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Fluidized Bed Reactor Technology
Fluidized Bed Reactor Technology
Fluidized-Bed Reactors
Joachim Werther, Hamburg University of Technology, Hamburg, Germany
Related Articles For other industrial reactors and their applications, see Stirred-Tank and Loop Reactors,
Tubular Reactors, Fixed-Bed Reactors, Bubble Columns, Three-Phase Trickle-Bed Reactors,
Reaction Columns, Thin-Film Reactors, Metallurgical Furnaces, and Biochemical Engineering.
Introduction . . . . . . . . . . . . . . .
The Fluidization Principle . . . . . .
Forms of Fluidized Beds . . . . . . .
Advantages and Disadvantages of
the Fluidized-Bed Reactor . . . . . .
2.
Fluid-Mechanical Principles . . . . .
2.1.
Minimum Fluidization Velocity . . .
2.2.
Expansion of LiquidSolid
Fluidized Beds . . . . . . . . . . . . . .
2.3.
Fluidization Properties of Typical
Bed Solids . . . . . . . . . . . . . . . . .
2.4.
State Diagram of Fluidized Bed . . .
2.5.
Gas Distribution . . . . . . . . . . . . .
2.6.
Gas Jets in Fluidized Beds . . . . . .
2.7.
Bubble Development . . . . . . . . . .
2.8.
Elutriation . . . . . . . . . . . . . . . .
2.9.
Circulating Fluidized Beds . . . . . .
2.9.1. Hydrodynamic Principles . . . . . . . .
2.9.2. Local Flow Structure in Circulating
Fluidized Beds . . . . . . . . . . . . . .
2.9.3. Design of Solids Recycle System . . .
2.10. Cocurrent Downow Circulating
Fluidized Beds (Downers) . . . . . .
2.11. Attrition of Solids . . . . . . . . . . . .
3.
Solids Mixing in Fluidized-Bed
Reactors . . . . . . . . . . . . . . . . . .
3.1.
Mechanisms of Solids Mixing . . . .
3.2.
Vertical Mixing of Solids . . . . . . .
3.3.
Horizontal Mixing of Solids . . . . .
3.4.
Solids Residence-Time Properties .
3.5.
Solids Mixing in Circulating
Fluidized Beds . . . . . . . . . . . . . .
1.
1.1.
1.2.
1.3.
3
3
3
4.
4
5
5
4.2.
6.
7.
6
7
8
10
10
12
13
13
15
16
16
17
20
20
21
22
22
22
The article gives an overview on fundamentals and applications of uidized-bed technology. Some basic uid-mechanical principles
minimum uidization velocity, status diagram,
gas distribution, bubble development, and solids
entrainment and elutriationare presented at
the beginning, followed by a detailed discussion of circulating uidized beds, downers,
and attrition effects in uidized-bed systems.
Sections on solids mixing, gas mixing, and
c 2007 Wiley-VCH Verlag GmbH & Co. KGaA, Weinheim
10.1002/14356007.b04 239.pub2
4.1.
5.
8.
8.1.
8.2.
8.3.
8.4.
8.5.
9.
9.1.
9.2.
9.2.1.
9.2.2.
9.3.
9.3.1.
9.3.2.
10.
11.
23
23
23
24
25
26
26
27
29
30
30
36
37
37
37
37
38
40
40
41
42
43
heat and mass transfer in uidized beds complete the fundamentals section, which is followed by an overview on industrial applications.
Fluidized-bed processes for heterogeneous catalytic gas-phase reactions, for the polymerization of olens, for homogenous gas-phase reactions, gassolid reactions and applications in
biotechnology are described in detail. A nal
chapter is devoted to the modeling of uidizedbed reactors.
2
a
A0
Ar
At
b
cv
cb
cc
cj
Cb
Cd
do
dp
d pi
dt
dv
dv 0
D
Dsh
Dsv
Fr p
Gs
h
ho
hgs
hwb
H
H mf
kG
L
m. a
matt
mb
Fluidized-Bed Reactors
Symbols
volume-specic mass-transfer area between bubble and suspension phases,
m1
cross-sectional area of orice, m2
Archimedes number, dened by Equation (5)
cross-sectional area of reactor, m2
parameter def. by Equation (54)
solids volume concentration
bubble attrition rate constant, dened
by Equation (50), s2 /m4
cyclone attrition rate constant dened
by Equation (51), s2 /m3
jet attrition rate constant, dened by
Equation (52),s2 /m3
concentration in bubble phase,
kmol/m3
concentration in suspension phase,
kmol/m3
orice diameter, m
Sauter diameter, dened by Equation
(6), m
diameter of particle size class i, m
bed diameter, m
local bubble volume equivalent sphere
diameter, m
initial bubble diameter, m
coefcient of molecular diffusion, m2 /s
lateral solids dispersion coefcient,
m2 /s
vertical solids dispersion coefcient,
m2 /s
Froude number, dened by Equation
(29)
solids mass ow rate, based on reactor
cross-sectional area, kg m2 s1
height above distributor level, m
height above distributor where bubbles
are forming, m
gas-to-solid heat transfer coefcient, W
m2 K1
wall-to-bed heat transfer coefcient, W
m2 K
expanded bed height, m
bed height at minimum uidization, m
mass-transfer coefcient, m/s
jet length, m
mass of elutriated solids, kg
mass ow due to attrition, kg/s
bed mass, kg
ms
np
p
Per, c
Q3
ra
rj
Re
Sv
t
TDH
u
ub
uc
umf
uo
usl
u.t
Vb
.
V. mf
Vo
xi
pd
b
i
mf
*
ij
f
s
Fluidized-Bed Reactors
1. Introduction
1.1. The Fluidization Principle
In uidization an initially stationary bed of solid
particles is brought to a uidized state by an
upward stream of gas or liquid as soon as the
volume ow rate
. of the uid exceeds a certain
limiting value V mf (where mf denotes minimum
uidization). In the uidized bed, the particles
are held suspended by the uid stream; the pressure drop pfb of the uid on passing through
the uidized bed is equal to the weight of the
solids minus the buoyancy, divided by the crosssectional area At of the uidized-bed vessel (Fig.
