Chemical Engineering and Processing 43 (2004) 1511–1517

Gas–liquid mass transfer coefficient in stirred tanks interpreted through

models of idealized eddy structure of turbulence in the bubble vicinity
V. Linek∗ , M. Kordač, M. Fujasová, T. Moucha
Department of Chemical Engineering, Prague Institute of Chemical Technology, Technická 5, CZ-166 28 Prague 6, Czech Republic

Received 9 September 2003; received in revised form 26 September 2003; accepted 10 February 2004
Available online 24 April 2004

Abstract

Experimental data on the average mass transfer liquid film coefficient (kL ) in an aerated tank stirred by two Rushton turbines on common
shaft are presented. Liquid media used were distilled water and 0.5 M sodium sulphate solution. Volumetric mass transfer coefficient (kL a)
was measured by the dynamic pressure method with pure oxygen absorption. Specific interfacial area a was taken from Alves et al. [Chem.
Eng. Proc., in press] who measured data on local gas hold-up and local average bubble diameter in the same apparatus and batches. Values
of kL are quantitatively interpreted in terms of correlations based on idealized eddy structures of turbulence in the bubble vicinity, namely by
“eddy” model by Lamont and Scott [AIChE J. 16 (1970) 513] in the form of kL = 0.523(eν/ρ)0.25 (D/ν)1/2 , which fits the data with the mean
deviation of 4.7%. It is shown that the decisive quantity to correlate kL in the stirred tank is power dissipated in the liquid phase rather than
the bubble diameter and the slip velocity as assumed by Alves et al.
© 2004 Elsevier B.V. All rights reserved.

Keywords: Mass transfer coefficient; Bubble; Dynamic pressure method

1. Introduction surface due to the contamination), kL is (according to Alves

et al. [3]) given by the equation proposed by Frössling [1]
Mass transfer from swarm of bubbles into turbulent liq-

vsl 2/3 −1/6
uid controls the rate of many chemical and biochemical pro- kL = c1 D ν (1)
cesses; hence many papers were devoted to the problem. In d
spite of this, the mechanism of the transfer remains uncer- or (according to Calderbank and Moo-Young [2]) by the
tain. Various widely different, but yet partially successful, relation
approaches exist. They predict different, often contradictory,    
influence of operational conditions on mass transfer coeffi- ρνg 1/3 D 2/3
kL = 0.31 (2)
cient kL . Two of the most frequently used concepts assume ρ ν
the mechanism of mass transport in the liquid phase is due
to a renewal of the liquid at the bubble surface. For the bubbles that have completely mobile surface (large
The first group of the models (“slip velocity” models) as- bubbles in pure liquid or fresh bubble), Alves et al. [3] have
sumes a gross mean flow of fluid relative to the bubble (slip proposed for calculation of kL the equation, which follows
velocity) and a bubble surface rigidity control of this re- from the well-known penetration model with exposition time
newal. The surface rigidity depends on bubble size (accord- equal to d/vsl
ing to Calderbank and Moo-Young [2]) or on a degree of the

vsl 1/2
bubble surface contamination by surface-active impurities kL = 1.13 D (3)
(according to Alves et al. [3]). For the rigid bubbles (small d
bubbles d < 1 mm or bubbles with completely immobile and Calderbank and Moo-Young [2] have proposed the re-
lation
   
∗ Corresponding author. Tel.: +42-2-24353298; fax: +42-2-3117335. ρνg 1/3 D 1/2
kL = 0.42 (4)
E-mail address: linekv@vscht.cz (V. Linek). ρ ν

