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Characterization of Gas Transfer and

Mixing in a Bubble Column Equipped


with a Rubber Membrane Diffuser

Bjarne Rask Poulsen, Jens Jørgen Lønsmann Iversen

Institute of Biochemistry, Odense University, Campusvej 55, DK-5230


Odense M, Denmark; telephone: +45-6615-8600 (ext. 2376/2430);
fax: +45 6557 2467; e-mail: jjl.iversen@biochem.ou.dk
Received 20 June 1997; accepted 31 October 1997

Abstract: Gas transfer and mixing were characterized in the membrane are not clogged by suspended material and
a 32-L bubble column reactor equipped with a commer- microbial growth.
cially available rubber membrane diffuser. The perfor-
The aim of this work was to investigate the application of
mance of the membrane diffuser indicates that the slits
in the membrane are best described as holes with elastic these advantages of membrane diffusers in laboratory-scale
lids, acting as valves cutting off bubbles from the gas bioreactors.
stream. The membrane diffuser thus functions as a one-
way valve preventing backflow of liquid. Our design of
the bottom plate of the reactor enabled us to optimize the Comparative Studies
aeration by changing the tension of the membrane. We
thereby achieved mass transfer coefficients higher than Reports of similar work are scarce and difficult to find
those previously reported in bubble columns. A strong because a generally accepted name has not been given to
dependence of mass transfer on gas holdup and bubble membrane spargers. To our knowledge the use of commer-
size was indicated by estimates based on these two vari-
cially available membrane diffusers in bioreactors has not
ables. The microalga, Rhodomonas sp., sensitive to
chemical and physical stress, was maintained for 8 been reported.
months in continuous culture with a productivity identi- Rice et al. (1980) presented results obtained with diffus-
cal to cultures grown in stirred tank reactors. © 1998 John ers of their own construction using an ‘‘oscillating rubber
Wiley & Sons, Inc. Biotechnol Bioeng 58: 633–641, 1998. sheet sparger’’ in a bubble column. The gas holdup was
Keywords: bioreactor; elastic sparger; bubble size; oxy- doubled compared with a traditional ‘‘perforated plate
gen transfer efficiency; characteristic mixing time;
wrinkled bubbles sparger.’’ More detailed results were reported by Rice et al.
(1981) who used a 1.4-mm-thick vulcanized rubber sheet
with a diameter of 7.1 cm and 3.0 to 7.7 holes z cm−2 (the
INTRODUCTION diameter of the nails used to pierce the rubber sheet was 2.0
and 2.8 mm, respectively) in a 9.5-cm-inner-diameter
bubble column. They reported that these ‘‘flexible rubber
Rubber Membrane Spargers spargers’’ were self-cleaning due to oscillating hole size,
Membrane diffusers are often used to facilitate aerobic mi- produced a reduced bubble size, and allowed for signifi-
crobial degradation of organic material in biological waste- cantly higher gas rates and voidages (gas holdup) before
water treatment plants due to their efficient aeration. Dif- flooding occurred. They suggested that this was due to
fusers with perforated rubber membranes have several ad- ‘‘elastic holes’’ acting as valves or ‘‘knives’’ cutting off the
vantages compared with rigid spargers; small bubbles are air stream during bubble formation, and concluded that the
formed with high oxygen transfer rates due to a large inter- increased uniformity of bubbles reduced the axial mixing.
facial area between gas and liquid phases. Also, the pressure Later, Rice and Littlefield (1987) reported that an ideal
drop across the membrane is low compared with that of bubble flow (small uniform bubbles) was maintained at
rigid spargers. These characteristics are maintained at high relatively high superficial gas velocities with a ‘‘punctured
gas flow rates, giving competitive energy costs. Further- rubber membrane’’ in a bubble column giving minimal mix-
more, the membrane functions as a one-way valve prevent- ing.
ing backflow of liquid. Liquid is thus avoided in the gas Deckwer et al. (1982) measured the volumetric gas–
supply system and, in contrast to rigid spargers, the slits in liquid mass transfer coefficient, kLa (per second), obtained
with a ‘‘rubber plate distributor’’ made from a 2-mm-thick
rubber sheet with 6.5 holes z cm−2 (needle diameter 0.3 mm)
Correspondence to: J. J. L. Iversen
placed in a bubble column (14-cm inner diameter, 42-L
Contract grant sponsors: The Danish Research Councils; Novo Nor- liquid volume). The kLa (0.015 s−1 at superficial gas veloc-
disk A/S ity vs 4 0.02 m z s−1; method: gassing-in N2 in 0.7% CMC