1):
pfb =
At H (1) (s f ) g
At
(1)
As the volume
ow rate V or the supercial ve.
locity u = V /At of the uid increases beyond
Fluidized-Bed Reactors
the value V mf or umf (Fig. 2 A) corresponding to the minimum uidization point, one of
two things happens: in uidization with a liquid, the bed begins to expand uniformly; in uidization with a gasa process of greater industrial importance and the one discussed almost
exclusively in the following materialvirtually
solids-free gas bubbles begin to form (Fig. 2 B).
The local mean bubble size increases rapidly
with increasing height above the grid because
of coalescence of the bubbles. If the bed vessel is sufciently narrow and high, the bubbles
ultimately ll the entire cross section and pass
through the bed as a series of gas slugs (Fig. 2
C). As the gas velocity increases further, more
and more solids are carried out of the bed, the
original, sharply dened surface of the bed disappears, and the solids concentration comes to
decrease continuously with increasing height.
To achieve steady-state operation of such a turbulent uidized bed (Fig. 2 D), solids entrained
in the uidizing gas must be collected and returned to the bed. The simplest way to do this
is with a cyclone integrated into the bed vessel
and a standpipe dipping into the bed. A further
increase in gas velocity nally leads to the circulating uidized bed (Fig. 2 E), which is characterized by a much lower average solids concentration than the previous systems. The high
solids entrainment requires an efcient external
Fluidized-Bed Reactors
3) In catalytic reactions, undesired bypass or
broadening of residence-time distribution for
reaction gas due to bubble development
4) Erosion of internals and attrition of solids (especially signicant with catalysts), resulting
from high solids velocities
5) Possibility of deuidization due to agglomeration of solids
6) Gassolid countercurrent motion possible
only in multistage equipment
7) Difculty in scaling-up
Table 1 compares the uidized-bed reactor with alternative gassolid reaction systems:
xed-bed, moving-bed, and entrained-ow reactors.
Table 1. Comparison of gassolid reaction systems [2, 18]
2. Fluid-Mechanical Principles
2.1. Minimum Fluidization Velocity
The minimum uidization point, which marks
the boundary between the xed- and the
uidized-bed conditions, can be determined by
measuring the pressure drop p across
the bed
.
as a function of volume ow rate V (Fig. 1).
Measurement should always be performed with
decreasing gas velocity, by starting in the uidized condition.
Only for very narrow particle-size distributions, however, does a sharply dened minimum
uidization point occur. The broad size distributions commonly encountered in practice exhibit
Fluidized-Bed Reactors
it follows
umf = 7.14 (1mf ) Sv
1+0.067
3
( )g
mf
s 2f S13 1
(1mf )2
f
v
(2)
= 33.7
1+3.6105 Ar1
(3)
where
umf dp
(4)
gd3p s f
f
2
(5)
Remf =
Ar =
Here the surface mean or Sauter diameter calculated from the massdensity distribution q3 (d)
of the particle diameters
dp =
1
dmax
dmin
d1 q
(6)
(d) d (d)
(7)
4.65
4.4Re0.03
t
n=
0.1
4.4Ret
2.4
0<Ret 0.2
0.2<Ret 1
1<Ret 500
500<Ret
(8)
ut dp
(9)
Fluidized-Bed Reactors
The parameters employed are those crucial for
uidization properties: the mean particle diameter (d p ) and the density difference (s f ) between solid and uid. Figure 3 shows the Geldart
diagram with the interclass boundaries theoretically established by Molerus [35].
Solids of group C are very ne-grained, cohesive powders (e.g., our, nes from cyclones
and electrostatic lters) that virtually cannot be
uidized without uidization aids. The adhesion
forces between particles are stronger than the
forces that the uid can exert on the particles.
Gas ow through the bed forms channels extending from the grid to the top of the bed, and
the pressure drop across the bed is lower than
the value from Equation (1). Fluidization properties can be improved by the use of mechanical equipment (agitators, vibrators) or owability additives, e.g., Aerosil.
Solids of group A have small particle diameters (ca. 0.1 mm) or low bulk densities;
this class includes catalysts used e.g., in the
uidized-bed catalytic cracker. As the gas velocity u increases beyond the minimum uidization
point, the bed of such a solid rst expands uniformly until bubble formation sets in at u = umb
> umf . The bubbles grow by coalescence but
break up again after passing a certain size. At
a considerable height above the gas distributor
grid, a dynamic equilibrium is formed between
bubble growth and breakup. If the gas ow is
cut off abruptly, the gas storage capacity of the
4 gdp (s f )
Ar =
gd3p (s f )
2
f
(10)
8
M =
Fluidized-Bed Reactors
f
u3
g (s f )
(11)
o
CD u2o
2
V = No Ao uo
either the number of nozzles N o or the crosssectional area of the individual nozzle. Ao can be
calculated for a given gas ow rate V .
Problems related to the design of gas distributors are attrition of solids (see Section 2.11),
erosion, and back-ow of solids. Erosion may
occur at the distributor plate and at neighboring
Fluidized-Bed Reactors
Figure 5. Rehs uidized-bed state diagram with operating regions of different reaction systems
a) Circulating uidized bed; b) Fluidized-bed roaster; c) Bubbling uidized bed; d) Shaft furnace; e) Moving bed
10
Fluidized-Bed Reactors
f do
s dp
0.3
2
0.2
uo
1.3
1
gdo
(12)
0.4
u2
f 0.2
= 5.25 (1)o og d
s
s
p
0.2
d
dp
4.5
L
do
(13)
Fluidized-Bed Reactors
velocity ub to the interstitial velocity of the gas
in the suspension surrounding the bubble:
ub
=
umf/ mf
(14)
dv0
=
m
1/3
0.008b
. 2
0.2
1.3 Vgo
porous plate
(17)
.
