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Abstract
Current worldwide commercial activities in converting natural gas to fuels and chemicals, or gas-to-liquids technology use slurry bubble
column reactors with column sizes considerable larger than those currently in practice. Such commercial activities have prompted further
fundamental research interest in uid and bubble dynamics, transport phenomena and the scale up effects of three-phase uidization systems.
The fundamental behavior of particular relevance to these activities is associated with the elevated temperature and pressure conditions.
This review attempts to summarize the salient characteristics of liquid, bubbles, and particles and their interactive behavior and dynamics in
the process of bubble formation and bubble rising in gasliquidsolid uidization systems. Measurement techniques including both intrusive
techniques such as the probes, and non-intrusive techniques such as tomography, that are used to study uid and bubble properties in gasliquid
and gasliquidsolid systems, are illustrated. Governing mechanisms of bubbleparticle collision and bubble breakup are discussed. The stateof-the-art computational techniques, that consider both the discrete and the continuum approaches for movement of the particle and bubble
phases along with the discrete simulation results, are presented. Of particular emphasis is the effect of pressure and temperature on the uid
and bubble dynamics in three-phase uidization.
2006 Elsevier Ltd. All rights reserved.
Keywords: Bubble formation; Bubble dynamics; Measurement techniques; Gasliquidsolid uidization; Pressure; Computational uid dynamics (CFD);
Bubbleparticle collision; Bubble breakup
1. Introduction
Gasliquidsolid uidization systems have been applied
extensively in industry for physical, chemical, petrochemical
and biochemical processing (Shah, 1979; LHomme, 1979;
Ramachandran and Chaudhari, 1983; Fan, 1989). Current
worldwide commercial activities in converting natural gas to
fuels and chemicals, or gas-to-liquids technology use slurry
bubble column reactors with column sizes considerable larger
than those currently in practice (Sookai et al., 2001). Such commercial activities have prompted further fundamental research
interest in uid and bubble dynamics, transport phenomena,
and the effects due to scale up of three-phase uidization
systems. The fundamental behavior of particular relevance to
these activities is associated with the elevated temperature and
pressure conditions.
In gasliquidsolid uidization systems, bubble dynamics
plays a key role in dictating the transport phenomena and
Corresponding author. Tel.: +1 614 688 3262.
ultimately affects the overall rates of reactions. It has been recognized that the bubble wake, when it is present, is the dominant
factor governing the system hydrodynamics (Fan and Tsuchiya,
1990). In general, consideration of the ow associated with the
bubble wake near the bubble base, whether laminar or turbulent, is essential to characterize the complete behavior of the
rising bubble, including its motion. Conversely, examining the
shape, rise velocity, and motion of a bubble can provide an indirect understanding of the dynamics of the liquidsolid ow
around the bubble.
Most of the three-phase processes with considerable
commercial interest are conducted under high pressure
and high temperature, for example, methanol synthesis (at
P = 5.5 MPa and T = 260 C), resid hydrotreating (at
P = 5.521 MPa and T = 300425 C), FischerTropsch synthesis (at P = 1.55.0 MPa and T = 250 C), and benzene
hydrogenation (at P = 5.0 MPa and T = 180 C) (Fox, 1990;
Jager and Espinoza, 1995; Saxena, 1995; Mills et al., 1996;
Peng et al., 1999). Fundamental study of bubble dynamics in
these gasliquidsolid uidization systems, particularly under
high-pressure and high-temperature conditions, is thus crucial.
