Particuology 16 (2014) 213–217

Contents lists available at ScienceDirect

Particuology
journal homepage: www.elsevier.com/locate/partic

Mass transfer between bubbles and the dense phase

in gas fluidized beds夽
Hongyong Xie ∗ , Zhiguo Sun
School of Urban Development and Environmental Engineering, Shanghai Second Polytechnic University, Shanghai 201209, China

a r t i c l e i n f o a b s t r a c t

Article history: Mass transfer between a bubble and the dense phase in gas fluidized beds of Group A and Group B particles
Received 14 December 2013 was proposed based on previous experimental results and literature data. The mass transfer coefficient
Received in revised form 10 February 2014 between bubbles and the dense phase was determined by kbe = 0.21db . A theoretical analysis of the mass
Accepted 5 March 2014
transfer coefficient between a bubble and the dense phase using diffusion equations showed that the
mass transfer coefficient between a bubble and the dense phase is kbe ∝ εmf Dub /db in both three- and
Keywords:
Fluidized beds
two-dimensional fluidized beds. An effective diffusion coefficient in gas fluidized beds was introduced
2.7
Bubbles and correlated with bubble size as De = 13.3db  A and Group B particles. The mass transfer
for Group
Dense phase coefficient kbe can then be expressed as kbe = 0.492εmf ub db1.7 for bubbles in a three-dimensional bed
Mass transfer 
and kbe = 0.576εmf ub db1.7 for bubbles in a two-dimensional bed.
Effective diffusion coefficient
© 2014 Published by Elsevier B.V. on behalf of Chinese Society of Particuology and Institute of Process
Engineering, Chinese Academy of Sciences.

1. Introduction et al., 2007), and injection of an isolated or stream of tracer bubbles.

In gas–solid fluidized beds, bubbles are formed near the bottom
of the bed, and exchanges between the gases inside the bubbles
and in the dense phase happen all the time as the bubbles rise
through the bed. The mass transfer between bubbles and the dense
phase plays an important role in fluidized beds of Group A and
Group B particles (Geldart, 1973), and is the controlling step for
chemical and physical processes taking place in the fluidized beds
provided that the chemical reactions or physical processes are fast.
Therefore, understanding the mass transfer between bubbles and
the dense phase in fluidized beds is important not only for process
control but also for fluidized bed design.
The study of the interface mass transfer has used UV absorption
techniques (Chavarie & Grace, 1976; Chiba & Kobayashi, 1970; Sit
& Grace, 1978), sampling methods (Song, 2004; Song & Xie, 2003,
2006; Wu & Agarwal, 2003), gas sensors (Solimene, Marzocchella,
Passarelli, & Salatino, 2006), nuclear magnetic resonance (Pavlin
夽 This paper is adapted from the presentation at the 4th UK-China International
Particle Technology Forum, October 15–19, Shanghai, China, as recommended by
Prof. Xiaoshu Cai and Dr. Jerry Heng, the co-chairs of the scientific committee.
∗ Corresponding author. Tel.: +86 13061662936.
E-mail addresses: hyxie@163.com, hyxie@sspu.edu.cn (H. Xie).
By injecting a stream of tracer bubbles and using UV absorption
to measure the tracer concentration (Chiba & Kobayashi, 1970),
the mass transfer coefficient in a bubbling fluidized bed of Group
B particles was obtained. The mass transfer in a two-dimensional
fluidized bed of Group B particles was also investigated by inject-
ing a single tracer bubble (Chavarie & Grace, 1976; Sit & Grace,
1978). In addition, the effect of the bubble’s interaction on the mass
transfer between bubbles and the dense phase was also investi-
gated by injecting two equally-sized bubbles (Sit & Grace, 1978). For
Group A particles, by injecting a single tracer bubble and measur-
ing tracer concentration inside the bubble using a sampling method
(Song, 2004; Song & Xie, 2003, 2006), the mass transfer coefficient
between a bubble and the dense phase has been obtained.
Two mechanisms of the diffusive and convective transfer
between a bubble and the dense phase have been modeled the-
oretically, and interaction factors have been introduced to modify
the mass transfer coefficient as the sum of the two mechanisms,
as reviewed by Sit and Grace (1978). Although agreement was
excellent for some individual cases, none of these models gave
consistently good results over the whole range of particle sizes
examined. From the diffusion equation around a bubble, Song and
Xie (Song, 2004; Song & Xie, 2006) derived a mass transfer coeffi-
cient by considering the turbulence caused by the particle’s flow
in the dense phase. An effective diffusion coefficient in a fluidized