V b 0.8 (uumf )
The case > 1 is typical for solids of Geldart groups A and B. The gas rising in the bubble
ows downward again in a thin layer of suspension (cloud) surrounding the bubble. An
important point for heterogeneous catalytic gasphase reactions is that the presence of a boundary between bubble gas and suspension gas leads
to the existence of two distinct phases (bubble
phase and suspension phase) with drastically different gassolid contact.
If < 1, some of the gas in the suspension
phase undergoes short-circuit ow through the
bubble, while only part of the bubble gas recirculates through the suspension. This type of ow
is typical for uidized beds of coarse particles
(Geldart group D).
Under the real operating conditions of a
uidized-bed reactor, a number of interacting
bubbles occur in the interior of the uidized bed.
As a rule, the interaction leads to coalescence.
As detailed studies have shown, this process is
quite different from that between gas bubbles in
liquids because of the absence of surface-tension
effects in the uidized bed [48, 49].
For predicting mean bubble sizes in freely
bubbling uidized beds, a differential equation
for bubble growth should be used in the case of
Geldart group A and B solids [50]:
2b
9
(16)
b = V b /ub
d
dv =
dh
11
1
3
dv
3 ub
(15)
(18)
ub =V b +0.71b
b =
gdv
(19)
(20)
umf
g
(21)
12
Fluidized-Bed Reactors
the size d v of bubbles bursting at the bed surface
[56]:
T DH = 18.2dv
(22)
2.8. Elutriation
When bubbles burst at the surface of the uidized
bed, solid material carried along in their wake is
ejected into the freeboard space above the bed.
The solids are classied in the freeboard; particles whose settling velocity ut is greater than
the gas velocity fall back into the bed, whereas
particles with ut < u are elutriated by the gas
stream. As a result, both the volume concentration of solids cv and the mass ow rate of entrained solids in the freeboard show a characteristic exponential decay (Fig. 9). With increasing
height above the bed surface, the transport disengaging height (TDH) is nally reached. Here
the increased local gas velocities due to bubble eruptions have decayed, and the gas stream
contains only particles with ut < u. When the
TDH can be reached in a uidized-bed reactor,
this is associated with minimum entrained mass
ow rates and solids concentrations, and hence
with minimum loading on downstream dust collection equipment. Design of the dust collection system requires knowledge of the entrained
mass ow rate Gs and the particle-size distribution of the entrained solids. For the design
of the uidized-bed reactor, the distribution cv
(h) of the solids volume concentration and, for
gassolid reactions, the local particle-size distribution as a function of height in the freeboard
must be known.
For solids of Geldart group A, the TDH can
be estimated with the diagram shown in Figure
10 [55]. The following relation is given for the
TDH of Geldart group B solids as a function of
Fluidized-Bed Reactors
Gs =
i
xi i
(23)
u (Gs /s )
13
(24)
p
(s f ) (1mf ) g h
(25)
u
(s f )
gdp
f
(26)
(27)
14
Fluidized-Bed Reactors
(28)
increasing Fr p ). With increasing Fr p the volume ow ratio increases; that is, relatively more
solids are elutriated (and thus circulated).
If Fr p is allowed to drop below the limit
F rpmax (Fig. 13 B, Fig. 12) two steady-state
sections appear in the riser tube: the one in the
lower part is marked by a high pressure gradient, that in the upper part by a lower gradient.
Figure 13 illustrates the physical signicance
of these two pressure gradients. In practice, the
transition between the two linear regions takes
place gradually. The height of the transition zone
corresponds to the transport disengaging height
(TDH).
The picture changes further if the gas velocity
declines to values lower than the settling velocity
ut of a single isolated particle. In this case (for
Fr p < Fr pt , Fig. 13 A, Fig. 12), no more solids
can be elutriated, and the pressure gradient in the
upper linear region vanishes. All the solid material is now in the form of a bubbling or turbulent
uidized bed.
The solids concentrations averaged over the
tube cross section (1 ) can be calculated from
the dimensionless pressure drop:
1 = (1mf )
(29)
Figure 13. Pressure prole in the circulating uidized bed with siphon, according to Wirth [64]
A) F rpumf <F rp <F rpt ; B) F rpt <F rpmax ; C) F rp >F rpmax
Fluidized-Bed Reactors
present in the bed vessel (i.e., F rpumf < Fr p
< Fr pT ), the mass ow rate of entrained solids
depends on the physics of the gassolid ow.
Figure 14 plots the dimensionless solids mass
ow rate versus Fr p , with the Archimedes number as parameter. For a given Ar, the ow rate
tends to zero as Fr p Fr pt and reaches a maximum at Fr p = Fr pT . The slope of the elutriation
curve becomes greater with increasing Ar; that
is, the coarser the particles, the greater is the relative change in the circulating mass ow rate of
solids with a change in gas velocity.
At high gas velocities in the circulating uidized bed (i.e., when a single steady-state section exists), the entrained mass ow rate depends
on the particle Froude number and the solids
holdup. More detailed information about the application of Wirths theory in practice may be
found in [11].
Whereas Wirths analysis of the circulating
uidized bed starts from the pneumatic transport
condition, the models of Rhodes and Geldart
[66], as well as Kunii and Levenspiel [2, 58],
are based on the bubbling uidized bed and describe the circulating uidized bed as a limiting
15
16
Fluidized-Bed Reactors
tential. Least resistance means that the volumespecic energy consumption for suspending and
transporting solids is minimized, and minimization of the gravitational potential is equivalent
to the requirement that the local mean voidage
attains a minimum. The model has been applied as a description of uid-mechanical phenomena in CFB risers of different sizes [74, 75]
but also for the prediction of ow patterns of
gas and solids in industrial-scale units, such as a
CFB boiler [76] and a petrochemical processing
unit [77]. Another promising line of development is the introduction of the EMMS concept
into computational uid dynamical calculations
of multiphase ows; rst results obtained with
a drag model based on the EMMS model are
encouraging [78].