The impedance probe has been applied to measure the bubble volume fraction, bubble length and bubble rise velocity in
three-phase uidized beds with relatively high liquid conductivity. The method utilizes the difference in conductivity between
the liquid and the gas phase. For the three-phase uidized beds
with low liquid conductivity, the addition of some salts into the
system is required (Boyer et al., 2002). Hills and Darton (1976)
investigated the bubble rising velocity in a bubble column by
an impedance probe. Matsuura and Fan (1984) studied the bubble size and bubble rise velocity in three-phase uidized beds
under three different ow regimes by using a dual electrical resistivity probe. Tang and Fan (1989) applied a dual-resistivity
probe to study the bubble size distribution and the axial distribution of gas volume fraction. Liu (1993) used a dual-sensor
resistivity probe to measure the bubble size, bubble rise velocity
and bubble frequency in the bubble column. Chen et al. (1998)
applied a dual-resistivity probe to measure the axial and radial
distributions of bubble diameter, bubble rise velocity, bubble
frequency and gas volume fraction in a three-phase uidized
bed. Zenit et al. (2001) applied a dual impedance probe to study
the gas volume fraction, bubble velocity and bubble collision
in a vertical channel. To obtain accurate bubble volume fraction using the impedance probe technique, the interaction between bubbles and the probe must be considered (Zenit et al.,
2003). Based on the statistical, fractal, chaos and wavelet analyses, the conductivity bubble probe signal can be analyzed to
discern the local ow structure of the three-phase uidized bed
(Briens and Ellis, 2005).
The optical ber probe utilizes the principle that the light
transmits in liquid medium and is reected by the gas medium
or bubbles. The optical probe is not effective, however, when
the difference in the refraction index between the gas and liquid phases is small. Lee et al. (1986) and Lee and De Lasa
(1987) measured the local gas volume fraction and bubble frequency in a three-phase uidized bed using the U shape optical
ber probe. Yu and Kim (1988) applied the U shape optical
ber probe to study the radial distributions of the bubble size,
bubble rise velocity and bubble volume fraction in three-phase
uidized beds. Frijlink (1987) developed a four-point probe to
improve the detection of the direction of the movement and the
shape of the bubble. Chabot and de Lasa (1993) measured the
axial and radial distributions of the bubble chord length, bubble
rise velocity and gas volume fraction in a bubble column at high
temperature by using the refractive optical probe. Xue et al.
(2003) applied the four-point optical ber probe to investigate
the bubble size and bubble rise velocity in gasliquid systems.
They found that a precise calibration of the probe by a CCD
camera was needed to obtain the accurate measurement on the
bubble size and bubble rise velocity. Shoukri et al. (2003) measured the gas volume fraction, bubble size, bubble rise velocity,
bubble frequency and interfacial area in a large scale bubble
column using a dual optical probe. One of the advantages for
the optic ber probe technique is that it can also be effectively
applied to high-pressure and high-temperature conditions for
the bubble property measurement (Luo et al., 1997, 1998b).
Stolojanu and Prakash (1997) obtained the solids concentration and bubble volume fraction in a three-phase uidized bed
and slurry bubble column using the gas disengagement technique together with PIV technique. Vial et al. (2001) studied
the liquid velocity and turbulence in the bubble columns with
different distributors by using the LDA technique. Kulkarni et
al. (2004) applied the LDA technique to study the bubble size
distribution in the bubble columns. Braeske et al. (1998) measured the size, velocity and holdup of bubble and solid phases in
the three-phase uidized beds using the PDA technique. Brenn
et al. (2002) applied the PDA technique to measure the velocities of liquid and bubbles in the bubble column. Cui and Fan
(2004, 2005) investigated the turbulence energy distribution in
bubble columns and three-phase uidized beds by measuring
the liquid velocity using the LDV technique. For all the laser
techniques, the laser beam needs to penetrate the ow system.
Thus, the laser techniques limited only to the low gas holdup
conditions.