0255-2701/$ – see front matter © 2004 Elsevier B.V. All rights reserved.
doi:10.1016/j.cep.2004.02.009
1512 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517
Gas–liquid slip velocities vsl are assumed to be close to
single bubble terminal velocities, vt , in still water on which
a correction for turbulence is introduced [3].
The second group of models (“eddy” models) assumes
that this renewal is due to the small scale eddies of the
turbulent field rather than to any gross mean flow of fluid
relative to the bubble. The models are based on idealized
eddy structures of turbulence in the bubble vicinity. Lamont
and Scott [4] assumed that the mass transfer in the liquid
is affected preponderantly by the small scales of turbulent
motion (the scales extend from the smallest viscous motions
into the inertial motions). In any case, these motions are
much smaller in scale than the gas bubbles and they “attack”
the surface of bubbles in the same way from any direction.
As a result, the size of the gas bubble is not a very critical
parameter for the estimation of kL . They deduced [4] the
following relation for kL
 1/4  1/2
eν D
kL = c5 (5)
ρ ν
Different authors predict different values of the constant c5 :
0.301 [5], 0.4 [4], 0.592 [6], 1.13 [7].
These two groups of models are contradictory. The “eddy”
models predict an increase while the “slip velocity” mod-
els a decrease of kL with increasing turbulence intensity,
i.e. with increasing power dissipated in the liquid. This is
due to the fact, that kL from rigid bubbles is lower than
from the ones with a mobile surface by a factor around 5.
The small bubbles, which either have lower kL (according
to Calderbank’ variant of “slip velocity” models) or become
rigid more quickly (according to Alves’ variant) are gener-
ated in larger amount just at higher turbulence intensities. As
a result this leads to the decrease of average mass transfer
coefficient in dispersion with increasing power dissipated in
the liquid. Literature data on kL in stirred tanks supporting
both these models can be found. Contradictory results on the
mass transfer coefficients kL determined by various authors
can be partially explained by errors in kL a values used in
their evaluation from the relation kL = kL a/a. It was shown
[8], that the kL a values measured by dynamic methods based
on the inlet gas exchange at high mixing intensities are un-
derestimated even by multiples due to an incorrect flow pat-
tern of gas phase used in the model for the kL a evaluation. It
was demonstrated [8] on the data of different authors [9,10]
that the reported decrease of kL with increasing power input
dissipation in the liquid does not reflect real phenomena but
is only the result of error in the measuring methods of kL a
at high mixing intensities.
Alves et al. [3] presented data on kL in a double Rushton
turbine stirred tank. Their experimental kL falls between the
limits defined by Eqs. (1) and (3), which differ by a factor
around 5. The data are quantitatively interpreted in terms of
bubble contamination kinetics, using a stagnant cap model,
according to which bubbles suddenly change from a mobile
interface to a rigid condition when surface tension gradients,
caused by surfactant accumulation, balance out shear stress.
The overall volumetric mass transfer coefficients kL a were
measured by the peroxide decomposition steady-state tech-
nique with air as a gas phase. It was shown [11], however,
that the steady-state methods with air absorption/desorption
gives substantially lower kL a values at high mixing intensi-
ties as compared to pure oxygen absorption.
Aim of this paper is to show that if the overall volu-
metric mass transfer coefficients kL a are measured by the
non-problematic pressure dynamic method [12] with pure
oxygen absorption in the same apparatus as Alves, the rel-
evant kL data are well interpreted in terms of the “eddy”
model by Lamont and Scott [4]. The paper should support
opinion that the decisive quantity to correlate kL in stirred
tanks is power dissipated in the liquid phase rather than the
bubble diameter and their slip velocity.
2. Experimental
The experiments were performed in a fully baffled (four
baffles, 1/10 of the vessel diameter width) cylindrical ves-
sel of i.d. 0.29 m equipped with two standard Rushton tur-
bines. The impeller diameter was equal to 1/3 of the tank
diameter as well as the bottom impeller clearance and the
inter-impeller distance was equal to the tank diameter. An
aeration gas was introduced 2 cm under the bottom im-
peller through a ring distributor with diameter 4 cm and with
nine orifices (1 mm in diameter). The membrane-covered
polarographic type oxygen probes were located in the liq-
uid batch at the impeller’s planes. A sketch of the vessel
indicating locations of oxygen probes is in Fig. 1. The ex-
periments were performed in distilled water and in 0.5 M
Na2 SO4 aqueous solution, which represents non-viscous co-
alescent and non-coalescent batch, respectively. The vessel
was filled with the liquid to the height of two times the ves-
sel diameter. Superficial velocities of aeration gas (air in the
measurements of power and gas hold-up, pure oxygen in
the measurements of volumetric mass transfer coefficient)
were 2.12, 4.24 or 8.48 mm s−1 . The experiments were per-
formed in the impeller speed range from 4.17 to 14.17 s−1
at 20 ◦ C.
The impeller power was measured by a strain gauge on the
impeller shaft. The gas hold-up was determined by visual in-
spection from the difference between the batch level height
with and without aeration. The volumetric mass transfer
coefficient was measured by the dynamic pressure method
(DPM) described earlier [12]. Physical correctness of the
method has been verified by the agreement between kL a
measured by absorption of air and pure oxygen: physically
consistent kL a data should not depend on the driving force
of the absorption, i.e., the kL a values should be the same no
matter what oxygen concentration in aeration gas is used.
The principle of the DPM lies in the fast change of the to-
tal pressure in the vessel and the consequent recording the
oxygen probes response in liquid phase in both stages. In
evaluation of the kL a the dynamic of the oxygen probes was
 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517 1513