http://dx.doi.org/10.1016/j.partic.2014.03.016
1674-2001/© 2014 Published by Elsevier B.V. on behalf of Chinese Society of Particuology and Institute of Process Engineering, Chinese Academy of Sciences.
214 H. Xie, Z. Sun / Particuology 16 (2014) 213–217

A integral constant, kmol/m3

ab bubble’s surface area based on projected bubble size
per unit bubble volume, m−1
b parameter given by Eq. (17), m
c tracer concentration, kmol/m3
cb tracer molar concentration inside bubble, kmol/m3
ce tracer molar concentration in the dense phase,
kmol/m3
C bubble velocity constant defined by Eq. (4)
D molecular diffusion coefficient, m2 /s
De effective molecular diffusion coefficient in the dense
phase, m2 /s
db projected bubble size, m
dbh pierced bubble size, m
dbv bubble volume size, m
g gravitational acceleration, m/s2
kbe mass transfer coefficient between a bubble and the Fig. 1. Illustration of the experimental apparatus used in this study.
dense phase, m/s
L width of two-dimensional bed, m
Nb gas exchange between a bubble and the dense pressure drop of approximately 0.2 m H2 O at a superficial velocity
phase, kmol/s of 1 cm/s.
r radial distance in spherical and cylindrical coordi- Nitrogen was used as the fluidizing gas and was measured and
nates, m controlled by a mass flow controller to give a superficial velocity
rb radius of projected bubble, m just above the minimum fluidization velocity of the particles. Oxy-
ub bubble velocity, m/s gen was used as the tracer gas and was introduced into the bed
u␪ tangential velocity of gas around a bubble, m/s by a solenoid valve controlled by a timer to generate a single bub-
xb tracer volume fraction inside a bubble ble. The bubble generator was a 6 mm × 1 mm stainless steel tube
bent at a right angle at the bottom and rested on the distributor.
Greek letters The size of a generated bubble was controlled by the opening time
ˇw volume fraction of bubble wake of the solenoid valve set by the timer. The gauge pressure of the
εmf voidage at the incipient fluidization oxygen cylinder was keep at 0.1 bar. A 0.1–0.5 s opening time of
 normalized variable parameter defined by Eq. (10) the solenoid valve provided a bubble size from 3 to 10 cm for the
 inclination angle in spherical and cylindrical coor- present experiments. The experimental apparatus is illustrated in
dinates, rad Fig. 1.
 bubble residence time, s Four batches of FCC particles were used in the experiments.
They were prepared by sieving an original batch, with median
sizes ranging from 50 to 90 ␮m. The particle properties of median
size, particle density, minimum fluidization and minimum bub-
bed was introduced, and the results showed that the effective
bling velocities of the four FCC particles are given in Table 1.
diffusion coefficient could be correlated well with the bubble’s
The projected bubble size was measured visually at the top of
Reynolds number.
the bed when a bubble burst out at the bed surface for the bubbles in
In this paper, the mass transfer coefficient between a bubble
the three-dimensional fluidized bed, and it was measured visually
and the dense phase in gas fluidized beds of Group A and Group
from a side of the two-dimensional fluidized bed. The residence
B particles, and a correlation of the effective diffusion coefficient
time of a bubble in the bed was measured by a stopwatch, and its
with the bubble size are proposed based on previous experimental
rise velocity was then obtained by the known bed height. The gas
results (Song, 2004; Song & Xie, 2003) and literature data (Chavarie
inside a generated bubble was sampled by an injector at the top of
& Grace, 1976; Chiba & Kobayashi, 1970; Sit & Grace, 1978) and on
the bed surface when the bubble burst out. The sampling duration
a theoretical analysis from diffusion equations (Song, 2004; Song
was restricted within 1 s to minimize the mixing effect caused by
& Xie, 2006).
freeboard gas, and approximately 5–10 mL gas was sampled each
time. The oxygen volume fraction of a sample was measured by an
2. Experimental oxygen analyzer (CYS-1). The response time of the analyzer was
15 s, and the measurement range of the analyzer was 0–100%. The
For Group A particles, the mass transfer between a bubble and resolution of the analyzer was ±0.7% in the measurement range of
the dense phase was investigated by injecting a single tracer bub- 0–25% and was ±2.5% in the measurement range of 25%–100%. In
ble (Song, 2004; Song & Xie, 2003) in a three-dimensional fluidized the experiments, a few replicates of each sample were taken, and
bed and a two-dimensional fluidized bed. The three-dimensional
fluidized bed was a 0.182 m diameter Perspex column, 1 m tall
equipped with a 0.2 m steel bottom section and a high pressure- Table 1
Physical properties of particles used in the experiments.
drop distributor. The distributor was made up of ten layers of filter
paper glued at the edges and supported by a coarse sieve to give a Particles d50% (␮m) Bulk density(kg/m3 ) umf (m/s) umb (m/s)
pressure drop of approximately 0.6 m H2 O at a superficial velocity FCC1 70 721 0.0053 0.0107
of 1 cm/s. The two-dimensional fluidized bed was made up of Per- FCC2 53 840 0.0021 0.0065
spex, 0.3 m in width, 0.01 m thick and 1 m tall. The distributor was FCC3 93 686 0.0108 0.0192
FCC4 55 747 0.0037 0.0065
a fixed bed 0.3 m tall filled with 300 ␮m glass beads, which gave a
 H. Xie, Z. Sun / Particuology 16 (2014) 213–217 215

