0.0300 m
B
2
Y -0.5
Equation (14) differs from the annular mass balance for
.&
the Patience-Chaouki (1993, 1995) and h g s l e y (1995)
models because our model accounts for the downward flow
of gas in the annulus. Consequently, a convective term is -1 .o
included in the mass balance.
The boundary conditions for Equations (1 3) and (14) are: 4
At z = 0: The molar flow rate of species i in the core is -1.5
, 1
,
I

equal to the inlet flow of i plus the flow rate of i in the
. annulus at z = 0.
At z = L: The concentration of species i in the annulus
is equal to the concentration of i in the core. (The molar
flow rate of i in the annulus at z = L is determined by
maintaining the overall mass balance on i.)
Similarly, for the solids:
At z = 0: The solids flow rate in the core is equal to the
inlet solids flow rate plus the flow rate of solids in the
annulus.
At z = L: The solids flow rate in the core is equal to the
inlet solids flow rate; the solids flow rate in the annulus
is determined by maintaining the overall mass balance
(or by using the solids mass flux profile and the radius
of the core given by the hydrodynamic model).
Differential Equations (13) and (14) and their boundary
conditions define a two point boundary value problem with
a condition that must be met at z = L (Ci,a= Ci,,) given the
inlet feed. The solution methodology is presented in the
Results and Discussion section.
Results and discussion
Given riser diameter and height, particle characteristics,
and inlet gas superficial velocity, composition, temperature,
and pressure, Equations (2) through (1 0) were solved to
describe the hydrodynamics within various risers. Each of the
cases used to validate our model were non-reactive systems.
Equations ( 13) and (14) were used in the simulation of a
riser reactor to demonstrate the effects of backmixing. The
numerical solution methodology for the reaction modelling
was as follows:
1. Solve Equations (2) through (10) to determine the
hydrodynamics in the riser reactor.
2. Calculate the voidage in the core (E,) and annulus (E,)
by averaging the non-linear solids’ profiles in each of
the two regions.
3. Estimate the composition of the gas flowing from the
annulus to the core at the base of the riser. (In our
simulation the we initially took the equilibrium com-
position).
-1.0 -0.5 0.0 0.5 1 .o
Reduced Radius. r / R
Figure 2 -Comparison between the predicted ( a = 3.14, h =
-1.24) and measured solids mass flux profile. [Data of Rhodes
et al. (1992); D = 74.9 p,p, = 2456 kg/m3, D = 0.305 m, L =
6.6 m, G, = 60 Rg/m2.s,ugo = 4 d s ] .
4. Integrate Equation (13), with the inlet and annular
inputs, from the base of the riser to the top storing the
gas composition at each node in the core. (The first
time through set the cross-flow coefficient to zero).
5. Maintain the overall mass balances on the reactor riser.
6. Compare the flow rates of the components leaving the
riser reactor with the results obtained from the previ-
ous iteration. (If the flows are within the specified tol-
erance the simulation converged.)
7. Initialize the gas composition at the top of the annulus
to be equal to the composition at the top of the core.
8. Integrate Equation (14) from the top of the riser to the
base storing the compositions at each node in the annulus.
9. Go to Step 4.
The system took five iterations to converge with the com-
position tolerance of Step 6 set to l v .
VERIFICATION
OF OUR HYDRODYNAMIC MODEL
Equations (2) through (10) are the basis for the predictive
nature of our model. It is necessary to validate the predicted
profiles with experimental data. Rhodes et al. (1992) measured
the solids mass flux rofile in two risers using solids with a
P
density of 2456 kg/m and a surface-volume mean diameter of
74.9 p.The larger of the two risers was 30.5 cm in diameter
and 6.6 m tall while the smaller one was 15.2 cm in diameter
and 6.2 m tall. A comparison between the measured solids
mass flux profile in the hlly developed zone of the larger riser
and the profile predicted by our model for the case of an inlet
solids mass flux of 60 kg/m2.s is shown in Figure 2. For the
smaller riser operating with an inlet solids mass flux of
11 1 kg/m2.s, the measured data and predicted profile are
shown in Figure 3. The comparison in each case is reasonable.

