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constant all the time. For this purpose, compensated Oxygen inter-phase mass transfer source term
kla values were corrected to a standard temperature was calculated by:
of 20 °C using the following formula proposed by
Whitton and Nienow (1993):15 G o , gl = k l aa g [( r l x *o , l ) - ( r l x o , l )] (8)
x o,l + x n,l = 1 (7) The equivalent total air flow rate can be calcu-
lated by the following equation:
Gas phase oxygen kinematic diffusivity
Do,g=2´10–5 m2 s–1; liquid phase oxygen kinematic 1
Q equ = Q b + Q p (11)
diffusivity Do,l=2.54´10–9 m2 s–1.18 2
170 Z. ZHOU et al., Experimental Study and CFD Simulation of Mass Transfer …, Chem. Biochem. Eng. Q. 27 (2) 167–175 (2013)
Then the equivalent superficial gas velocity Influence of pulsating amplitude on kla
was obtained from Qequ divided by the bubble col- The pulsating flow rate Qp was changed to
umn cross-section area: work at different pulsating amplitude, which varied
Q equ from 0.36 to 2.88 m3 h–1, and the digital time con-
ug = (12) troller was fixed to tb=tp engendering a constant
S pulsating frequency of 0.9 Hz during the experi-
Correlation between the volumetric mass trans- ments. The experimental observation of the influ-
fer coefficient and superficial gas velocity was usu- ence of pulsating amplitude on kla is shown in
ally represented by an equation of the following Fig. 3. It was noted that kla values obtained from
type, frequently found in the literature:3,4 the pulsating state with a fixed base flow rate of
0.18 m3 h–1 were smaller than those obtained from
k l a µ (ug ) b (13) the steady state at the same ug, and the exponent in
Eq. (13) b=0.414 representing the dependence of
Three different operating conditions were ap- kla on ug under the pulsating state was also lower
plied in this work respectively: steady state with than that under the steady state in which b=0.529.
base flow rate of 0.54 m3 h–1 to 1.62 m3 h–1 and This may be due to the equivalent superficial gas
without pulsating airflow; pulsating state with a velocity comparison necessity for the two different
fixed base flow rate of 0.18 m3 h–1, which was states. For a lower base flow, a higher pulse air in-
found to be the critical value for this gas-liquid col- flux was required for the balance with the steady
umn to be normally fluidized, and pulsating flow state, which would lead to a relatively short contact
rate of 0.72 m3 h–1 to 2.88 m3 h–1; pulsating state time between the two phases and thus may limit the
with equal base flow rate and pulsating flow rate mass transfer rate.6 It can be seen in the experi-
(Qp=Qb) of 0.36 m3 h–1 to 1.08 m3 h–1. The equiva- ments that more large bubbles formed in the col-
lent superficial gas velocity ranged from 3.75 mm umn as gas flow rate increased; however, many
s–1 to 11.25 mm s–1 in this study. small bubbles were also engendered by the highly
The regression of kla values followed Eq. (2), induced turbulence. These two-opposite effects may
typical samples were shown in Fig. 2 for two oper- have a great influence on the total interfacial area a,
ating states with the same superficial gas velocity. which was a crucial element of the volumetric mass
kla values obtained in this study ranged from transfer coefficient. Then the compromised pulsat-
6´10–3 s–1 to 15´10–3 s–1, while the oxygen probe ing state with equal base flow rate and pulsating
time constant tp was about 6 s of this sensor, indi- flow rate (Qp=Qb) was adopted to compensate the
cating that the above assumption of kla · t<1 was abovementioned effects of high air flow rate. As
justified. It was also found that kla obtained from can be seen in Fig. 3, nearly 30 % enhancement in
the two different locations of the column almost kla was achieved under the pulsating state with
held the same values within experimental errors. Qp=Qb in comparison with the steady state, espe-
This indicated that the system was in complete mix- cially for higher gas flow rate. The larger exponent
ing state, and the local kla measurements can gener- b=0.654 was also obtained for this state.
ally represent the overall kla of the column. Conse-
quently, only the measured kla from the upper loca-
tion are displayed in this work.
F i g . 2 – Typical oxygen uptake curves under ug=0.00625 m s–1 F i g . 3 – Influence of pulsating amplitude on oxygen volu-
and f=0.9 Hz metric mass transfer coefficient under f=0.9 Hz
Z. ZHOU et al., Experimental Study and CFD Simulation of Mass Transfer …, Chem. Biochem. Eng. Q. 27 (2) 167–175 (2013) 171
The physical mechanisms responsible for this same values with different time series. The increase
performance improvement were the highly induced in frequency f represented the decrease in the pulse
phase turbulence in this air-water non-coalescent feed time tp and the base feed time tb, which had a
system, which would accelerate the recirculation of correlation as follows:
the induced turbulent liquid flow and the continu-
1
ous gas-liquid surface renewal by the constant gen- f = (14)
eration and breakup of gas bubbles with phase tb + t p
pulse.