Table 2
A typical result of the oxygen volume fraction measured.

Bed height (m) umf (m/s) db (cm) xb (×102 ) Average xb (×102 )

0.578 0.0108 8 8.4, 6.5, 8.0, 6.7,9.5, 9.9, 8.7, 9.7 8.43

the average of the oxygen volume fractions of the samples was used
in calculating the mass transfer coefficient between a bubble and
the dense phase. A typical example of the oxygen volume fraction
measured is given in Table 2.
The mass transfer coefficient kbe is defined as follows:

dcb
= kbe (cb − ce )ab , (1)
dt
where cb and ce are the oxygen concentration in the bubble and the
dense phase, respectively, and ab is the bubble’s surface area based
on the projected bubble size per unit bubble volume, expressed as:

6
ab = . (2)
db

The mass transfer coefficient kbe can thus be obtained by

neglecting oxygen in the dense phase (i.e., assuming ce = 0), as fol-
Fig. 3. Bubble volume size dbv and pierced bubble size dbh vs. projected bubble size
lows: db .
db 1
kbe = ln , (3)
6 xb
and
where  is the residence time of a bubble in the bed, db is the pro-
2 3
db3
jected bubble size and xb is the oxygen volume fraction inside the 3db dbh − 2dbh = , (6)
tracer gas bubble at the bed surface. 1 + ˇw