Some other non-intrusive techniques are used for tracking
the particle movement, and/or mapping the instantaneous or
time-averaged, local or cross-sectional averaged, phase holdups
and phase velocities. They include PET (e.g., Bemrose et al.,
1988; Stein et al., 2000; Dechsiri et al., 2005; Hoffmann et al.,
2005), and RPT (e.g., Cassanello et al., 1995; Larachi et al.,
1996, 1997; Chaouki et al., 1997; Chen et al., 1999; Kiared
et al., 1999; Nedeltchev et al., 2003), ultrasonic tomography
(e.g., Wolf, 1988; Xu et al., 1997; Warsito et al., 1999; Utomo
et al., 2001), nuclear magnetic resonance imaging (NMR or
MRI) (e.g., Gladden, 1994, 2003; Chaouki et al., 1997; Leblond
et al., 1998; Le Gall et al., 2001; Lim et al., 2004; Sederman
and Gladden, 2005; Gladden et al., 2005), electrical impedance
tomography (EIT) (George et al., 2001; West et al., 2001; Kim
et al., 2005) and electrical capacitance tomography (ECT)
(Warsito and Fan, 2001, 2003). The details of each of these
techniques and the specic hydrodynamic parameters they
measure can be found in the corresponding references.
The MRI technique has been widely used in medical applications. This technique, however, has also been used for the
measurement of multiphase ow systems such as the xed beds
and trickle beds (Gladden, 1994, 2003; Chaouki et al., 1997;
Leblond et al., 1998; Le Gall et al., 2001; Lim et al., 2004;
Sederman and Gladden, 2005; Gladden et al., 2005). Lim
et al. (2004) applied the ultra-fast MRI technique to investigate the hydrodynamics in the trickle bed reactors. The 2D
images of the trickle bed can have a higher spatial resolution
of 351 m 351 m with a slow acquisition time of 6.4 s,
or a low spatial resolution of 1.4 mm 2.8 mm with a relatively fast acquisition time of 20 ms. The MRI can also be
used to quantify the ow eld in bubble column systems. The
relatively high cost of the technique and certain uid property requirements, however, may hamper widespread usage
of the MRI as a process tomography technique. The ECT
is developed to image the multiphase media with dielectric
properties. It can be used to quantify the dynamic bubble
ow behavior in the gasliquid and gasliquidsolid threephase uidized beds. Compared to the CT, the ECT technique
has a relatively low spatial resolution but a relatively high
temporal resolution. The ECT is suitable for process tomography applications for various multiphase ow systems. The
Fig. 1. Snapshots of the 3D volume images of bubble plumes compared with photographs: Ug = 0.02 m/s (from Warsito and Fan, 2005).
FI,m
FC
s= 0.3
Key P(MPa)
0.1
2.0
8.0
VB106 (m3)
FB
FM
FBA
0.1
FI,g
FD
0.01
0.01
0.1
10
Qg106 (m3/s)
Fig. 3. Effect of pressure on initial bubble volume (from Yoo et al., 1997).
ro
Fig. 2. The balance of all the forces acting on a growing bubble (from Luo
et al., 1998a).
(1)
The expansion stage and the detachment stage follow the same
force balance equation, although the expression for the same
force in the two stages may be different due to different bubble
moving velocities in the two stages. The expressions for all the
forces under two stages are given in Table 1.
The effect of pressure on the initial bubble volume is shown
in Fig. 3. Under relatively low pressures (less than 2.0 MPa),
the pressure effect on the initial bubble volume is seen to be
signicant; however, under relatively high pressures, the effect
of pressure on the initial bubble volume becomes insignicant
(Yoo et al., 1997).
The effect of wetting conditions on bubble formation at a very
low gas ow rate was recently investigated by Gnyloskurenko
et al. (2003, 2005). The wetting conditions were varied via
coating the orice plate by vacuum silicon grease or by parafn. In their experiments, the equilibrium contact angles were
changed from 68 to 110 (the higher contact angle, the poorer
wettability). It was found that the nal bubble size detached
from the orice increased signicantly as the wetting condition
worsened, i.e., a higher contact angle.