© 1998 John Wiley & Sons, Inc. CCC 0006-3592/98/060633-09


solution) of this construction was approximately twice the pressure drop relationship. The Bernoulli relationship is
size of the value observed with perforated or sintered plates. modified to give the orifice equation (Rice and Howell,
Deckwer’s group also noticed that, with this rubber plate 1986):
distributor, clogging was avoided because of its elastic
Qo 4 Co z Ao z (2 z Dp/rg)1/2 (1)
properties. Medic et al. (1989) used a ‘‘perforated rubber
aeration pad’’ in a bubble column with a 2-m2 cross- where Qo (m3 z s−1) is the volumetric gas flow rate per ori-
sectional area and from 2 to 5 m of liquid above the mem- fice, Co (dimensionless) is the orifice coefficient, Ao (m2) is
brane. The aeration pad made from reinforced rubber of 1.5 the orifice area, Dp (Pa) is the pressure difference across the
mm thickness with 4 holes z cm−2 (1 mm approx. size, made membrane sparger, and rg (kg z m−3) is the gas density. If Co
with a needle) covered the entire bottom. They achieved is assumed to be constant it is seen from Eq. (1) that
higher kLa values (ca. 0.01 s−1 at vs 4 0.004 m z s−1; Qo z Dp−1/2 is proportional to the area of the hole. Rice et al.
method: sulfite oxidation in 2 mM sodium sulfite solution) (1981) observed a linear relationship between Qo z Dp−1/2
than expected from correlations obtained with other sparger and Dp and concluded that the hole area is proportional to
types. Weber et al. (1990) described a tubular ‘‘elastic the pressure difference across the membrane. Consequently,
sparger’’ made from 3.2-mm-thick natural latex rubber with the membrane is self-regulating: the hole area increases
12 holes z cm−2 (0.6 mm approx. slit size, made with a when increasing pressure is applied. The proportionality
needle). The kLa values (0.061 s−1 at vs 4 0.03 m z s−1; between Qo z Dp−1/2 and Dp for elastic holes observed by
method: gassing-out N2 in tap water, 9-L liquid volume) Rice et al. (1981) can be rewritten as a proportionality be-
were twice the values of a similar rigid sparger. They found tween Dp and Q2/3 o . From the experimentally observed lin-
no effect of prestretching the membrane in the longitudinal earity between Dp and Q2/3 o , Weber et al. (1990) also con-
direction of the slits. They observed that the enlargement of cluded that there was proportionality between the hole area
the orifices as gas pressure and flow rate increased delayed and the pressure difference across an ‘‘elastic sparger.’’ In
the onset of jetting, resulting in more uniform bubbles over comparison, Eq. (1) shows that, for rigid holes, Dp is pro-
a wider range of flow rates than with a rigid sparger. Only portional to Q2o because the hole area is constant.
one report (Talbot et al., 1990) has described a ‘‘porous
membrane diffuser’’ inferior to other spargers. Similar kLa
values (0.011 h−1 at vs 4 0.004 m z s−1; method: gassing-in Model Media
N2 in distilled water, 50-L liquid volume) were measured Equilibrium between coalescence and dispersion of bubbles
for the porous membrane and the porous plate investigated. is obtained so rapidly in coalescent liquids that formation of
The details of the membrane diffuser were not given, but a bubbles smaller than the equilibrium size will have no in-
slightly larger average bubble diameter was observed with fluence on the actual bubble size in the reactor (Heijnen and
the porous membrane as compared with the porous plate, in van’t Riet, 1984). Consequently, when characterization of
contrast to results obtained with other membrane diffusers. spargers is made in coalescent liquids the improved perfor-
Thus, apart from the results of Talbot et al. (1990) im- mance of a sparger due to formation of bubbles smaller than
proved mass transfer has been observed in all cases in which equilibrium size will not be observed. This is in agreement
membrane diffusers were compared with traditional rigid with observations by Bovonsombut et al. (1987), who found
spargers in bubble columns. This improvement is caused by that the improved mass transfer obtained with a porous plate
a reduction in bubble size, maintained at high gas velocities, relative to a perforated ring was more evident in noncoa-
thereby increasing the operational range of bubble columns. lescent liquid. A minimal medium for growth of heterotro-
However, most of the kLa values reported in these studies phic microorganisms is mostly coalescent, but, during batch
were relatively low and the improvement of gas transfer was culture, the broth often changes to mainly noncoalescent, as
always at the expense of mixing intensity. the result of the accumulation of metabolites excreted by the
microorganisms (Oolman and Blanch, 1986). Therefore,
Membrane Characteristics both coalescent and noncoalescent liquids were used to
characterize the performance of the rubber membrane in this
To explain the improved gas-transfer performance of mem- study.
brane spargers as compared with rigid spargers, Rice and
Howell (1986) developed an ‘‘elastic theory’’ by which the
shear modulus of ‘‘elastic membrane spargers’’ can be cal- MATERIALS AND METHODS
culated from the vertical displacement of the membrane at
the center and the pressure difference across the membrane. Bubble Column Reactor
They introduced this as an important element in membrane
sparger design. Geary and Rice (1991) predicted the bubble A perspex prototype bubble column was built in our work-
size from rigid and ‘‘flexible spargers,’’ but several vari- shop. It was 2 m high with an inner diameter of 15 cm and
ables have to be measured to use their theory. insertions for probes at 5 cm, 74 cm, 128 cm, and 197 cm
A more quantitative description of the excellent perfor- above the bottom plate. The maximal working volume was
mance of membrane spargers can be found in the flow rate– 32 L. As shown in Figure 1, the membrane sparger covered