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997 32 I

 2.5 7 1

2.0

1.5
G \ 4. t ' .
\

\ II
1 .o
\

3-
2
2
0.5
v)

5 0.0
-
a VI

$ -0.5
T 0

3 -l.O
-1.5
I
- Predicted G./G.,

-2.0
I I
-2.5 1 I
-4
-1.0 -0.5 0.0 0.5 1 .o -1 .o -0.5 0.0 0.5 I.o
Reduced Radius, r / R Reduced Radius, r / R
Figure 3 - Comparison between the predicted (a = 4.20, b = Figure 4 -Comparison between the predicted (c = 8.95, d = 3.15)
-2.00) and measured solids mass flux profile. [Data of Rhodes and measured solids velocity profile at 4.18 rn. [Data of Miller and
et al. ( 1 992); Dp = 74.9 pn, p, = 2456 kg/m3, D = 0. I52 rn,L = Gidaspow (1992); Dp= 75 pn, p, = 1654 kg/m3, R = 3.75 cm. L =
6.2 rn, G,T= 1 1 1 kg/m2.s,us0 = 5 d s ] . 6.58 m. G, = 32.8 kg/m2.s, uno = 2.89 d s ] .

The data in Figure 3 could have been matched more pre-
cisely if a higher value of m was chosen. A value of m = 7
would have flattened the predicted profile even more at the
centerline. Similarly, the data in Figure 2 could have been
matched more precisely if a lower value of m was chosen.
The set value of m = 5 in our model is a good compromise
for matching the two cases and maintains consistency with
the findings of Rhodes et al. ( 1 992).
Miller and Gidaspow ( 1 992) measured both the solids
mass flux and interparticle voidage profiles in a 7.5 cm
diameter riser circulating 75 pn FCC catalyst. the measure-
ments were made at three different axial locations of 1.86,
4.18 and 5.52 m in their 6.58 m tall riser. The calculated
solids velocity profiles show that only the 4.18 m sampling
location was in the fully developed zone of the riser. The
lowest sampling location was influenced by the acceleration
zone while the highest sampling location was subject to exit
effects. Figure 4 shows a comparison of the solids velocity
profile predicted by our model and the experimental data at
4.18 m. The data show some skewedness which could be a
consequence of non-uniform injection of solids at the base of
the riser. It also demonstrates that it is imperative to traverse
the entire column when taking profile samples. The match
between the data and the predicted profile is quite good.
Industrially, large solids mass fluxes are employed and
are of interest to this study. Pugsley (1995) measured the
interparticle voidage profile using a capacitance probe in a
CFB with a solids mass flux of 240 kg/m2.s. The particles in
his riser were silica sand with a mean diameter of 208 pn
and a density of 2580 kg/m3. Our model predicts an average
voidage in the core of 0.86 and 0.68 in the annulus. Figure
5 shows the predicted values of the voidage are good at the
centerline and at the wall. The deviation between the data
and predicted values elsewhere could be a consequence of
skewing similar to that shown in Figure 4.
CFB RISER REACTOR - THEEFFECTS OF
CLAUS BACKMIXING
In order to demonstrate the effects of backmixing in a CFB
operating in the fast fluidization regime, a simulation was
performed on a single reactor with the main Claus reaction:
Note that this is a fast, reversible reaction. Operating con-
ditions (Table 3) and other relevant details (Table 4) of the
Claus reactor simulation are given in the Appendix. Bi et al.
(1995) define the critical velocity as the velocity at which
the transition from the turbulent regime to the fast fluidiza-
tion regime occurs. For the system under consideration, the
critical velocity is 1.7 d s . The choking velocity, the veloc-
ity at which the transition from the fast fluidized regime to
the pneumatic transport regime occurs, is 10.6 m / s (Bi et al.,
1993). The inlet gas superficial velocity was set at 6 m/s to
ensure operation of the CFB in the fast fluidization regime.
The calculated parameters for our model applied to the
Claus simulation are shown in Table 5. The concentration
profiles of the reactants and products generated by our
model and the plug flow model can be seen in Figures 6
through 9. As expected, the effect of backmixing was a
decrease in conversion; the H,S flow at the outlet of the
reactor for the PFR model was 5.9% lower than the outlet
flow for our model. That difference in conversion may not

322 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1YY7
 1 .oo TABLE 5
Calculated Hydrodynamic Parameters for Our Fast Fluidized
CFB Model for The Simulation of a Claw Riser Reaction with an
0.95 Inlet Feed Given in Table 3 (Main Claw Reaction)
4 4 u , [kg/m2.s]
~ 2.25 1
0.90 b [kg/rn2.s] -0.608
c [ds] 9.736
W
d [dsl -1.151
$ 0.85
k* [ d s l 0.032
3
9 ' c [ml 0.492
2
0
0.80 ugo [ d s l -0.396
.-
5 ugc [ d s l 8. I40
5C
c3
0.75 usa [ d s l -0.576
us<.[m/sI 4.292
0.70 'a 0.702
E, 0.840
\
0.65
14.5 7

y
1
0.60
I
I
I
I I
-1.0 -0.5 0.0 0.5 1.o 1 Annulus7
Reduced Radius, r / R
Figure 5 - Comparison between the predicted and measured
voidage profile at 2.5 m.[Data of Pugsley (1995); D = 208 p,p,
= 2580 kg/m3, R = 2.5 cm, L = 6.4 m, G, = 240 Rg/m2.s, ugo =
5ds].
' Core