Table 1
Parameters C1 , C2 and C3 in correlations (6), (8) and (9) obtained by the
experimental data regression
Batch C1 C2 C3 S.D. (%)

Specific power dissipated by agitators, correlation (6)

Water 0.155 3.141 −0.365 4.6
0.5 M Na2 SO4 0.208 2.932 −0.393 5.2
Gas hold-up, correlation (8)
Water 0.2346 0.3091 0.7347 5.6
0.5 M Na2 SO4 0.0505 0.4903 0.5788 9.3
Volumetric mass transfer coefficient, correlation (9)
Water 0.0108 0.699 0.581 9.6
0.5 M Na2 SO4 0.978E−3 1.233 0.55 10

3.2. Gas hold-up

The gas hold-up as a function of the specific power dissi-

pated by agitators in the liquid and superficial gas velocity
was fitted by empirical relation
ε = C1 (eagit )C2 vC
s
3 (8)

The parameters C1 , C2 and C3 obtained by the experimental

data regression are given for both batches used in Table 1.

3.3. Volumetric mass transfer coefficient

The overall volumetric mass transfer coefficients were

Fig. 1. Scheme of the apparatus.
taken into account [12] and the kL a value for each stage
of the vessel was evaluated. Fast response oxygen probes
with time constants above 0.8 s−1 were used (polypropylene
membrane, 10 ␮m thick). An average kL a value was calcu-
lated as an arithmetic mean of both stage values. The arith-
metic mean was used as it was shown [13] that its value is
not affected by axial dispersion of both phases.
3. Results
3.1. Power dissipated
The specific power dissipated by agitators in the liquid
was well fitted by the following relations
eagit = C1 N C2 vC
s
3 (6)
The parameters C1 , C2 and C3 obtained by the experi-
mental data regression are given for both batches used in
Table 1. These empirical correlations fit the experimental
data with high accuracy (standard deviations lower than 5%,
see Table 1). The total specific power dissipated in the liquid
by agitator and by rising bubbles was calculated from
e = eagit + ρgvs (7)
expressed as a function of the total specific power dissipated
in the liquid and gas superficial velocity as follows (the usage
of e gave closer correlation than the usage of an agitator
power eagit )
kL a = C1 eC2 vC
s
3 (9)
C1 , C2 and C3 values are given for both batches in Table 1.
Experimental data are fitted with the correlations very well
as is demonstrated in Fig. 2. Standard deviation of the data
is 10%.
The overall volumetric mass transfer coefficients were
measured by Alves et al. [3] using the peroxide decomposi-
tion steady-state technique with manganese dioxide as the
catalyst in the same apparatus as it is used in this work.
The only difference is higher bottom impeller clearance
(0.146 m instead of 0.097 m). Such small difference has
inexpressive effect on mass transfer characteristics of dis-
persion. Operational conditions used in this work (impeller
speed 4.17–14.17 s−1 , gas superficial velocity 0.00212,
0.00424 and 0.00848 m s−1 ) fully overlap the conditions
under which Alves et al. [3] performed their experiments
(impeller speed 4.2–10 s−1 , gas superficial velocity 0.00249
and 0.00497 m s−1 ). The liquid media used by Alves were
water and 0.3 M aqueous solution of Na2 SO4 . In this work
0.5 M solution of Na2 SO4 is used. It is well known that
the addition of an electrolyte to water reduces the rate of
bubble coalescence resulting in an increase in kL a up to a
limiting concentration beyond which a further increase in
1514 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517

evaluation of the characteristics at operational conditions at

which Alves et al. [3] performed their measurement.
Table 2 brings together average tank data on operational
conditions, gas hold-up, bubble diameter, specific area and
volumetric mass transfer coefficients measured by Alves and
those calculated from correlations (6) to (9). There is very
good agreement in gas hold-up values but there is strong
disagreement in volumetric mass transfer coefficients. kL a
values calculated from correlation (9) are up to six times
higher than Alves’ kL a data. The reliability of our data (9)
on kL a measured in two-impeller configuration supports the
agreement with those determined [11] in one-impeller con-
figuration by dynamic pressure method for air and pure oxy-
gen absorption and by steady-state sulphite feeding method
for pure oxygen absorption. The one-impeller data were cor-
related [11] by the equation
kL a = 3.11 × 10−4 e1.24 v0.4
s (10)

which gives up to 20% higher data compared to Eq. (9).