634 BIOTECHNOLOGY AND BIOENGINEERING, VOL. 58, NO. 6, JUNE 20, 1998
between 0.5 and 1 s, placed 128 cm above the bottom plate.
pH was measured with two glass electrodes (GK4103C,
Radiometer, Copenhagen, Denmark) placed 5 cm and 197
cm above the bottom plate.

Photographs of Bubbles

Air bubbles were photographed in the bubble column using


a black background and light perpendicular to the direction
of photography from a 300-W video light (Type 8S, Kaiser
Fototechnik GmbH & Co., Buchen, Germany) connected to
an adjustable power supply. The lens used was a Micro
Nikor equipped with a filter (PL-linear M52, Nikon). Pic-
tures were taken using Fuji Neopan 1600 film (lens aperture
8, shutter speed 10−3 s). A ruler was placed on the outside
of the reactor wall for measurement of bubble size. There
was no optical distortion through the liquid and perspex in
the vertical direction and the distortion in the horizontal
direction was small (<2.5%) when bubbles near the reactor
Figure 1. Cross-section of lower part of bubble column. wall were photographed. This was confirmed by placing a
ruler in the liquid inside the bubble column.
the entire bottom of the reactor (aerated area Ai 4 170 cm2)
and consisted of a modified commercially available mem-
Measurement of Gas–Liquid Mass Transfer
brane diffuser, Sanitaire 99 (Water Pollution Control Corp,
WI), a 2-mm-thick EPDM rubber plate with 15 holes z cm−2 The dynamic methods for determination of kLa are based on
and a perforated area of 295 cm2. The holes in the mem- an abrupt formation of a difference between the oxygen
brane are slits of an approximate length of 1 mm cut in the concentration in the liquid in equilibrium with the gas phase
tangential direction. Before use, growth-inhibiting chemi- CG (mol z m−3) and the oxygen concentration in the liquid
cals in the membrane were removed by autoclaving in 5% CL (mol z m−3), followed by recording of CL. We deter-
Deconex (Borer Chemie AG, Zuchwil, Switzerland) solu- mined the kLa by two different dynamic methods: the stan-
tion and rinsed in distilled water. This was repeated three dard dynamic method (SDM), in which the sparger gas is
times. changed from atmospheric air to nitrogen or vice versa
The central part of the membrane was positioned as (Bartholomew et al., 1950); and the pressure step dynamic
shown in Figure 1. By moving the inlet up and down it was method (PDM; Linek et al., 1989), in which the pressure in
possible to change the tension of the membrane until the the reactor is abruptly changed by 20%. We obtained the
best performance was observed (i.e., the highest gas pressure changes by switching the outflow gas through a
holdup). column of liquid. Measurements using both SDM and PDM
Characterization was done at 20°C in distilled water and were automatized using an analog/digital interface (Degn
0.25 M NaCl as coalescent and noncoalescent liquids, re- and Nielsen, 1987) and an IBM-compatible computer run-
spectively (Oolman and Blanch, 1986). The gas flow rate ning specially written computer programs.
was controlled and measured with a mass flow controller
(Bronkhorst Hi-Tec, Type F-201AC-FD-44-V, Ruurlo, The
Netherlands). The liquid volume was between 25 and 31 L Measurement of Mixing Intensity
depending on the gas flow rate, which was varied between
5 and 30 L z min−1 corresponding to superficial gas veloci- Mixing was characterized using a buffer (2 mM succinate
ties between 0.006 and 0.033 m z s−1, respectively, and and malonate) in the model medium giving a linear rela-
power inputs per liquid volume between 100 and 650 tionship between the tracer concentrations (20 mL 1 M HCl
W z m−3, respectively. The superficial gas velocity is de- or NaOH ∼1 mM in the reactor) and pH (Poulsen and
fined as the gas flow rate divided by Ai and is equal to the Iversen, 1997). Acid and base reservoirs were pressurized to
gas velocity in the reactor without liquid. The gas holdup, e prevent formation of air bubbles in the tubings and to in-
(dimensionless), was determined from surface levels of crease the accuracy of tracer/titrant additions. The differ-
nonaerated liquid and dispersion as the ratio between the ence between the signals from two pH probes placed at the
volume of gas bubbles and the total volume of liquid and top and bottom of the reactor was used as the tracer signal.
gas (dispersion). The oxygen probe was a polarographic The characteristic mixing time, tM, was defined as the time
YSI-5331 oxygen probe with a YSI standard Teflon mem- constant of the exponential equation fitted to the response
brane (YSI Inc., Yellow Springs, OH), giving half-times curve (Poulsen and Iversen, 1997).