TABLE 3 P
Claw Riser Reactor Feed Stream Properties Used to Demonstrate
the Effects of Backmixing in a Fast Fluidized CFB u80 13.0 /,/
( P =216.0 kPa. T = 539 K1
Molar Flow [mol/s]
1.48
9,
X

--
28.1 1 12.5
0.86
0.98
4.1 1
66.97 12.0
14.83
0 2 4 6 8 lo
Axial Position, z [m]
135.00
Figure 6 -Model predictions of axial H,O concentration profiles
0.0 1
for fast fluidized and plug flow reactors in a Claus plant (only the
8.73 main Claw reaction).

TABLE 4 be significant for many processes but, for the Claus process,
Riser Reactor and Kaiser-201 Catalyst Properties for The a decrease of that magnitude could be disastrous.
Simulation of a Claw Riser Reactor with an Inlet Feed Given in Note in the schematic representation of our model pre-
Table 3 sented in Figure 1, the gas and solids are introduced into the
Reactor Radius [rn] 0.536 annulus at the top of the reactor. Following the H,O con-
Reactor Height Iml 10 centration profile (Figure 6) in the annulus from fhe fop qf
the reactor to the bottom, it can be seen that concentration
rises quickly at first. The sharp rise is due to the increased
reaction rate in the annulus brought on by the relatively
higher suspension density in the annulus compared to the
core. In the upper portion of the reactor, the concentration
gradient between the core and annulus is small and the gen-
eration of water is greater than the flux leaving the annulus.

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997 323
 1.8

1.6

-
,-€ 1.4
k
v;
g 1.2
.-
U
(d
b
1.0
3
2 0.8 _ _
0.6 __

Annulus --.... -.
. ~. ...
0.2s 5 0.4
0 2
I
I

4
I

6
I

8
I

10
0 2 4 b 8 10
Axial Position, z [m] Axial Position, z [m]
Figure 7 -Model predictions of axial H,S concentration profiles Figure 9 - Model predictions of axial SO, concentration profiles
for fast fluidized and plug flow reactors in a Claw plant (only the for fast fluidized and plug flow reactors in a Claus plant (only the
main Claus reaction). main Claus reaction).

the generation of H,O in the annulus due to the large con-

.-.. centration gradient between the two regions. That results in
__--- the H,O concentration decreasing.
Interestingly, Figure 8 shows that at the axial location of
approximately z = 5 m to z = 6 m. the sulphur concentration
in the annulus is constant which indicates that the generation
of sulphur in the annulus is exactly equal to the transfer of
sulphur to the core. This “equilibrium” is destroyed when
the concentration gradient between the core and annulus is
either very large or small.
The concentration profiles of the reactants, H,S and SO,,
in the annulus are similar to the products but have an oppo-
site sign. That is, rather than being quickly generated at the
top of the reactor, the reactants are quickly consumed.
The reduction in conversion due to backmixing is less
pronounced than was anticipated. The backmixing effect in
a CFB operating in the fast fluidized regime is offset by the
densification of the suspension in the core due to the inter-
nal circulation of the solids from the annulus to the core.
Had the gas flow in the annulus been greater, it would have
caused the solids fraction in the core to decrease and the
backmixing effect would have been greater.
I I I 1
Conclusions
0 2 4 6 8 10
Axial Position, z [m] The practical model developed in this paper was able to
adequately represent the solids mass flux and velocity pro-
Figure 8 -Model predictions of axial S, concentration profiles for files in a CFB operating in the fast fluidized regime. The
fast fluidized and plug flow reactors in a Claw plant (only the main downflow of gas and solids in the annulus, incorporated in
Claus reaction). our model, caused the average solids fraction in the fully
developed zone to be altered significantly from the “plug
Therefore, the concentration in the annulus continues to flow” solids fraction. Additionally, the effect of the back-
increase. In the lower portion of the reactor the mass trans- mixing of the gas was found to decrease conversion in a
fer between the core and annulus becomes dominant over riser reactor for the fast, main Claus reaction.