Fluidized-Bed Reactors
17
Figure 17. Pressure distribution in solids recycle system of a circulating uidized bed
a) Fluidized bed; b) Return leg
[83], and solids mixing [84, 85] have been investigated both experimentally and by numerical
simulation [86]. It has been found that the hydrodynamics of the downer are also characterized
by a wall zone of increased solids concentration. However, axial and radial gas-solids ow
structures are much more uniform than in conventional uidized beds. Another result is that
the length of the ow development zone is much
shorter for the downer than for the riser, which
means that reactions with very short contact
times can be carried out under near-plug-ow
conditions. However, the solids feeding process
and the geometry of the entrance region are critical points that deserve special attention [87].
The patent and open literature suggest various applications for downer reactors, e.g., residual oil cracking [88], coal pyrolysis [89], and
biomass pyrolysis [90]. The catalytic pyrolysis
of heavy feeds for the production of light olens
has been investigated on the laboratory scale
with promising results [88]. However, no largescale industrial process has emerged yet.
The attrition of solid particles is an unavoidable consequence of the intensive solids motion in the uidized bed. The attrition problem is especially critical in processes where the
18
Fluidized-Bed Reactors
1 ma
mb t
(30)
Fluidized-Bed Reactors
Under steady-state conditions the jetattrition-related mass production of nes per
unit time for a gas distributor with a number no
of orices from mother particles with diameter
d p,i which are present in the catalyst inventory
with a mass fraction Q3i is proportional to the
particle size d pi , the mass fraction Q3i , the
density o of the gas issuing from the orice,
the square of the orice diameter d o , and to the
cube of the jet exit velocity uo [97, 98]:
(31)
(32)
tj
t
/t for in bed attrition
=
19
(35)
where the denition of the characteristic parameters t j , t b , and np can be taken from Figure
21, np is the number of passages of a given particle through the cyclone, and t b and t j are the
time periods during which the particle is subjected to bubble and jet stress, respectively. If it
is assumed that the effects of the different stress
mechanisms on the catalyst particles are additive, a uniform treatment of the overall stress
history for all three attrition mechanisms is given
by
matt ()
matt,
1.1b
1/
b
1/
b
>1.1
1.1
(36)
(33)
c =
mc
c uc Ac
(34)
20
Fluidized-Bed Reactors
are shed at irregular intervals during bubble motion, and new portions of solids are taken into the
wake (Fig. 23 B). Solids transport in the wake is
essentially the reason that vertical solids mixing
is from one to two orders of magnitude better
than horizontal mixing.
For reasons of continuity, the upward transport of particles by bubbles is coupled with a
downward movement in the suspension phase
that surrounds the bubbles. Measurements of the
local bubble-gas ow have shown that the rising bubbles are not distributed evenly over the
bed cross section. As a typical example, Figure
24 A gives a plot of the radial distribution of
the bubble-gas ow at three heights above the
grid in a uidized bed 1 m in diameter. The prole is comparatively at in the bottom zone but
exhibits a steeper slope as the height increases,
with an annular zone of preferentially rising bubbles. The resulting circulation of the solids also
features an annular region of upward transport
in the wakes with predominantly downward motion of the solids in the center and at the periphery of the bed (Fig. 24 B).
The large-scale solids circulation can be reinforced by uneven distribution of the uidized gas
over the distributor cross section [106]. Figure
25 presents examples of industrial uidized-bed
furnaces in which forced circulation of the solids
is employed to improve coal burnup.
Fluidized-Bed Reactors
21
Dsv
m2 /s
= 0.06+0.1
u
m/s
(37)
Dsv
m2 /s
= 0.056
uumf
m/s
(38)
22
Dsv
m2 /s
Fluidized-Bed Reactors
= 0.030
dt
m
0.65
(39)
1
H
H
0
1b
gd3v dh (40)
mb
.
ms
(41)
The mass fraction dms /mb of solids having a residence time between t and t + dt is
t
dms
1
= e dt
mb
(42)
Similarly, the fraction f of solids having a residence time less than t in the bed is calculated
as
f = 1et/
(43)
Fluidized-Bed Reactors
2.9. Different regions can be discriminated with
respect to the prevailing mechanisms of solids
motion and mixing. An extensive survey on experimental ndings in solids mixing is given in
[116]. In the upper diluted zone of the circulating uidized bed, clusters are formed with
mainly upward ow in the core and predominantly downwards motion near the wall. While
the wall region can be modeled by a plug-ow
approach, the core region exhibits radial gradients. The Peclet number characterizing radial
solids mixing in the core region
P er, s =
uc 2R
Dr, s
23
24
Fluidized-Bed Reactors
uc 2R
Dr, c
hgs dp
0.33
= 2+1.8 Re0.5
p Pr
g
Single particle
(44)
Nu =
hgs dp
0.33
= 2+0.6 Re0.5
p Pr
g
where hgs is the gassolid heat-transfer coefcient, d p the particle size, and g the thermal
conductivity of gas. The mass transfer coefcient can be determined applying the analogy of
heat and mass transfer by replacing in the above
formulas the Nusselt number Nu by the Sherwood number Sh and the Prandtl number Pr by
the Schmidt number Sc. For particle Reynolds
numbers below 100 and for ne particles, the
transfer coefcients are signicantly lower than
estimated by the above formulas. If necessary,
the effect of adsorption in mass transfer and of
radiation in heat transfer needs to be taken into
account additionally.
Fluidized-bed reactors exhibit a uniform temperature distribution even in case of highly exothermic or endothermic reactions. Approximations
of the heat transfer rates are necessary for the
design and control of uidized-bed reactors in
order to determine the appropriate design of internals for cooling or heating and to estimate the
Fluidized-Bed Reactors
at the wall. The solids adsorb heat and are mixed
into the uidized bed [9].