POULSEN AND IVERSEN: BUBBLE COLUMN EQUIPPED WITH A RUBBER MEMBRANE DIFFUSER 635
RESULTS AND DISCUSSION takes place when the local pressure difference is established
again, giving an oscillating behavior.

Mode of Action
Bubble Morphology
As seen in Figure 2, the membrane sparger described in this
study has a flow rate–pressure drop relationship character- Photographs were taken of air bubbles in coalescent and
istic for rigid spargers. This unexpected result is in contrast noncoalescent liquids (Figs. 3 and 4) in the bubble column.
to the observations of Rice et al. (1981) and Weber et al. As a consequence of coalescence the bubbles in distilled
(1990), who found a linear relationship between Dp and water are larger than the bubbles in the noncoalescent 0.25
Q2/3
o for their ‘‘elastic spargers.’’ Therefore, the holes in the
M sodium chloride solution. If the bubbles are assumed to
membrane used here are obviously not elastic. This can be be spherical the specific gas–liquid interfacial area per unit
explained by the membrane material, which is a hard rubber liquid volume, a (m−1), is given by:
(EPDM) as compared with the latex used by Weber et al.
AG
(1990). Co is assumed constant, but might vary due to a=
changes in the Reynolds number. However, it is unlikely VL
that this would give the exact flow rate–pressure drop rela- AG e
= ?
tionship characteristic of rigid spargers. VG ~1−e!
The critical pressure difference, Dpc (Pa), at which the (4p~db,i / 2!2 e
slits in the EPDM membrane open was 4.6 kPa (Fig. 2). = ?
3 ~1−e !
(4 / 3p~db,i / 2!
Weber et al. (1990) also reported threshold values for slit
opening (20 kPa). However, the total area of the holes did 6(d2b,i e
= ?
not increase significantly when the pressure difference (db,i
3 ~ 1−e !
across the sparger increased (Fig. 2). Therefore, we suggest 6 e
that the membrane slits can be described as holes with elas- = ? (2)
ds ~1−e!
tic lids, rather than elastic holes characterized by increasing
hole area at increasing pressure. This suggestion is in agree- where AG is the total interfacial area of bubbles, VL (m3)is
ment with the idea that the membrane slits act as valves, the liquid volume, VG is the total volume of bubbles, db,i (m)
cutting off bubbles during their birth process, thereby re- is the diameter of the ith bubble, and ds (m) is the Sauter
ducing bubble size (Rice et al., 1981). This ‘‘knife’’ action mean bubble diameter, often used to correlate bubble size
is possibly caused by a local pressure drop after the release with mass transfer:
of one bubble to a value below Dpc, which is, by definition,
insufficient to maintain an open hole/elastic lid. Reopening

Figure 2. Pressure difference across membrane sparger in bubble column


at different liquid volumes: s, 0 L; n, 5 L; ,, 10 L; L, 15 L; +, 25 L
(corresponding to hydrostatic pressures above the membrane of 0, 3.00,
6.15, 9.37, and 15.5 kPa, respectively). The equation Dp 4 c1 z Q2o + Dpc Figure 3. Photograph of air bubbles in coalescent liquid (distilled water)
is fitted to the results (z z z z), giving Dp 4 2.5 z 1014 kPa z m−6 z s2 z Q2o + 4.6 in bubble column at a superficial gas velocity of 0.0153 m z s−1. Bar 4
kPa; r2 4 0.96. 1 mm.