An internal camera CCD bubble measurement Linear relationship between kla and f were
technology21 was applied for the analysis of the lo- found in this study:
cal bubble size distribution (BSD) under the differ- k l a ´ 10 3 = -1566
. f + 9.438 (15)
ent operating conditions. Samples were taken at the
upper section of the column. Nearly 300 bubbles of Linear correlation coefficients R2 were above
diameters ranging from 1 mm to 15 mm were 0.99. The minus slope of the curve indicated a de-
counted. The circle time averaged BSDs obtained creasing trend of kla with the increase in pulsating
experimentally are shown in Fig. 4. For higher gas frequency f for such an operating condition, which
flow rate, large fast-rising bubbles or gas caps were is clearly shown in Fig. 5. The decrease in kla with
observed in the column especially at the lower sec- the increase in f may be due to the initial bubble
tion. However, the highly developed turbulence size formation at the gas distributor. As can be ob-
would also cause the breakage of large bubbles into served in these experiments, many large bubbles
small ones. The conjunct performance would have a (even some little bubble caps) formed from the dis-
great influence on the BSDs. As the figure shows, tributor at the very beginning of the pulse feed
many small bubbles formed under the pulsating state time, which would lead to the decrease in the
with Qp=Qb=0.6 m3 h–1; while for Qp=1.44 m3 h–1 gas-liquid interfacial area a for the mass transfer
and Qb =0.18 m3 h–1, a great many large bubbles oc- process. However, if the pulse flow was fed in con-
cupied the column in comparison with the steady tinuously as pulse went on, the large bubbles and
state. caps would be replaced by the uniform small bub-
bles. As a result, kla values were higher for lower
pulsating frequencies.
Different time series with tb=tp were used to en- Influence of bubble properties on kla
gender a pulsating frequency spectrum from 0.5 Hz
to 2.67 Hz for the unsteady state operations by the Bubble properties, such as size and distribu-
time controller. In these experiments, Qp was kept at tion, have significant effects on oxygen mass trans-
a constant value of 1.44 m3 h–1 and Qb of 0.18 m3 h–1. fer in the gas-liquid interface. However, it is expen-
The equivalent total air flow rate Qequ as well as the sive and sometimes difficult to experimentally mea-
superficial gas velocity ug were calculated to be the sure the local and transient changes of bubble prop-
172 Z. ZHOU et al., Experimental Study and CFD Simulation of Mass Transfer …, Chem. Biochem. Eng. Q. 27 (2) 167–175 (2013)
F i g . 9 – Model prediction of DO distribution under ug=0.01 m s–1 (Qp=2.52 m3 h–1 and Qb=0.18 m3 h–1) and f=1.25 Hz
tion at the inlet of the column was made in the DO concentration fluctuations in real
model, which neglected the effect of the pulsating bioprocess systems
inlet air and then resulted in a deviation of the The most important parameter in real bio-
model simulated gas distribution. process systems is definitely the DO concentration,
which is essential for aerobic microorganism culti-
Prediction of DO distribution vation. To reveal the DO concentration fluctuations
in such systems, new experiments were designed
The main advantage for adopting the CFD and carried out in a typical bioprocess: phenol
model in this work was its ability to predict the lo- biodegradation by Candida tropicalis as described
cal and transient mass transfer characteristics of the by Feng et al.22 in this specific gas-induced pulsat-
gas-induced pulsating flow bubble column, for ex- ing flow bubble column reactor. Experiments were
ample, the DO concentration distribution in liquid done in two different cases: Case 1 that started from
phase within the column, as shown in Fig. 9, to fa- saturated DO concentration, or Case 2 that started
cilitates the understanding and controlling of the from zero DO concentration in the liquid phase as
corresponding chemical and biochemical processes, shown in Fig. 10. Comparisons were made between
which can cover the shortage of the experiments to the simulated reactor volume-averaged DO concen-
a large extent. trations calculated by the current model and the ex-
perimental data of the averaged value measured by
From this figure, it was observed that DO con- the two DO sensors. Differences were found
centrations increased with time, reaching an almost through the comparisons as the current model did
uniform distribution within the whole column (indi- not consider the bioreaction by the biomass
cated by the narrowing of the upper and lower lim- (Candida tropicalis) and the substrates (phenol and
its of the scales). The distribution of DO concentra- oxygen). In Case 1, the decrease in the DO concen-
tion along the vertical position is also reflected in tration as a result of biomass consumption was cap-
Fig. 9, whose values increased with height, making tured experimentally but was ignored in model sim-
the largest ones appear in the top region. This may
be mainly attributed to the better mixing of the two
phases, as well as a more sufficient mass transfer
along with the up-flow gas bubbles and developing
fluid flow. However, bubble coalescence had an op-
posite effect. Larger bubbles had smaller interfacial
area which was essential for oxygen mass transfer
between phases, thus the top and near-wall regions
of the column where larger bubbles accumulated
had lower interfacial area compared with the bot-
tom and middle regions of the column where
smaller bubbles had accumulated (as shown in Fig.