3.2. Bubble shape
The characteristics of a rising bubble can be described
in terms of the shape, rise velocity, and motion of the bubble. These rise characteristics are closely associated with the
behavior of the bubble wake, and the ow and physical
properties of the surrounding medium (mainly viscosity and
the presence/absence of solid particles) as well as the interfacial properties of the bubble surface (i.e., presence/absence of
surfactant). In this section, the bubble shape and the single bubble rise velocity in both liquids and liquidsolid suspensions
are described.
Table 1
Expressions for the forces involved in the bubble formation process
Forces
FB
FM
Expansion stage
6
4
Detachment stage
db3 (l g )g
Do2 g u2o
db2
u2
l b
2
24
Re
Same as expansion stage
FD
CD
F
Do cos
FI,g
d 3
d ub
dt g 6 b
FBA
Not applicable
t
3 2
dt d
d l l 0 du/
t
2 b
FC
FI,m
d(
m um V )
dt
4
=
d 3
d ub
dt m 6 b
The shape of bubbles moving in Newtonian liquids can generally be identied as spherical, oblate ellipsoidal and spherical/ellipsoidal cap. The observed bubble shape is a result of an
intricate balance among forces acting on the rising bubble, including surface tension, viscous, and buoyancy forces. As the
dominant forces change with increasing bubble size, the bubble
shape undergoes changes from spherical, ellipsoidal to spherical cap shape.
When the bubble size, db , is small, e.g., less than 1 mm
in water, and the shape is spherical, viscous forces and surface tension forces dominate. At low Reynolds numbers (i.e.,
Re = l ub db /l < 1), the HadamardRybczynski theory and
the Stokes theory apply to spherical bubbles of mobile and
immobile (rigid) surfaces, respectively. In practice, especially
when bubbles in low viscosity liquids, the Reynolds number
easily exceeds unity and the inertial term is no longer negligible. Levich (1962) obtained an equation for bubble rise velocity based on the boundary layer theory for spherical bubbles at
higher Reynolds numbers. All these theories result in an identical analytical expression with different constants accounting for
different bubble surface conditions (Fan and Tsuchiya, 1990).
For bubbles of an intermediate size, both the surface tension
and the inertia (buoyancy) force are important in dictating the
shape uctuation and the dynamics of motion of the bubble.
The wake forms and undergoes a complex shedding process for
an intermediate size of bubbles, which is also the case when the
bubble size is large. For large bubbles, the inertia force dominates and the effects of the surface tension, viscosity, and purity
of the liquid media on bubble dynamics are negligible. A large
bubble rising in water is of a spherical cap shape whereas it is
of an ellipsoidal shape for an intermediate bubble (Clift et al.,
1978; Fan and Tsuchiya, 1990).
In slurry bubble columns and gasliquidsolid uidized
beds of small and light particles, bubble behavior has often
been observed to resemble that in viscous liquids (Stewart and
Davidson, 1964; Oestergaard, 1973; Dayan and Zalmanovich,
db2 s s u2
db ub l
,
l
(2a)
Eo =
gdb2
,
(2b)
Mo =
g4l
2l 3
where = l g .
(2c)
1,
Ta < 1,
0.24,
39.8 Ta.
Here, Ta(=Re Mo0.23 ) is the Tadaki number.
ations of such physical properties, particularly the liquid viscosity and surface tension, be included in the analysis of data,
empirical correlation, theory and model developments and numerical simulations.
Since the bubble rise velocity depends on liquid properties,
the pressure and temperature thus affect the bubble rise characteristics. Krishna et al. (1994) studied the pressure effect on
the bubble rise velocity and found that the single bubble rise
velocity does not depend on the gas density over the range of
0.130 kg/m3 . The conclusion is limited to a narrow range of
pressures. Lin et al. (1998) measured the rise velocity of single bubbles of known sizes in the Paratherm NF heat transfer
uid at various pressures and temperatures. The pressure ranges
from 0.1 to 19.4 MPa. For a given bubble size, ub tends to decrease with increasing pressure at both temperatures. The effects of pressure and temperature, or more directly, the effects
of the physical properties of the gas and liquid phases on the
variation of ub with db can be predicted by the FanTsuchiya
equation (Fan and Tsuchiya, 1990), the modied Mendelsons
wave-analogy equation (Mendelson, 1967) by Maneri (1995)
and a correlation proposed by Tomiyama et al. (1995).