An example of the time-averaged local heat
transfer along the circumference of a tube immersed horizontally in a uidized bed is given
in Figure 28. It exhibits lower values of the heattransfer coefcient below the tube due to a gas
gap caused by bubbles and lower values on top
of the tube because of solids being at rest. With
intensied mixing this effect becomes less signicant.
The dependence of the heat-transfer coefcient on the supercial gas velocity is illustrated in Figure 29. Fluidized beds of ne particles yield a larger heat-transfer coefcient than
coarse particles. According to Molerus and
Wirth [126], different transfer mechanisms can
be identied. In case of ne particles, solids
act as agents transporting heat between walls
and bed, whereas gas convective transport is
the mechanism dominating the heat transfer of
coarse particles. The heat-transfer coefcient of
particles of intermediate sizes exhibits a maximum due to the superposition of these two transport mechanisms. Heat-transfer rates in circulating uidized beds are lower than in bubbling uidized beds due to reduced solids volume concentrations and are dominated by clusters and
strands [130].
25
6. Gas-Solid Separation
The uidizing gas inevitably carries ne catalyst
particles by entrainment to the reactor exit. Not
only for environmental reasons (i.e., to minimize
emissions) is it necessary to separate the solids
from the gas. It may also be necessary to stop the
main reaction and to avoid unwanted side or consecutive reactions or to protect following process
steps or machines from particle-laden streams.
In uidized-bed technology cyclones are mostly
used for this purpose. Knowlton [133] has given
a survey on the state of the art of cyclone design
and application in uidized-bed reactors.
The cyclone should not be considered as a
separate apparatus following the uidized bed
but should be seen as an integral part of the
uidized-bed process. The reason is that, not
only in circulating uidized beds but also in
bubbling or turbulent uidized beds, the catalyst particles which are recovered in the cyclone
are recycled to the uidized bed. The collection efciency of the cyclone is thus responsible
for maintaining the particle size distribution in
the bed inventory, which in turn determines the
uidized-bed uid mechanics and the chemical
performance of the bed as a reactor. The interrelation between uidized bed and cyclone is
discussed in Section 9.3.2.
The inuence of cyclone performance on the
overall process performance is increasingly considered. For example, Pulupula et al. [134] investigated the role of cyclones in the regenerator system of a commercial FCC unit. Arnold
et al. [135] were able to trace the deterioration
of plant performance in the ALMA maleic process back to problems with cyclone efciency. A
change of the cyclone design improved the particle size distribution of the bed inventory and
consequently bed hydrodynamics and chemical
conversion. Smit et al. [136] report on cyclone
performance in turbulent uidized-bed Synthol
reactors for FischerTropsch synthesis. Carbon
deposition on the catalyst particles inuences
the bed hydrodynamics, which in turn, via the
26
Fluidized-Bed Reactors
Figure 29. Heat-transfer coefcients determined with a tube immersed vertically in a uidized bed of glass beads of different
size operated at ambient conditions, adapted from [126, 129]
evaporated from their surface while the particles were mixing in the bulk of the bed [140,
141]. This latter mechanism helps to transport
the reactant away from the location of the nozzle and thus contributes to equalization of the
feed distribution inside the reactor. The special case that a large oil droplet impinges on a
smaller hot catalyst particle was recently investigated in a 3D direct numerical simulation to analyze dropletparticle collisions in the Leidenfrost regime [142]. The calculations were carried
out for conditions prevailing near the feed nozzle
in an FCC riser. Vapor layer pressure induced by
evaporation and the droplet surface tension are
the driving forces for droplet recoiling and rebounding. The contact time for a FCC particle
and an oil droplet turned out to be about 140 s.
8. Industrial Applications
In this chapter the industrial uses of uidizedbed reactors are classied as follows:
1)
2)
3)
4)
5)
Fluidized-Bed Reactors
27
Figure 30. Fluid catalytic cracking process (KelloggOrthoow system; according to [143, 144])
a) Reactor; b) Regenerator
28
Fluidized-Bed Reactors
Synthesis of Acrylonitrile. The crucial factor in the successful use of the uidized-bed reactor for the synthesis of acrylonitrile by the
ammonoxidation of propene (Sohio process)
( Acrylonitrile) was reliable control of this
strongly exothermic reaction:
C3 H6 +NH3 +3/2 O2 C3 H3 N+3 H2 O Hr
= 515 kJ/mol of acrylonitrile.
The reaction is carried out at a bed temperature of 400500 C and gas contact time of 115
s [145] or 520 s [2]. Figure 32 is a schematic
of the reactor. Air is fed to the bottom of the
uidized-bed vessel. The reactants ammonia and
propene are fed in through a separate distributor (b). Catalyst regeneration by carbon burnoff
occurs in the space between the air distributor
and the feed-gas distributor. The heat of reaction is removed by bundles of vertical tubes (a)
inside the bed (horizontal tubes are used in other
designs [146]).
However, experience has shown that this reactor is costly, relatively expensive to operate
and maintain, and scale-up to the size of the reactors in operation is probably close to the maximum achievable for operation at 350 C and 2.5
MPa. Therefore, in the 1990s the 16 circulating uidized-bed reactors operating at Sasols
Secunda site were replaced by eight turbulent
uidized-bed reactors each of 10.7 m diameter,
which achieve a higher per-pass syngas conversion [150].
Different process routes have been developed for the synthesis of maleic anhydride. The
Mitsubishi process [152, 153] used the naphtha
Fluidized-Bed Reactors
cracker C4 fraction. The ALMA process uses nbutane as feedstock [154, 155]. A more recent
development is the Du Pont process, which is
also based on n-butane but uses a circulating uidized bed as reactor (Fig. 34) [156]. It is based
on a vanadium phosphorus oxide (VPO) catalyst
which oxidizes n-butane to maleic anhydride by
a redox mechanism on its surface layers [157]. In
the riser n-butane is selectively oxidized by the
oxidized catalyst. In the uidized-bed regenerator the spent catalyst is reoxidized. Since 1996 a
commercial plant has been operating in Asturias,
Spain [158].