636 BIOTECHNOLOGY AND BIOENGINEERING, VOL. 58, NO. 6, JUNE 20, 1998
0.52 mm, respectively, and ds was 5.0 mm and 1.1 mm,
respectively (Table I). In a stagnant pool of water, these
Sauter mean bubble diameters were shown to give bubble
rise velocities vb (m z s−1) of around 0.25 m z s−1 and 0.20
m z s−1, respectively (Clift et al., 1978; Table I). The air
bubbles were not photographed at every superficial gas ve-
locity used, but we did not visually observe any difference
in bubble size except from a few large bubbles in the upper
part of the reactor at high gas velocities in the coalescent
liquid. In distilled water the bubbles were of approximately
the same size as in 0.25 M sodium-chloride close to the
membrane surface, but already at 5 cm above the membrane
the bubble size had stabilized to the equilibrium value char-
acteristic of the liquid. The formation of bubbles was there-
fore apparently independent of the liquid coalescence prop-
erties.
It is seen in Figure 3 that the bubbles in the coalescent
liquid are neither spherical nor ellipsoidal as usually as-
sumed. The shape is undefined and the surface is wrinkled,
increasing the surface area. This unusual surface pattern has
to our knowledge not been reported before, which can be
Figure 4. Photograph of air bubbles in noncoalescent liquid (0.25 M explained by our observation that the wrinkled surfaces
NaCl) in bubble column at a superficial gas velocity of 0.0153 m z s−1. Bar
4 1 mm.
(Fig. 3) are only seen when pictures are taken using light
perpendicularly directed to the focus line, in combination
with the filter as described in Materials and Methods. If the
(d3b,i filter is omitted the bubble surfaces appear normal (smooth)
ds = (3) on the photographs (not shown). The wrinkled bubble sur-
(d2b,i face is probably due to local microturbulence at the bubble
The Sauter mean bubble diameter (ds) is the diameter of a surface caused by the high bubble rise velocity characteris-
hypothetical bubble with a volume:area ratio equal to the tic of large bubbles. Turbulence is also created by high local
average ratio of all bubbles. We also calculated the mean densities of bubbles (bubble swarms), resulting in high local
bubble diameter dm: liquid velocities. The height of such local ‘‘airlifts’’ was
visually determined to be in the range of 5 to 20 cm. As a
(db,i result of wall effects the upward liquid velocity is highest in
dm = (4) the middle of the column.
N
In their study of aeration in bubble columns Heijnen and
where N is the number of bubbles. The different definitions van’t Riet (1984) distinguished between fine bubble sys-
(ds and dm) of average bubble diameter can give very dif- tems (small bubbles, 0.5 mm < ds < 1 mm) and coarse
ferent values. ds is always larger than or equal to dm. In bubble systems (large bubbles, 4 mm < ds < 6 mm). Fine
coalescent and noncoalescent liquids dm was 4.5 mm and bubble systems are obtained with porous discs, two-phase

Table I. Characteristic variables in coalescent and noncoalescent liquids.

Liquid

Variable Coalescent Noncoalescent Reference

ds 3.0 mm 1.0 mm Burckhart and Deckwer (1976)


ds 5.0 mm 1.1 mm This work
eest 4 s z m−1vs 5 s z m−1vs This work
e 0.6vs0.7 — Heijnen and van’t Riet (1984)
e 4.4 s z m−1vs 5.5 s z m−1vs This work
vb 0.25 m z s−1 0.20 m z s−1 Clift et al. (1978)
vb,ave 0.23 m z s−1 0.18 m z s−1 This work
(kLa)est 2.1 m−1vs z (1–4.4 s z m−1 vs)−1 4.5 m−1 vs z (1–5.5 s z m−1 vs)−1 This work
kLa 0.32 vs0.7 — Heijnen and van’t Riet (1984)
kLa 1.0 vs0.79 1.5 vs0.78 Burckhart and Deckwer (1976)
kLa 0.67 vs0.73 2.5 vs0.84 This work