where ˇw is the volume fraction of the bubble wake which can

3. Results and discussion be obtained graphically from the particle Archimedes number
(Baeyens & Geldart, 1986). The bubble volume size dbv and pierced
3.1. Experimental results bubble size dbh are presented in Fig. 3 against the projected bubble
size for the results presented in Fig. 2. It can be seen that both the
The experimental results of the bubble rise velocity ub versus the bubble volume size dbv and the pierced bubble size dbh are pro-
projected bubble size db are plotted in Fig. 2. The figure showed that portional to the projected bubble size db . Thus, the dependence
the experimental results could be fitted by: of bubble rise velocity on the bubble volume size or pierced bub-
 ble size has the same pattern as that on the bubble projected size,
ub = C gdb , (4) shown in Fig. 2. The bubble velocity can be fitted by Eq. (4) with
C = 0.5 for the bubble volume size dbv and with C = 0.6 for the pierced
where C is a constant of 0.5, and g is the gravitational acceleration bubble size dbh . These values of constant C are consistent with the
(Xie, 1994, 1997). typical value of 0.5–0.66 for Group A and B particles (Clift, 1986).
For a spherical cap bubble, the bubble volume size dbv and The mass transfer coefficient kbe measured at different bed
pierced bubble size dbh can be estimated from the projected size db heights is shown in Fig. 4 against the projected bubble size for glass
by geometrical relations (Xie & Liu, 2007, chap. 5) as follows, beads of 75 ␮m (Song & Xie, 2003). The same measurement results
db for the mass transfer coefficient kbe were obtained at bed heights
dbv = , (5)
1/3
(1 + ˇw )

Fig. 4. The measured mass transfer coefficient kbe vs. projected bubble size at dif-
Fig. 2. Bubble rise velocity ub versus projected bubble size db . ferent bed heights.
216 H. Xie, Z. Sun / Particuology 16 (2014) 213–217

and by setting (Song, 2004; Song & Xie, 2006).

∂c ∂c ∂ d 1
= , where = , (10)
∂ ∂ ∂ d sin 
 2
∂c ∂c ∂ d 2r 3 + rb3
= , where = , (11)
∂r ∂ ∂r dr r4

Eq. (8) becomes

2D ∂2 c ∂c
− = 0, (12)
ub ∂ 2 ∂

where d2 /dr 2 was neglected. By introducing (Song, 2004; Song &

Xie, 2006).

 Drb
˛ = √ , where b = , (13)
b  ub
Fig. 5. Mass transfer coefficient kbe vs. projected bubble size db .
Eq. (12) becomes a 2nd order ordinary differential equation.
of 0.563 and 0.745 m. The results indicate that the mixing effect of d2 c ˛ dc
the freeboard gas on the sampling may be insignificant. =− , (14)
d˛2 2 d˛
The experimental results of the mass transfer coefficient kbe are √
shown in Fig. 5 against the projected bubble size. In the calculation with the boundary conditions r = rb , c = cb , ˛0 = ()r=rb /b  =
of kbe from the experimental results of Chiba and Kobayashi (1970), 0; r → ∞, c = ce , ˛ → ∞.
the constant C in Eq. (4) was taken as 1.5 (Xie, 1997) because the Integrating Eq. (14), one can obtain
bubbles were in a bubbling bed as the tracer bubbles were contin-
 ∞
1 2 √
uously generated in the bed. While in the calculation of kbe from ce − cb = Ae− 4 ˛ d˛ = A , (15)
0
the experimental results of Sit and Grace (1978), the constant C in
Eq. (4) was taken as 0.35 because it was in a two-dimensional bed where A is an integration constant.
(Agarwal, 1985). Since the mass transfer coefficient kbe was almost The gas exchange between a bubble and the dense phase is equal
proportional to the projected bubble size, the experimental data to
were fitted with Eq. (7), as shown in Fig. 5.    
∂c
Nb = −D 2εmf rb2 sin  d, (16)
kbe = 0.21db , (7) ∂r
0 r=rb
where the SI units should be used. This is in contrast with the exist-
where
ing theoretical models and simulations by two-fluid method for      2