29
163]; the synthesis of phthalonitrile by ammoxidation of o-xylene ( Phthalic Acid and Derivatives) [164]; the synthesis of aniline by gasphase hydrogenation of nitrobenzene ( Aniline, Chap. 3.2) [165]; and the low-pressure synthesis of melamine from urea ( Melamine and
Guanamines) [166].
An overview on the various uidized-bed catalytic processes has been given [167].
30
Fluidized-Bed Reactors
Fluidized-Bed Reactors
31
Figure 37. Power plant with circulating uidized-bed furnace (Lurgi process) [180]
a) Circulating uidized-bed reactor; b) Recycling cyclone; c) Siphon; d) Fluidized-bed heat exchanger; e) Convective pass;
f) Dust lter; g) Turbine; h) Stack
CaCO3 CaO+CO2
yields CaO, which can bind in situ the SO2 produced in combustion:
SO2 +CaO+1/2 O2 CaSO4
During the 1980s the uidized bed was established in power-plant engineering. The unit size
rapidly increased from 5 MWe in 1970 to about
350 MWe during this time [179]. Meanwhile (ca.
2006) some 500 power plants are in operation
worldwide. By far the majority of these plants
operate with circulating uidized beds. As an
example, Figure 37 shows a Lurgi design.
The staged admission of the combustion air
minimizes NO production from nitrogen in the
fuel in the lower part of the combustion chamber. The admission of secondary air completes
the combustion in the upper part of the chamber by oxidizing most of the CO. Some of the
circulating solids are led through the external
uidized-bed cooler, which enhances the exibility of control and permits load variation over
a wide range.
More recent developments aim at even larger
capacities with a further enlargement of the combustion chamber and making use of supercritical steam conditions and once-through boiler
design. One problem associated with the size
enlargement is the distribution of both the coal
32
Fluidized-Bed Reactors
Figure 38. Furnace cross section of a large CFB combustor (after [179])
Figure 39. Power plant with pressurized uidized-bed combustor (ABB design) [187]
a) Pressurized uidized-bed boiler; b) Cyclone; c) Gas turbine; d) Economizer; e) Ash removal; f) Fuel feed; g) Feed-water
tank; h) Steam turbine; i) Condenser; j) Bed material hopper
Fluidized-Bed Reactors
the uidized bed by means of piston pumps.
The uidizing air is preheated in an oil-red
mufe before reaching the furnace. Fuel oil,
used as a supplemental fuel, is metered directly
into the bed. Developments in sludge incineration have achieved energy autarky by recovering
waste heat and utilizing it to predry the sludge
so that self-sustaining combustion is possible
[194 196]. Later, the more stringent emission
limits set forth in the 17th Bundesimmissionschutzverordnung (BImSchV, regulation in the
Federal Republic of Germany concerning the
limitation of immissions) may necessitate staged
combustion (as in power generation), particularly to control NOx emissions [197, 198].
For the incineration of municipal waste, a furnace with a rotating uidized bed has been
developed. The inclined distribution grid in this
design generates two rollerlike ows of circulating bed solids, leading to rapid and efcient
mixing of the waste in the bed [199].
Coal Gasication. A number of uidizedbed processes have been developed for gasifying
coal ( Gas Production; e.g., [2]). Interest in
these processes for cogeneration power plants
has recently become more intense. In the cogeneration system shown in Figure 41, highpressure gasication is combined with com-
33
bustion in a circulating uidized bed; efciencies of more than 40 % are expected, depending on the available gas turbine technology
[180]. The Rheinische Braunkohlenwerke company has developed a high-temperature Winkler
(HTW) process based on Winkler gasication
(Fig. 42) [200]. The pressure (ca. 10 bar) and
temperature (ca. 1100 C) are higher than in the
Winkler process; coal is gasied with oxygen
and steam. Recycling of solids from the cyclone
to the uidized bed results in a much higher carbon conversion than in the Winkler process.
Gasication of Solid Waste. In comparison
with incineration, the gasication of solid waste
offers the advantage of a smaller volume of offgas, so the cleaning system can be made smaller.
In the Japanese Pyrox process, heat required
by the gasication reactor is supplied by sand
heated in a uidized-bed furnace, so that a highBtu-gas can be generated [2].
A cement kiln plant at Ruedersdorf in Germany is operated with a biomass gasication reactor. This circulating uidized-bed reactor designed by Lurgi supplies fuel gas for the calciners [201].
Calcination. The calcination of aluminum
hydroxide in the Vereinigte Aluminiumwerke
(VAW)/Lurgi circulating uidized-bed process
features an overall thermal efciency of more
than 70 %, which is achieved through downstream heat recovery from the calcined alumina
and the off-gas [18, 202 204]. The circulating
uidized bed proper (c) is coupled to two venturi
uidized beds (a), in which the moist hydroxide
is rst dried and heated by direct contact with the
off-gas before it is forwarded to the calcination
furnace (see Fig. 43). The ve-stage uidizedbed cooler (d) downstream of the furnace serves
to preheat the combustion air. A furnace 3.8 m
in diameter and 20 m tall, with a uidization velocity of 3 m/s and mean particle diameter of
0.040.05 mm, produces more than 500 t/d of
Al2 O3 [18].
Other applications include the calcination
of limestone (in multistage uidized-bed furnaces), lime muds, and crude phosphates [2, 18].
Roasting Processes. Fluidized-bed roasting
follows the general reaction equation
34
Fluidized-Bed Reactors
Figure 41. Concept for cogeneration power plant based on high-pressure gasication in circulating uidized bed [185]
a) High-pressure CFB gasication; b) Gas cleaning; c) CFB combustion; d) Waste-heat boiler; e) Gas turbine; f) Steam turbine
heat generated by the exothermic roasting reaction is removed by tube banks immersed in the
bed, via a solid heat-transfer agent, or by simple
water injection. Roasting furnaces are available
in very large sizes (bed diameters up to 11 m)
with capacities of several hundred tonnes of ore
per day [2, 18].