POULSEN AND IVERSEN: BUBBLE COLUMN EQUIPPED WITH A RUBBER MEMBRANE DIFFUSER 637
ejectors–injectors (gas and liquid are concurrently pumped cial gas velocity and gas holdup (equal to assuming constant
through a nozzle), or membrane spargers (as in this study) vb,ave) it is concluded that a homogeneous flow regime is
in noncoalescent liquids or at relatively low superficial gas obtained (Fig. 5), giving vb,ave 4 0.23 m z s−1 and vb,ave 4
velocities in coalescent liquids. Coarse bubble systems are 0.18 m z s−1 in the coalescent and noncoalescent liquid, re-
obtained in both types of liquid by sparging through holes spectively.
larger than 1 mm as in most ring spargers or perforated
plates.
Gas–Liquid Mass Transfer Coefficient Measured
by Dynamic Methods
Comparison of Measured and Estimated
Gas Holdup Measurements of kLa using two methods are shown in Fig-
ure 6. Values based on pressure change (PDM), where the
Gas holdup measured volumetrically as described in Mate- change in CG is most abrupt, are expected to be somewhat
rials and Methods is increased by 25% in the noncoalescent higher than the values determined by change in gas com-
liquid (0.25 M NaCl) compared with the coalescent liquid position (SDM). When the rate of change in CG is low
(distilled water, see Fig. 5). This number is twice the in- compared with the mass transfer, as in the case of SDM, the
crease reported by Bello et al. (1985) (using a perforated time course of CL, which is used for determination of kLa,
plate) reflecting the formation of small bubbles by the mem- will be a result of both the rates of mass transfer and change
brane sparger—a characteristic which is less obvious in the in CG. The effect of the latter change is of course more
coalescent liquid. In spite of this, our values for the coales- pronounced at high kLa values, in agreement with the results
cent liquid (coarse bubbles) are high compared with other in Figure 6.
systems (Bello et al., 1985; Heijnen and van’t Riet, 1984). Heijnen and van’t Riet (1984) derived a power law cor-
In the homogeneous flow regime gas holdup depends relation for coarse bubble systems obtained with different
linearly on gas velocity (Deckwer and Schumpe, 1993) and conventional rigid spargers in water: kLa (20°C) 4 0.32vs0.7
can be estimated from Eq. (5) using the bubble rise velocity (different methods). The power law correlation obtained
predicted from the Sauter mean bubble diameter as the av- here for the coalescent liquid (kLa 4 0.67vs0.73; Table I)
erage bubble rise velocity, vb,ave. The gas holdup estimated shows an increase in kLa, but almost the same dependency
this way, eest (dimensionless), is 4 s z m−1 vs and 5 s z m−1 vs on vs.
in the coalescent and noncoalescent liquid, respectively The kLa values in the noncoalescent liquid (Fig. 6) are
(Table I), because the bubble rise velocity predicted from higher than, but in the range of, the values previously pub-
the Sauter mean bubble diameter in a stagnant liquid is 0.25 lished in fine bubble systems (Onken and Weiland, 1983;
m z s−1 and 0.20 m z s−1 (Clift et al., 1978), respectively. Heijnen and van’t Riet, 1984; kLa determined with different
e 4 vs/vb,ave (5) methods). Burckhart and Deckwer (1976) found a power
law correlation, kLa 4 1.5vs0.78 (method: gassing-in/out N2,
In a heterogeneous flow regime, the correlation between e 78-L liquid volume), for a sintered plate sparger in NaCl
and vs is given by e 4 0.6vs0.7 (Heijnen and van’t Riet,
1984). From the direct proportionality between the superfi-

Figure 6. Mass transfer coefficient kLa in distilled water and 0.25 M


NaCl measured with the standard dynamic method (SDM) and pressure
step dynamic method (PDM): h, distilled water PDM; L, distilled water
Figure 5. Gas holdup in distilled water (h) and 0.25 M NaCl (,) as a SDM; ,, 0.25 M NaCl PDM; n, 0.25 M NaCl SDM. Solid lines are power
function of superficial gas velocity. Lines are the equation e 4 c2 z vs fitted laws fitted to PDM results: kLa 4 0.67vs0.73, r2 4 0.986 (h) and kLa 4
to the results, giving e 4 4.4 s z m−1 vs, r2 4 0.996 (h) and e 4 5.5 s z m−1 2.5vs0.84, r2 4 0.990 (,). Dashed lines are estimates of kLa from gas
vs, r2 4 0.996 (,). holdup and bubble size [Eqs. (6) and (7)].