The FanTsuchiya equation, generalized for high-pressure
systems, can be written in a dimensionless form:
n
1/4
l
Mo1/4 5/4 2
u b = ub
=
db
g
Kb
l
n/2 1/n
2c
db
+ +
,
(4)
db
l
2
where the dimensionless bubble diameter is given by
db = db (l g/)1/2 .
(5)
10
(8a)
(8b)
K=
and
(6)
11
dl
32 l 3
=
,
dt
3Rd2 l db
(9)
where the parameter is a measure of the surface drag or velocity gradient at the surface due to the adsorbed layer of the gas.
It is known that surface tension decreases and liquid viscosity increases with increasing pressure. In addition, increases
with pressure. As can be seen from Eq. (9), all of these variations contribute to the reduction of the lm thinning velocity,
and hence the bubble coalescence rate, as pressure increases.
As a result, the time required for two bubbles to coalesce is
longer and the rate of overall bubble coalescence in the bed
is reduced at high pressures. Moreover, the frequency of bubble collision decreases with increasing pressure. An important
mechanism for bubble collision is the bubble wake effect (Fan
and Tsuchiya, 1990). As the bubble size and the rise velocity
reduce at high pressures, the likelihood of small bubbles being
caught and trapped by the wakes of large bubbles decreases.
Therefore, bubble coalescence is suppressed by the increase in
12
(10)
13
bubbles in gasliquid systems (Walter and Blanch, 1986). Calculations by Lin et al. (1998) showed that the theory underpredicts the maximum bubble size obtained by experiments and
could not predict the effect of pressure on the maximum bubble
size.
A maximum stable bubble size exists for bubbles rising freely
in a stagnant liquid without external stresses, e.g., rapid acceleration, shear stress, and/or turbulence uctuations (Grace
et al., 1978). The RayleighTaylor instability has been regarded
as the mechanism for bubble breakup under such conditions. A
horizontal interface between two stationary uids is unstable to
disturbances with wavelengths exceeding a critical value if the
upper uid has a higher density than the lower one (Bellman
and Pennington, 1954):
c = 2
.
(11)
g(l g )
the centrifugal force to be equal to the dynamic pressure induced by the gas moving at the bubble rise velocity, that is,
kf g u2b /2 (kf 0.5), and proposed a simple equation to calculate the maximum stable bubble size:
Dmax
3.63
.
u2b 3 2l g
(12)
8
4/3 E( 1
2 )
2
ub db
.
(13)
0.312
g
in liquids, and
Dmax 3.27
gg
(for = 0.3)
(14b)
14
bubble columns, the gas holdup can be related to the supercial gas velocity, Ug , and the average bubble rise velocity, ub ,
(based on bubble volume) by a simple equation:
Ug = g ub .
(17)
15
16
Fig. 6. A series of photographs showing the bubblingjetting transition at P = 4.24 MPa and T = 28 C for (a) uo = 0.27 m/s and Reo = 1075; (b) uo = 1.35 m/s
and Reo = 5321; (c) uo = 2.23 m/s and Reo = 8809; (d) uo = 2.60 m/s and Reo = 10, 243; (e) uo = 3.99 m/s and Reo = 15, 759; (f) uo = 6.42 m/s and
Reo = 25, 355 (from Luo et al., 1998b).