Fluidized-Bed Reactors
35
36
Fluidized-Bed Reactors
mm in diameter serve as support for the microorganisms; at uidization velocities of 820 m/h,
the biolm grows to a thickness of 0.060.2 mm
on these particles. The reactors are large devices
with diameters of 4.6 m and bed heights of 21 m.
Fluidized-Bed Reactors
the bed from above to maintain the proper moisture level; electrodes (b) dipping into the bed
measure this parameter. The moisture content
of the solids is generally a critical parameter
for the uidized-bed fermenter; the bioreactions
extinguish if it becomes too low, whereas the
particles agglomerate and uidization is disrupted if it becomes too high. Sterilized air is
used for uidization. Seed spores of the microorganisms are fed into the bed via the ejector
(e). This system achieves a considerable gain in
cell yield and an enrichment of certain enzymes
by a factor of 515 over conventional xed-bed
cultures. The generated biomass forms the basis
for soy sauce production.
9. Modeling of Fluidized-Bed
Reactors
9.1. Modeling of LiquidSolid
Fluidized-Bed Reactors
An expansion formula of the RichardsonZaki
type, Equation (7), describes the hydrodynamics
of liquidsolid uidized beds fairly well [218].
The difculty in modeling this kind of reactor
for bioreactions thus lies not so much in determining the ow and mixing conditions in the
uid as in describing the diffusion processes in
the biolm and the kinetics of the biological reactions [219]. In view of the small number of
experimental studies reported thus far, no nal
judgment can be made on the suitability of various models [208].
37
38
Fluidized-Bed Reactors
(45)
Suspension phase
di
(1b ) [mf + (1mf ) i ] C
=
t
di
umf (1b ) C
+k
a
(C
G,i
bi Cdi )
h
M
+ (1b ) (1mf ) s
i,j rj
(46)
j=1
In Equations (45) and (46) the following simplifying assumptions have been made:
1) Plug ow through the suspension phase at an
interstitial velocity (umf /mf )
2) Bubble phase in plug ow, bubbles are solids
free
3) Reaction in suspension phase only
4) Constant-volume reaction (see [224] for handling a change in number of moles)
5) Sorption effects neglected (see [229] for handling sorption)
Here i is the porosity of the catalyst particles; a is the local mass-transfer area per unit of
uidized-bed volume, which can be calculated
as
a=
6b
dv
(47)
for spherical bubbles; r j is the rate of partial reaction j per unit mass of catalyst; and ij is the
stoichiometric number of species i in reaction j.
The relation
kG,i =
umf
+
3
4Di mf ub
dv
(48)
proposed by Sit and Grace [230] has proved useful for describing the mass-transfer coefcient
k Gi associated with component i in mass transfer
between the bubble and suspension phases; Di
is the molecular diffusion coefcient of species
i.
The freeboard space above the bubbling uidized bed must be considered in the reactor
model if the entrainment rate is high and the
reactions in the freeboard are not quenched, for
example, by cooling.
Most uidized-bed models include concentration proles only for the vertical direction.
This one-dimensional modeling is acceptable
when the reactants are admitted uniformly over
the bed cross section. If, however, reactants are
metered into the bed at individual feed points,
three-dimensional modeling may become necessary. Such models have been devised for the
combustion of coal in bubbling uidized beds
[232 234].
As a rule, the modeling of solids behavior in
bubbling uidized-bed reactors is based on that
in stirred tanks. Fluidized-bed combustion is one
of the few exceptions; here the model must take
account of the propagation of coal from the feed
point if the furnace emission behavior is to be
described correctly [232, 234].
Temperature homogeneity is a virtually fundamental property of the uidized-bed reactor.
Even so, one exception is industrially important:
in high-pressure uidized-bed furnaces, the high
energy density can cause local hot spots near the
fuel injection points [235]. Reactor models that
take care of this have been described, e.g., in
[236].
9.2.2. Circulating Fluidized-Bed Reactors
In the early days of circulating uidized-bed reactor modeling, negligible axial dispersion and
laterally uniform ow structure were believed to
characterize these systems. Thus, simple plugow models were used [237]. This approach was
found to oversimplify the behavior of circulating uidized-bed reactors, because a signicant
amount of axial dispersion was observed. As a
result, the plug-ow model has often been modied by adding a dispersion term to the balance
equations. Axial dispersion coefcients have
Fluidized-Bed Reactors
39
been determined by many authors who measured the residence time distribution of tracer
gases [238, 239]. Typical values of Peclet numbers they found are on the order of 10.
By means of a model reaction it has been
proved that in many cases circulating uidizedbed reactors cannot be characterized by solely
considering mixing phenomena [240]. Instead,
the presence of mass-transfer limitations and bypassing was found to have a signicant inuence. In analogy to low-velocity uidized beds
a detailed description of the local ow structure
within the reaction volume must serve as a basis
for appropriate reactor modeling.
The highly nonuniform ow structure of circulating uidized beds described in 2.9.2 has
led to reactor models which separately deal with
different axial zones. The bottom zoneif it exists under the given operating conditionscan
be described by models whose basic approaches
were originally developed for modeling of bubbling uidized beds [241]. Modeling of the upper section of the circulating uidized bed is
in most cases based on a proper description of
the heterogeneous coreannulus ow structure
[242 244]. These state-of-the-art models are
one-dimensional and dene two phases or zones
which are present at every axial location:
1) A dense phase or annulus zone: high solids
concentration, gas stagnant or moving downwards
2) A dilute phase or core zone: low solids concentration, gas owing quickly upward.