638 BIOTECHNOLOGY AND BIOENGINEERING, VOL. 58, NO. 6, JUNE 20, 1998
solutions. Our correlation in noncoalescent liquid shows an (>400%) even when the value of C was set to zero, which
increase in kLa and a minor increase in the dependency on indicates too strong dependency on ds (ds−3/2).
vs (kLa 4 2.5vs0.84; Table I). Bello et al. (1985) found kLa
values for a perforated plate (conventional rigid sparger) in
a ‘‘bubble coalescence-inhibiting system’’ of 0.15 M NaCl Oxygen Transfer Efficiency
(method: gassing-in/out N2, 30-L liquid volume) of only The mass transfer coefficients reported in Figure 6 are high
40% to 50% of the values obtained in this report. compared with literature values, emphasizing the capacity
Again, it is noteworthy that the different methods used of the membrane to produce small bubbles. Small bubbles
make a direct comparison difficult. However, it is obvious affect a positively by increasing AG and residence time.
that the PDM is the most reliable method for reactors with They affect kL negatively via a low vb, which decreases
slow exchange of the gas phase in agreement with the sug- mixing of gas and liquid interfaces. However, kLa increases
gestion of Linek et al. (1990). with decreasing bubble diameter in the range of bubble
diameters studied here. The superior performance in terms
Gas–Liquid Mass Transfer Coefficient Estimated of gas transfer is seen more clearly from kLa values than
from Bubble Size and Gas Holdup from gas holdup values. This confirms that the mass transfer
coefficient is the most important variable for description of
The volumetric gas–liquid mass transfer coefficient can be aeration. Oxygen transfer efficiency, OTE (kg O2 z kWh−1),
estimated from bubble size (ds) and gas holdup. The liquid is commonly used in the industry to describe power con-
mass transfer coefficient kL (m z s−1) is approximately sumption. When CL 4 0, it attains its maximal value:
4 z 10−4 m z s−1 at Sauter mean bubble diameters above 2
mm, and around 1.5 z 10−4 m z s−1 at a Sauter mean bubble kLa ? CG ? VL
OTE = (9)
diameter of 1 mm (Heijnen and van’t Riet, 1984). However, P
it most be noted that the variations in kL determinations are
where P (W) is the power consumption of the air pump
inherently high. It is obvious from Figure 3 that a is under-
calculated from the measured pressure of the incoming gas,
estimated if it is calculated assuming spherical bubbles in
pg (Pa), assuming a pumping efficiency of 63%:
the case of coalescent liquids. However, it seems to be a
good approximation in the case of noncoalescent liquids. A vs ? Ai ? pamb ? ln~pg / pamb!
direct proportionality between vs and e was found in Figure P= (10)
0.63
5. By substitution of e 4 4.4 s z m−1 vs (coalescent liquid)
or e 4 5.5 s z m−1 vs (noncoalescent liquid) into Eq. (2), a where pamb (Pa) is ambient pressure. Our results expressed
can be estimated as a function of vs. This gives: as OTE are shown in Figure 7. Only a few values of OTE are
given in the literature. Calculation of OTE based on pub-
(kLa)est (coalescent) 4 2.1 m−1vs z (1 − 4.4 s z m−1vs)−1 (6) lished kLa values is essentially impossible because informa-
(kLa)est (noncoalescent) 4 tion about the power consumption is not provided or the
4.5 m−1 vs z (1 − 5.5 s z m−1 vs)−1 (7) term is defined in various ways. Therefore, a comparison
with literature values is difficult. However, it is noteworthy
Estimated and measured mass transfer coefficients are simi- that the decrease in OTE with increasing vs is small.
lar in the coalescent and noncoalescent liquids (Fig. 6).
Because the interfacial area, a, was underestimated in the
case of coalescent liquid, due to the irregular shape and
surface of the bubbles (Fig. 3), it follows that kL has been
overestimated.
Ayazi Shamlou et al. (1995) found that kLa also is highly
dependent on ds in an airlift reactor and suggested that kLa
is given by:

kLa 4 12(D/p)1/2 z [vb + C z (vs,r + vL,r)]1/2


z ds−3/2 z e(1 − e)−3/2 (8)

where D (m2 z s−1) is the diffusion coefficient, C (dimen-


sionless) is the distribution parameter dependent on the type
of sparger, vs,r (m z s−1) is the superficial liquid velocity in
the riser. We exchanged vs,r with vs and used the values 1,
0, and 2.0 z 10−9 m2 z s−1 for C, vL,r, and D, respectively, and
found kLa values almost identical to our estimated values for
the coalescent liquid (within 8%). However, for the non- Figure 7. OTE in distilled water (h) and 0.25 M NaCl (,). CG 4 240
coalescent liquid, Eq. (8) gave highly overestimated values mM was used.