17
18
Fig. 7. Simulation results of air bubble formation from a single nozzle in water (nozzle size 0.4 cm I.D. and nozzle gas velocity 10 cm/s) (from Ge and Fan, 2006).
requiring 3D calculation. The VOF method was used to simulate the liquid droplet collision with solid surface (e.g., Karl
et al., 1996; Bussmann et al., 1999, 2000; Harvie and Fletcher,
2001a,b). Mehdi-Nejad et al. (2003) also used the VOF method
to simulate the bubble entrapment behavior in a droplet when
it impacts a solid surface. The VOF was also used in the 2D
discrete phase simulation of bubble motion in gasliquid and
gasliquidsolid ows (Li et al., 1999, 2001; Zhang et al., 2000;
Dijkhuizen et al., 2005). In the approach of Li et al. (1999), the
Eulerian volume-averaged method, the Lagrangian DPM, and
the VOF volume-tracking method were employed to describe
the motion of liquid, solid particles, and gas bubbles, respectively. A bubble induced force (BIF) model, a CSF model, and
Newtons third law are applied to account for the couplings
of particlebubble, bubbleliquid, and particleliquid interactions, respectively. A close distance interaction (CDI) model is
included in the particleparticle collision analysis, which considers the liquid interstitial effect between colliding particles
(Zhang et al., 1999). Other front capturing methods include the
constrained interpolation prole (CIP) method (Yabe, 1997),
and the phase-eld method (Jamet et al., 2001).
In the level-set method, the moving interface is implicitly represented by a smooth level-set function (Sethian and Smereka,
2003). The level-set method has proved capable of handling
19
Fig. 8. Simulation results of bubble formation and rising in Paratherm NF heat transfer uid with and without particles (nozzle size 0.4 cm I.D., liquid velocity
0 cm/s, gas velocity 10 cm/s, and particle density 0.896 g/cm3 ): (a) no particle; (b) 2000 particles; (c) 8000 particles; (d) 8000 particles (from Ge and Fan, 2006).
20
level-set interface tracking approach are presented, which account for the bubble, particle and liquid interactive behavior
and the ow structure in three-phase ows. Challenges on CFD
remain, however, with respect to improving computational accuracy, as well as incorporating reaction kinetics and transport
phenomena properties into uid dynamics calculations, and the
micro-scale ow properties into simulation of a large scale
three-phase reactor. The formulation of closure relationships
for the Eulerian computation is also in need of further work.
Notation
b
c
CD
db
db
dp
dvs
Dmax
Do
e
E( 1
2 )
Eo
f (db )
FB
FBA
FC
FD
FI,g
FI,m
FM
F
g
h
Hd
K
Kb
l
Mo
n
ni
Nc
P
Qg
Q0
ro
Rd
Re
bubble breadth
parameter in FanTsuchiya equation reecting surface tension effect
drag coefcient
volume equivalent bubble diameter
dimensionless bubble diameter
particle diameter
Sauter mean bubble diameter
maximum stable bubble size
orice diameter
restitution coefcient
complete second kind Elliptic integral
Etvs number based on bubble diameter
probability density function of bubble size
effective buoyancy force; buoyancy force
Basset force
particlebubble collision force
liquid drag force
bubble inertial force
liquidsolid suspension inertial force
gas momentum force
surface tension force
gravitational acceleration
bubble height; particle penetration depth
height of a doughnut-shape bubble
proportionality constant for calculating the
effective viscosity of liquidsolid suspensions
parameter in FanTsuchiya equation reecting viscous nature of surrounding medium
thickness of the liquid lm between two coalescing bubbles
Morton number based on liquid properties
parameter in FanTsuchiya equation reecting system purity
number of bubbles
dimensionless capacitance number
system pressure
volumetric gas ow rate into the gas chamber
volumetric gas ow rate through the orice
radius of orice
radius of acontacting circle between two bubbles
bubble Reynolds number based on liquid
properties
Reo
t
T
Ta
u
ub
ub
ue
um
umax
uo
ut
ub
Ug
Ul
Up0
Vb
Vc
Wecr
21
Greek letters
g
l
s
sc
s0
c
g
l
m
g
l
m
s
Acknowledgment
The work was supported by the National Science Foundation
Grant CTS-0207068.
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