Similar to the situation in bubbling uidized
beds, the two phases exchange gas with each
40
Fluidized-Bed Reactors
Figure 47. The multiscale approach for CFD modeling of uidized-bed reactors [254].
dency to model the uid mechanics of uidizedbed reactors from rst principles. The problem
of computational uid dynamics (CFD) modeling in this area is that the particleparticle and
particleuid interaction must be considered on
the particle scale, while the reactor performance
must be described on a much larger scale, typically on the order of several meters. This leads
to computational difculties and problems with
available computing capacities. At present (ca.
2006) there is no generally accepted CFD model
of the uidized-bed reactor available, but rapid
progress can be seen in this area [249 253].
A promising approach appears to be multiscale
modeling strategy [254].
The idea essentially is that fundamental models which take into account the relevant details
of uidparticle (lattice Boltzmann model) and
particleparticle (discrete-particle model) interactions are used to develop closure laws to feed
continuum models which can then be used to
simulate the ow structures on a larger scale.
Figure 47 illustrates this approach, which nally
leads to the discrete-bubble model and should
be applicable to the large industrial scale of the
Fluidized-Bed Reactors
41
42
Fluidized-Bed Reactors
As an example, Figure 48 shows a uidizedbed coupled with a cyclone and its translation
into the model system. Attrition leads to a loss
of material from the system, which requires the
addition of fresh catalyst after some time (Fig.
49). A population balance model which considers the changes in the catalyst particle size
intervals allows the change in the catalyst inventory with time to be followed. We see that
it takes several weeks for the system to reach
a quasisteady state. As a consequence of attrition and incomplete separation in the cyclone,
the mean particle diameter in the bed increases
with time, and this leads to larger bubbles and
a reduced area of mass transfer between bubbles and the surrounding suspension in the bed.
As a further consequence the conversion rate of
a simple rst-order reaction falls off with time.
Finally, Figure 50 shows that improvements in
the efciency of the solids-recovery system are
able to increase the conversion rate again, which
is in agreement with large-scale industrial experience [258, 259].
10. Scale-up
Typical diameters of bench-scale uidized-bed
reactors are roughly 3060 mm, and of pilotscale units 450600 mm, which should allow a
reliable scale-up [9]. Full-scale uidized-bed reactors used in the chemical industry have diameters up to ca. 10 m. Circulating uidized
bed combustors are even bigger with bed crosssectional areas reaching 200 m2 [261]. As equipment size increases, characteristic changes take
place in the gassolid ow that can decisively
affect reactor performance. Such changes result
either directly from the geometry or indirectly
from design changes made as the unit is enlarged. In particular, experience has shown that
the following factors affect the performance of
bubbling uidized beds during scale-up [262]:
Bed Diameter. According to Equation (22),
the mean upward bubble velocity increases as
the bed diameter d t increases. As a result, the
bubbles have a shorter residence time in the bed;
hence the exchange area between the bubble and
suspension phases is smaller, so conversion is reduced [263]. In case of circulating uidized-bed
combustors, measurements have shown that the
downwards velocity of solids in the wall zone
increases drastically with increasing size of the
combustor [260].
Grid Design. In the laboratory, porous plates
are the preferred type of gas distributor because
of the ease of working with them. Gas distribution becomes worse when these are replaced by
industrial distributor designs; thus the exchange
area between the bubble and suspension phases
is reduced, again with consequently lower conversion [43].
Internals. Whereas the laboratory uidized
bed is generally operated with no internals, plant
equipment often must contain bundles of heatexchanger tubes. Screens, bafes, or similar internals are frequently used to redisperse the bubble gas in industrial reactors. The mass-transfer
area is thus increased relative to the uidized
bed without internals; the extra area can be utilized to partially offset the conversion-reducing
effects of bed diameter and gas distributor [263].
Catalyst Particle-Size Distribution. Bubble growth is inuenced by the proportion of
nes in the particle-size distribution of the bed
(usually measured as the weight fraction <
0.044 mm) or by the mean grain size d p (via
Fluidized-Bed Reactors
umf , Eq. 18). If the content of nes increases,
bubbles collapse sooner and the equilibrium
bubble size becomes smaller, with a resultant
greater bubblesuspension mass-transfer area.
This effect generally is fully developed only in
the plant-scale reactor, where bubbles can grow
without the hindrance of vessel walls. Thus, in
principle, the performance of catalytic uidizedbed reactors can be controlled by modifying the
catalyst particle-size distribution [112, 264]. The
recommended content by weight of nes (<
0.044 mm) for good uidization is 3040 %
[265], but maintaining this high a nes content
in the system over a long span of time requires
a very efcient solids recovery system.
Lateral Mixing of Reactants. On a laboratory scale, reactants experience compulsory uniform distribution over the bed cross section. In
plant equipment, on the other hand, reactants
often arrive in the reactor via individual feed
points. The resulting uneven distribution of reactants can have a marked effect on reactor performance, which has been shown for the effect
of coal feeding on the emission properties of
uidized-bed furnaces [248].
Secondary Reactions in the Freeboard. In
a bench-scale apparatus, the uidized gas is
rapidly cooled by the vessel wall in the freeboard space after leaving the bed, so secondary
reactions in the freeboard are often negligible.
Such is not the case in the plant-scale reactor.
The action of wall cooling is not signicant here,
and the entrainment rate is high because of the
higher uidization velocities common in fullscale equipment. Both effectslack of cooling
and high solids concentration in the freeboard
may lead to marked secondary reactions in the
freeboard of industrial uidized-bed reactors. In
the case of a system of consecutive reactions
where the desired product is formed as an intermediate, the freeboard reactions will generally
lower the selectivity. The effect of freeboard reactions has been demonstrated for the example
of NO and CO emissions from a uidized-bed
furnace [232].
Catalyst Attrition. Catalyst attrition is minimal in laboratory apparatus, because of the use
of porous plates as gas distributors, as well as
the low gas velocities and bed depths. Attrition
43
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