POULSEN AND IVERSEN: BUBBLE COLUMN EQUIPPED WITH A RUBBER MEMBRANE DIFFUSER 639
Mixing Intensity teristic of rigid spargers, in contrast to results from other
In parallel to the increase in mass transfer with smaller reports on ‘‘elastic spargers.’’ This can be explained by the
bubble diameters a decrease in mixing efficiency was seen, hard rubber material of the membrane. In spite of this, the
as expected (Fig. 8). The increase in mixing time as a result membrane diffuser produced very small bubbles over a
of the small bubbles characteristic of the noncoalescent liq- wide range of superficial gas velocities. Bubble formation in
uid is an order of magnitude larger compared with the co- this membrane is therefore not dependent on an increasing
alescent liquid. Similar results were described by Rice et al. area of holes with increasing flow rate. A possible expla-
(1981) and Rice and Littlefield (1987). The low mixing nation of this phenomenon is that the elastic holes act as
intensity in the noncoalescent liquid shows that the liquid valves dividing the gas stream into very small bubbles. We
flow is uniform and laminar, as expected from Figure 4, achieved mass transfer coefficients higher than those previ-
whereas it is turbulent in the coalescent liquid, as expected ously obtained in bubble columns, irrespective of aeration
from Figure 3. method. There are probably two reasons for this result: first,
our design enabled us to change the tension of the mem-
brane in a direction transverse to the slits; and second, the
Growth Experiments
intrinsic properties of the membrane were superior to those
The rubber membrane sparger described here has been used used by other workers. kLa could be reasonably well esti-
successfully in a bubble column. The simplicity of the me- mated from measured values of gas holdup and bubble size
chanical construction of the bubble column in combination and literature values of kL. The observed mixing intensity
with the self-cleaning property of the membrane sparger was very low. However, considering the high mass transfer,
allowed us to maintain the microalga Rhodomonas sp. in low energy costs, extremely low physical stress, and low
continuous culture for 8 months without interruption (de- maintenance, this bioreactor is competitive with not only
tails to be described elsewhere). Rhodomonas sp. is sensi- other bubble column reactors, but also stirred tank reactors.
tive to chemical and physical stress, but the yield coeffi-
cients obtained with the bubble column described in this We thank Raymond P. Cox for criticism and reading of the
study were identical to cultures grown in conventional bio- manuscript, and Svend Åge Madsen for technical assistance.
reactors (Eriksen and Iversen, 1995), ruling out any inhibi-
tory effects of the membrane material when treated as de-
scribed in Materials and Methods. NOMENCLATURE
The productivity of the bubble column was 4 z 109
cells z L−1 z day−1. The algae were used as feed for marine a specific gas–liquid interfacial area per unit liquid volume
(m−1)
invertebrates in bioenergetic studies of suspension feeding AG total area of gas bubbles (m2)
and growth (Eriksen and Iversen, 1997; Nielsen et al., 1995; Ai inner area of bubble column reactor (m2)
Thomassen and Riisgaard, 1995). The application of such A0 area of orifice (m2)
studies is important in aquaculture. c1 correlation factor (Pa z m−6 z s2)
c2 correlation factor (s z m−1)
C distribution parameter (dimensionless)
CONCLUSIONS Co orifice coefficient (dimensionless)
With the rubber membrane diffuser used in this study we CL oxygen concentration in liquid (mol z m−3)
CG oxygen concentration in liquid in equilibrium with gas phase
found the gas flow rate–pressure drop relationship charac- (mol z m−3)
db,i bubble diameter of ith bubble (m)
dm mean bubble diameter (m)
ds Sauter mean bubble diameter (m)
D diffusion coefficient (m2 z s−1)
kL liquid mass transfer coefficient (m z s−1)
kLa volumetric gas-liquid mass transfer coefficient (s−1)
(kLa)est estimated volumetric gas-liquid mass transfer coefficient (s−1)
N number of bubbles (dimensionless)
OTE oxygen transfer efficiency (kg O2 z kwh−1)
pamb ambient pressure (Pa)
pg pressure of incoming gas (Pa)
Dp pressure difference across sparger (Pa)
Dpc critical pressure difference across sparger (Pa)
P compressor power input (W)
Qo volumetric gas flow rate per orifice (m3 z s−1)
tM characteristic mixing time (s)
vb bubble rise velocity (m z s−1)
vb,ave average bubble rise velocity (m z s−1)
vL,r superficial liquid velocity in the riser (m z s−1)
vs superficial gas velocity (m z s−1)
Figure 8. Characteristic mixing time, tM, in distilled water (h) and 0.25 vs,r superficial gas velocity in the riser (m z s−1)
M NaCl (,). VG total volume of bubbles (m3)

640 BIOTECHNOLOGY AND BIOENGINEERING, VOL. 58, NO. 6, JUNE 20, 1998
VL volume of liquid in reactor (m3) Heijnen, J. J., van’t Riet, K. 1984. Mass transfer, mixing and heat transfer
phenomena in low viscosity bubble column reactors. Chem. Eng. J. 28:
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eest estimated gas holdup (dimensionless) technol. Bioeng. 35: 766–770.
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measurement in large-scale bioreactors. Biotechnol. Bioeng. 33:
1406–1412.
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POULSEN AND IVERSEN: BUBBLE COLUMN EQUIPPED WITH A RUBBER MEMBRANE DIFFUSER 641

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