324 THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997
Acknowledgments Subscripts
We would like to acknowledge the Natural Sciences and 0 = inlet or superficial
Engineering Research Council of Canada for their generous sup- a =annulus
port. DMJP would also like to thank the Alberta Natural Gas c = core or number of components
Company Ltd. for the John S. Poyen Scholarship. i = component index
j = reaction index
Appendix g =gas
pf = plug flow
The details pertaining to the CFB riser reactor used to demon-
r = number of reactions
strate the effects of backmixing are derived from a modified Claus
s = solids
plant being fed 200 tonnes per day of sulphur (Puchyr. 1997). Table
t = terminal velocity
3 gives the inlet gas composition, pressure, and temperature while
the riser reactor and catalyst characteristics are presented in Table 4.
The intrinsic rate expression for the main Claw reaction, References
Reaction 15, on the Kaiser 201 catalyst is given by the Liu I1
Model (Birkholz, 1987): Bermti, F., J. Chaouki, L. Godfroy, T. S. Pugsley and G. S.
Patience, “Hydrodynamics of Circulating Fluidized Bed Risers:

[-T-O)x
- r i 2 s = 1.663 x lo4 exp -
A Review”. Can. J. Chem. Eng. 73.579-602 ( 1995).
Bi, H. T., J. R. Grace and J. X. Zhu, “Regime Transitions Affecting
GasSolids Suspensions and Fluidized Beds”, Trans. Inst.
Chem. Eng. 73. 154-161 (1995).

..(.,)-
p ~0.1875 Bi, H. T., J. R. Grace and J. X. Zhu, “Types of Choking in Vertical
H 2 0 S, Transport Reactors”, Int. J. Multiphase Flow 19, 1077-1092
y0.5
‘1 ......... ( 1993).
Birkholz, R. K. O., L. A. Behie and I. G. Dalla Lana, “Kinetic
1 + 1.125 x lo4 -2510 Modelling of a Fluidized Bed Claus Plant”, Can. J. Chem. Eng.
65, 778-784 (1 987).
Bodelin, P., Y. Molodtsof and A. Delebarre, “Flow Structure
Investigations in a CFB”, in “Circulating Fluidized Bed
where Technology IV”, A. Avidan, Ed., American Institute of
Chemical Engineers, New York ( I 994), pp. 118-122.
Brereton, C. M. H., J. R. Grace and J. Yu, “Axial Gas Mixing in a
Circulating Fluidized Bed”, in “Circulating Fluidized Bed
Technology II”, P. Basu and J. F. Large, Eds., Permagon Press,
New York (1 988), pp. 307-3 14.
evaluated at equilibrium. Note that -ri2s has units of mol/s.kg cat. Chehbouni, A,, J. Chaouki, C. Guy and D. Klvana,
The results of our calculations that give the hydrodynamics “Characterization of the Flow Transition Between Bubbling and
within the riser are presented in Table 5. Turbulent Fluidization”, Ind. Eng. chem. Res. 33, 1889-1 896
( 1994).
Nomenclature Contractor, R. M., G. S. Patience, D. I. Gamett, H. S. Horowitz,
G. M. Sisler and H. E. Bergna, “A New Process for n-Butane
a = parameter for our new model (Equation 3) [kg/m2.s] Oxidation to Maleic Anhydride Using a Circulating Fluidized
A = cross sectional area [m2] Bed Reactor”, in “Circulating Fluidized Bed Technology IV”,
b = parameter for our new model (Equation 3) [ks/m2.s] A. A. Avidan, Ed., American Institute of Chemical Engineers,
c = parameter for our new model (Equation 4) [ d s ] New York (1994), pp. 387-389.
d = parameter for our new model (Equation 4) [ d s ] Grace, J. R., “Contacting Modes and Behaviour Classification of
D = riser diameter [m] Gas-Solids and Other Two-Phase Systems”, Can. J. Chem. Eng.
D = catalyst pellet diameter [m] 64,353-36 1 (1986).
Fp = molar flow rate [ m o ~ s ] Hartge, E. U., D. Rensner and J. Werther, “Solids Concentration
G = mass flux [kg/m2.s] and Velocity in Circulating Fluidized Beds”, in “Circulating
k = cross-flow coefficient [ d s ] Fluidized Bed Technology II”, P. Basu and J. F. Large, Eds.,
f = reactor length [m]
Permagon Press, New York (1988), pp. 165-1 80.
rn = constant in Equation (3) Higbie, R., “The Rate of Absorption of a Pure Gas into a Still
m = mass flow rate [kg/s] Liquid During Short Periods of Exposure”, Trans. Amer. Inst.
P = pressure [Pa]
Chem. Eng. 31,365-389 (1935).
r = radial co-ordinate [m] or reaction rate [mol/m3.s]
Kruse, M., H. Schoenfelder and J. Werther, “A Two-Dimensional
r’ = rate of reactionj [mol/s.kg cat]
Model for Gas Mixing in the Upper Dilute Zone of a Circulating
d = riser radius [m] Fluidized Bed Reactor”, Can. J. Chem. Eng. 73, 620-634
Re = Reynolds number
(1995).
R = universal gas constant [J/mol.K] Louge, M. and H. Chang, “Pressure and Voidage Gradients in
f = temperature [K]
Vertical GasSolid Risers”, Powder Technol. 60, 197-201
u = velocity [ d s ]
(1990).
y = mole fraction
z = axial position in the riser [m]
Miller, A. and D. Gidaspow, “Dense, Vertical Gas-Solid Flow in
a Pipe”, AIChE J. 38, 1801-1 845 (1 992).
Greek letters Ouyang, S., X. G. Li and 0. E. Potter, “Investigation of Ozone
Decomposition in a Circulating Fluidized Bed on the Basis of a
E = interparticle voidage Core-Annulus Model”, in “Fluidization VIII Preprints”, Tours,
v = stoichiornetric coefficient France (1 995), pp. 457-466.
p = density [kg/m3] Patience, G. S. and J. Chaouki, “Gas Phase Hydrodynamics in the
0 = fraction of the riser cross-sectional area occupied by the core Riser of a Circulating Fluidized Bed”, Chem. Eng. Sci. 48,
= slip factor ( u ~ J E uSa)
, 3195-3205 (1993).