Possible reasons for too low kL a values measured by
Fig. 2. Comparison of kL a data with the correlation (9).
Alves et al. [3] in comparison with our data are 2:

electrolyte concentration no longer has an effect on kL a.
The concentrations 0.5 and 0.3 M are higher than the limit-
ing value for Na2 SO4 . This follows from Fig. 3, where kL a
data measured [14] by dynamic start-up method 0 → O2
(the batch is degassed at the beginning of experiment) in
one-impeller configuration in sodium sulphate solutions of
different concentrations are compared: kL a data produced
in stirred vessel in 0.5 and 0.2 M Na2 SO4 do not differ.
All these facts support conclusion that the correlations
presented in this paper for e, ε and kL a can be used for
(ii) Presence of magnesium dioxide in dispersion (in a form
Fig. 3. Comparison of kL a data measured by Linek et al. [14] in
one-impeller configuration by start-up dynamic method in sodium sul-
phate solution of various concentrations.
(i) It was shown [11] that steady-state sulphite feeding
method for air absorption gives kL a values substan-
tially lower (two times) than those for pure oxygen ab-
sorption in the region of kL a > 0.1 s−1 . This is caused
by the fact that the residence times of individual bub-
bles differ considerably. The small bubbles, with lower
tendency to coalesce, stay in the reactor significantly
longer than the mean residence time and have higher
surface to volume ratio. During absorption of a diluted
gas, a part of bubbles is therefore formed in the ves-
sel, the content of which is in equilibrium with the sur-
rounding liquid and which is ineffective with respect
to absorption. As a result, kL a data measured by di-
luted gas are lower because they do not include these
bubbles. In other words, the interfacial area a in kL a
values measured by diluted gas (air) is not a geometric
surface area of all the bubbles in dispersion but only
its part that is effective in the mass transfer. The geo-
metric surface area of all bubbles is active only in the
kL a data measurement by some steady-state methods
with pure oxygen absorption or by the pressure dy-
namic method regardless whether air or pure oxygen
absorption is used.
of fine powder of approximately 20 ␮m Sauter mean
diameter at the concentration of 0.8 g l−1 [15]) can en-
hance the rate of bubble coalescence and as a result may
diminish interfacial area. It was shown [15] that MnO2
does not influence kL a values in coalescent batch of
water. In non-coalescent batches, however, MnO2 may
enhance the bubble coalescence significantly. The kL a
values measured by Alves et al. [3] in sulphate solution
are as low as they correspond rather to water (coales-
cent batch) than to non-coalescent batches. Compare
 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517 1515

Table 2
Average tank data on operational conditions, gas hold-up, bubble diameter, specific area and volumetric mass transfer coefficients measured by Alves
et al. [3] and those calculated from correlations (6) to (9)
Batch N (s−1 ) vs e (W m−3 ) d23 (mm) a (m−1 ) ε (×102 ) kL a (×102 s−1 ) kL (×104 m s−1 )
(mm s−1 ) (this work) (Ref. [3]) (Ref. [3])
Ref. [3] This work Ref. [3] This work Ref. [3] This work

0.3 M Na2 SO4 4.2 2.49 173 2.3 47 1.8 1.8 0.80 2.08 1.69 4.42
0.3 M Na2 SO4 5.0 2.49 271 1.67 78 2.2 2.3 1.3 3.61 1.66 4.63
0.3 M Na2 SO4 6.3 2.49 510 1.52 135 3.3 3.3 2.8 7.88 2.07 5.84
0.3 M Na2 SO4 7.5 2.49 832 1.24 213 4.4 4.2 3.0 14.4 1.41 6.77
0.3 M Na2 SO4 10.0 2.49 1901 0.9 512 7.2 6.3 6.2 39.9 1.21 7.80
0.3 M Na2 SO4 7.5 4.97 666 1.34 233 5.0 5.5 3.0 16.0 1.29 6.88
Water 7.5 2.49 800 2.89 53 2.5 2.3 1.7 3.54 3.19 6.89