Geldart B particles (Hemandez-Jimenez, Gomez-Garcia, Santana, ∂c ∂c ∂˛ − 1 d
= = Ae 4b2 
√
& Acosta-Iborra, 2013), which predict that the mass transfer rate ∂r ∂˛ ∂r b  dr
r=rb r=rb r=rb
decreases with increasing bubble size. Fig. 5 shows that Eq. (7)
√
predicts the experimental results within a relative error of ±35%. 3A 1
=−√ √ . (17)
rb b 
3.2. Theoretical analysis
Substituting Eq. (17) and using Eqs. (13) and (10), integrating
In general, gas “throughflow” is of important consequence to Eq. (16) yields
interface mass transfer in gas fluidized beds. However, the effect
is insignificant due to the small minimum fluidization velocity for   − 21
3   
d
fine particles. Moreover, gas inside a bubble could be uniform due Nb = εmf rb2 A 6Dub sin  d
to gas recirculation in a single spherical cap bubble in an incipient 0 0
sin 
fluidized bed. Under the assumptions that gas through the dense
phase is a piston flow, the bubble size and its rising velocity are
3 
= 0.272εmf rb2 A 6Dub . (18)
kept unchanged throughout the bed, and the mass transfer occurs
around the sphere whose diameter equals the projected bubble
size, the diffusion equation around a bubble in axi-symmetric According to the definition of the mass transfer coefficient, Nb =
spherical coordinates is given by the principle of relative motion 4rb2 (cb − ce )kbe ; the mass transfer coefficient kbe equals
as: 
Dub
u ∂c ∂2 c kbe = 0.135εmf . (19)
=D 2, (8) db
r ∂ ∂r
where c is the tracer concentration in the dense phase, D is the For a cylindrical cap bubble in a two-dimensional bed, the
tracer diffusion coefficient, and u␪ is the tangential velocity of the diffusion equation in axi-symmetric cylindrical coordinates has
gas in the dense phase around the bubble. the same form as Eq. (8) in axi-symmetric spherical coordinates.
According to the potential flow theory, the tangential velocity According to two-dimensional potential flow theory, the tangential
u␪ is given by: velocity u␪ is given by:
   
rb3 rb2
u = − 1+ ub sin , (9) u = − 1+ ub sin . (20)
2r 3 2r 2
 H. Xie, Z. Sun / Particuology 16 (2014) 213–217
Fig. 6. Effective diffusion coefficient De vs. bubble size db .
By the same differentiation formulas as in Eqs. (10), (11),
and (13), and neglecting d2 /dr 2 , the diffusion equation is trans-
formed to the same 2nd order ODE, i.e. Eq. (14), with the same
boundary conditions. The gas exchange between a bubble and the
dense phase in the axi-symmetric cylindrical co-ordinates is equal
to:
 2  
∂c
Nb = −D εmf rb L d, (21)
0
∂r
r=rb
where L is the width of the two-dimensional bed. Following the
same procedure as those for a spherical bubble, the mass transfer
coefficient kbe is obtained as:
 Baeyens, J., & Geldart, D. (1986). Solids mixing. In D. Geldart (Ed.), Gas fluidization
Dub
kbe = 0.158εmf . (22)
db
Both Eqs. (19) and (22) imply that the mass transfer coefficient
decreases with increasing bubble size, which conforms with the
prediction by the existing theoretical models, but it is contrary to
the experimental results. Considering the turbulence caused by
a particle’s flow in the dense phase, the diffusion coefficient D
should be increased. From the experimental results of the bub-
ble size db , bubble velocity ub , and mass transfer coefficient kbe ,
the effective diffusion coefficient De could be obtained from Eq.
(19) in a three-dimensional fluidized bed and from Eq. (22) in a
two-dimensional fluidized bed. The effective diffusion coefficients
De such obtained are plotted in Fig. 6 against the bubble size db
from the experimental results (Chiba & Kobayashi, 1970; Sit &
Grace, 1978; Song, 2004; Song & Xie, 2003, 2006;). The effective
diffusion coefficient can be correlated to the projected bubble size
as
2.7
De = 13.3db . (23)
The mass transfer coefficient kbe is then given by
kbe = 0.492εmf ub db1.7 , (24)
for bubbles in a three-dimensional bed and by:
kbe = 0.576εmf ub db1.7 , (25)
for bubbles in a two-dimensional bed.
217
4. Conclusions
The mass transfer coefficients between injected single bubbles
and the dense phase in gas fluidized beds of Group A and Group B
particles were studied. The mass transfer coefficient between bub-
bles and the dense phase was given by kbe = 0.21db for Group A and
Group B particles.
The mass transfer coefficient between a bubble  and the dense
phase from the diffusion equation is kbe ∝ εmf Dub /db in both
three- and two-dimensional fluidized beds, and an effective dif-
fusion coefficient in fluidized bed is introduced and correlated to
2.7
projected bubble size as De = 13.3db for Group A and Group B
particles.
 transfer coefficient kbe could be then given by kbe =
The mass
0.492εmf ub db1.7 for bubbles in a three-dimensional bed and by