6), which significantly influences the DO distribu-
tion. It was noted that there was a close relationship
between the distribution of DO and the fluid flow,
which can be concluded by the non-symmetric dis- F i g . 1 0 – Model prediction and experimental measure-
tribution of dissolved oxygen concentration as the ment of DO concentration fluctuations under ug=0.01 m s–1
result of the wiggling of the bubble swarms. (Qp=2.52 m3 h–1 and Qb=0.18 m3 h–1) and f=1.25 Hz
174 Z. ZHOU et al., Experimental Study and CFD Simulation of Mass Transfer …, Chem. Biochem. Eng. Q. 27 (2) 167–175 (2013)
ulations, which only hold a constant value. In Case tion along with time and different location within
2, the increase in the DO concentration was both the column. Comparison between measured and
noticed in experiments as well as simulations. Be- simulated kla was done to validate the model. Er-
cause the oxygen bioreaction consumption rate was rors occurred but lied within a reasonable and ac-
much smaller than the mass transfer rate, the differ- ceptable range, which may be improved by better
ence between the experimental data and model pre- modeling strategies in future work. DO concentra-
dictions was not so obvious compared with Case 1. tion fluctuations in a real bioprocess system, phenol
Moreover, it could be confirmed in these experi- biodegradation by Candida tropicalis, were experi-
ments that the pulsating state flow with the fixed mentally investigated and the advantage of the
base flow rate of Qb=0.18 m3 h–1 and the pulsating gas-induced pulsating flow in supply of oxygen in
flow rate of Qp=2.52 m3 h–1 did have an advantage the liquid phase was confirmed.
in oxygen supply in the liquid phase in such a short
time (150 s) compared with the steady state flow
with the base flow rate of Qb=1.44 m3 h–1 and the ACKNOWLEDGEMENTS
pulsating state flow with equal base flow rate and This work was financially supported by the Na-
pulsating flow rate of Qb=Qb=0.96 m3 h–1 under the tional Natural Science Foundation of China (No.
same superficial gas velocity u=0.01 m s–1 and pul- 20906070) and the Seed Foundation of Tianjin Uni-
sating frequency of f=1.25 Hz in real bioprocess versity.
systems.
Symbols
Conclusions a - interfacial area, m–1
c - DO concentration, kg m–3
In this study, gas-liquid mass transfer charac-
cL - time dependent DO concentration, kg m–3
teristics in a gas-induced pulsating flow square
cross-sectioned bubble column was investigated for D - kinematic diffusivity, m2 s–1
the first time by both experimental measurement d - diameter, m
and model simulation. f - pulsating frequency, Hz
The effects of pulsating amplitude and fre- kl - liquid side mass transfer coefficient, m s–1
quency on kla were investigated experimentally, kla - volumetric mass transfer coefficient, s–1
and the bubble size distributions are given for dif- kla20°C- volumetric mass transfer coefficient at 20 °C, s–1
ferent air influx feedings with the same superficial Q - air flow rate, m3 h–1
gas velocity ug. It was found that there was a nota- S - bubble column cross-section area, m2
ble difference in the volumetric mass transfer coef- ScT - turbulence Schmidt number, defined as
ficient subjected to the steady and pulsating flows, ScT=mT/GT, default value of 0.9
which indicated the advantage for the adoption of T - pulsating cycle, s
the gas pulse operation. It was concluded that en-
Tl - operating water temperature, °C
hancement of kla could be achieved for the syn-
t - time, s
chronized change of base flow as well as pulsating
flow (Qp=Qb) with the same ug in comparison with ug - equivalent superficial gas velocity, m s–1
the steady state, especially under high ug. More- u - velocity vector, m s–1
over, kla in the gas-induced pulsating flow bubble x - mass fraction
column was found to be in negative linear correla-
tion with pulsating frequency.
Greek letters
In the hope of gaining more detailed insight
into the mechanism of such an unsteady pulsating a - holdup
operation, a three-dimensional CFD model cou- b - constant
pling of the MUSIG model considering bubble size G - mass transfer source term, kg m–3 s–1
distribution was developed to simulate the distribu- e - turbulence eddy dissipation, m2 s–3
tion of the strongly flow-dependent parameters, like
m - molecular viscosity, Pa s
interfacial area and liquid side mass transfer coeffi-
cient, which was surely to be a necessary and im- r - density, kg m–3
portant supplement to experimental technologies. tp - oxygen probe time constant, s
Furthermore, information of local and transient
mass transfer properties, such as dissolved oxygen
Superscript
in liquid phase, was also predicted by the proposed
model, giving a direct visualization of its distribu- * - saturation state
Z. ZHOU et al., Experimental Study and CFD Simulation of Mass Transfer …, Chem. Biochem. Eng. Q. 27 (2) 167–175 (2013) 175