THE CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997 325
 Patience, G . S. and J. Chaouki, “Solids Hydrodynamics in the
Fully Developed Region of CFB Risers”, in “Fluidization VIII
Preprints”, Tours, France (1995) pp. 33-40.
Patience, G . S., J. Chaouki, F. Bermti and R. Wong, “Scaling
Considerations for Circulating Fluidized Bed Risers”, Powder
Technol. 72,31-37 (1992).
Puchyr, D. M. J., “Modelling and Optimization of a Claus Plant
Using Circulating Fluidized Bed Technology”, Ph.D.
Dissertation, The University of Calgary, Calgary, AB (1997, in
progress).
Pugsley, T. S., “Modelling the Catalytic Oxidation of n-Butane to
Maleic Anhydride in a Circulating Fluidized Bed Reactor”,
M.Sc. Thesis, The University of Calgary, Calgary, AB (1992).
Pugsley, T. S., “The Hydrodynamics of Circulating Fluidized
Beds”, Ph.D. Dissertation, The University of Calgary, Calgary,
AB ( 1 995).
Pugsley, T. S., G. S. Patience, F. Bermti and J. Chaouki,
“Modeling the Catalytic Oxidation of n-Butane to Maleic
Anhydride in a Circulating Fluidized Bed Reactor”, Ind. Eng.
Chem. Res. 31, 2652-2660 (1992).
Rhodes, M. J., X. S. Wang, T. Hirama and B. M. Gibbs, “Similar
Profiles of Solids Flux in Circulating Fluidized-Bed Risers”,
Chem. Eng. Sci. 47, 1635-1643 (1992).
326 T H E CANADIAN JOURNAL OF CHEMICAL ENGINEERING, VOLUME 75, APRIL, 1997
Soong, C. H., K. Tuzla and J. C. Chen, “Experimental
Determination of Cluster Size and Velocity in Circulating
Fluidized Bed”, in “Fluidization VIlI Preprints”, Tours, France
(1995) pp. 1-8.
van der Ham, A. G . , W. Prins and W. van Swaaij, “A Small-Scale
Regularly Packed Circulating Fluidized Bed Part 11: Mass
Transfer”, Powder Technol. 79, 29-42 (1 994).
Werther, J., “Fluid Mechanics of Large-Scale Units”, in
“Circulating Fluidized Bed Technology IV”, A. Avidan, Ed.,
American Institute of Chemical Engineers, New York ( 1994),
pp. 1-14.
Zhang, W., Y . Tung and F. Johnsson, “Radial Voidage Profiles in
Fast Fluidized Beds of Different Diameters”, Chem. Eng. Sci.
46,3045-3052 (1991).
Manuscript received March 2 I , 1996; revised manuscript
received November 22, 1996; accepted for publication December
10, 1996.