kbe = 0.576εmf ub db1.7 for bubbles in a two-dimensional bed for
Group A and Group B particles.
Acknowledgements
The authors are thankful for an innovation research grant
(13YZ130), a Leading Academic Discipline Project (J51803) from
the Shanghai Education Committee and a Cultivate Discipline Fund
of the Shanghai Second Polytechnic University (XXKPY1303).
References
Agarwal, P. K. (1985). Bubble characteristics in gas fluidized beds. Chemical Engi-
neering Research and Design, 63, 323–337.
technology (pp. 97–122). New York: John Wiley & Sons.
Chavarie, C., & Grace, J. R. (1976). Interphase mass transfer in a gas-fluidized bed.
Chemical Engineering Science, 31, 741–749.
Chiba, T., & Kobayashi, H. (1970). Gas exchange between the bubble and emulsion
phases in gas–solid fluidized beds. Chemical Engineering Science, 25, 1375–1385.
Clift, R. (1986). Hydrodynamics of bubbling fluidized beds. In D. Geldart (Ed.), Gas
fluidization technology (pp. 53–95). New York: John Wiley & Sons.
Geldart, D. (1973). Types of gas fluidization. Powder Technology, 7, 285–292.
Hemandez-Jimenez, F., Gomez-Garcia, A., Santana, D., & Acosta-Iborra, A. (2013).
Gas interchange between bubble and emulsion phases in a 2D fluidized bed as
revealed by two-fluid model simulations. Chemical Engineering Journal, 215–216,
479–490.
Pavlin, T., Wang, R., McGorty, R., Rosen, M. S., Cory, D. G., Candela, D., et al. (2007).
Noninvasive measurements of gas exchange in a three-dimensional fluidized
bed by hyperpolarized 129 Xe NMR. Applied Magnetic Resonance, 32, 93–112.
Sit, S. P., & Grace, J. R. (1978). Interphase mass transfer in an aggregative fluidized
bed. Chemical Engineering Science, 33, 1115–1122.
Solimene, R., Marzocchella, A., Passarelli, G., & Salatino, P. (2006). Assessment of gas-
fluidized beds mixing and hydrodynamics by zirconia sensors. AIChE Journal, 52,
185–198.
Song, C. L., & Xie, H. Y. (2003). Mass transfer between the bubble and emulsion phases
in gas–solid fluidized beds. In Proceedings of the 8th China Japan symposium on
fluidization Gifu, Japan, (pp. 150–157).
Song, C. L., & Xie, H. Y. (2006). Mass transfer between the bubble and emulsion phases
in gas–solid fluidized beds. In Proceedings of the 9th China Japan symposium on
fluidization Beijing, China, (pp. 195–201).
Song, C. L. (2004). Mass transfer between bubbles and the dense phase in gas fluidized
beds. (Master Thesis). China: Dalian University of Technology.
Wu, W., & Agarwal, P. K. (2003). The effect of bed temperature on mass transfer
between the bubble and emulsion phases in a fluidized bed. The Canadian Journal
of Chemical Engineering, 81, 940–948.
Xie, H. Y. (1994). Fluidization of fine particles. (Doctoral dissertation). UK: University
of Bradford.
Xie, H. Y. (1997). Pressure probes in the measurement of bubble properties in the
fluidization of fine particles. Advanced Powder Technology, 8, 217–235.
Xie, H. Y., & Liu, Z. J. (2007). Mechanics and process engineering of powder and particles
(2nd ed.). Beijing: Chemical Industry Press (in Chinese).