Alves’ kL a value 0.062 s−1 for sulphate solution with from the pertinent kL a-values. The resulting kL values are
kL a = 0.066 s−1 for water calculated from correlations plotted against total power dissipated in the liquid in Fig. 4.
(6) through (9) at N = 10 s−1 and vs = 0.00249 m s−1 . Our kL data for all batches are well fitted by equation
 0.244  1/2
eν D
kL = 0.48 (11)
3.4. Specific interfacial area ρ ν
with the mean deviation of 4.6%. If the theoretical value 1/4
The specific interfacial area was measured by Alves et al.
of the power exponent is used the equation changes to
[3]. They measured local gas hold-up and local bubble size
 1/4  1/2
in 33 points in the vessel. From these local data they cal- eν D
culated the average gas hold-ups ε and interfacial areas a, kL = 0.523 (12)
ρ ν
which are shown in Table 2. The batches in which the mea-
surements were performed did not contain catalyst MnO2 . with the mean deviation of 4.7%. Similar correlation of
Area measured by the method represents geometric surface Alves’ kL -data yields
of all bubbles in dispersion.  −0.0497  1/2
−3 eν D
kL = 2.16 × 10 (13)
ρ ν
3.5. Mass transfer coefficient
with the mean deviation of 24.4%. In contradiction to our
Mass transfer coefficients calculated by the ratio kL a/a are data Alves’ data show a weak fall with increasing power
given in Table 2. kL a values calculated from correlation (9) dissipated in the liquid.
were up to six times higher than Alves’ kL a data. Accord- In Fig. 5, our and Alves’ kL data are plotted against bub-
ingly, the same disagreement exists between kL calculated ble diameter together with the lines representing limiting

Fig. 4. Liquid film mass transfer coefficient versus total power dissipated in the liquid. Filled symbols: water; empty symbols: salt solution (vs = 2.5 mm s−1 );
empty symbols with +: salt solution (vs = 4.97 mm s−1 ).
1516 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517
Fig. 5. Liquid film mass transfer coefficient versus average bubble diameter. Filled symbols: water; empty symbols: salt solution (vs = 2.5 mm s−1 );
empty symbols with +: salt solution (vs = 4.97 mm s−1 ).
values for the rigid, Eqs. (1) and (2), and the fully mobile
bubbles, Eqs. (3) and (4). The lines which follow from Alves
et al. [3] model of bubble contamination kinetics in water
and sulphate solutions are also included in the figure. To fit
experimental kL onto the model they [3] used three empir-
ical constants: k/Csurf = 27.5 for water, k/Csurf = 15 for
sulphate solutions and a 35% reduction on rise velocities, as
calculated from terminal velocities vsl = 0.65vt . The model
fits Alves’ kL data with the mean deviation of 9.7%. Our kL
data for sulphate solutions are well fitted by Eq. (3) for fully
mobile bubble surface with vsl = 0.65 vt , but kL value for
water is higher by 64%. If the empirical reduction on rise
velocities is not used, i.e. vsl = vt , the model (3) does not
fit the data neither for sulphate solutions (being up to 35%
higher) nor for water (being by 32% lower), see Fig. 5.
We conclude that Eq. (12) with one empirical parameter is
much better for fitting kL data measured in all batches used.
4. Conclusions
Average volumetric mass transfer coefficients measured
by Alves et al. [3] using peroxide decomposition steady-state
method with air as gas phase are six times lower compared to
the data measured by dynamic pressure method using pure
oxygen. The abnormally low kL a results presented in [3] are
discussed and shown to be probably wrong, which implies
that kL data from the same source are unreliable. This kL
values are up to six times lower and decrease with increas-
ing power dissipated in the liquid. It seems that the reported
decrease of kL with increasing power input dissipation in the
liquid is a result of mistake in kL a data. On the contrary, the
data presented in this work increase with the power dissi-
pated in the liquid phase according to Eq. (12). The “eddy”
model [4] based on turbulence theory gives successful fit-
ting of all our kL results for water (coalescent batch) and
sulphate solution (non-coalescent batch), contrary to “slip
velocity” model [3], which is based on bubble diameter and
bubble-liquid relative velocity.
Acknowledgements
This work was supported by the Grant agency of Czech
Republic through the project No. 104/98/1126 and by Czech
Ministry of Education through the scientific project No.
223400007.
Appendix A. Nomenclature
a specific interfacial area based on the liquid
volume (m−1 )
c1,5 constants in Eqs. (1) and (5)
C1,2,3 constants in Eqs. (6)–(9)
d, d32 bubble diameter, Sauter mean diameter (m)
D gas diffusivity in the liquid (m2 s−1 )
e total specific power dissipated in the liquid
volume (W m−3 )
 V. Linek et al. / Chemical Engineering and Processing 43 (2004) 1511–1517 1517

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