DESALINATION

ELSEVIER Desalination 146 (2002) 103-109

www.elsevier.comAocate/desal

Gas-liquid two-phase flow in microfiltration mineral tubular

membranes: relationship between flux enhancement and
hydrodynamic parameters

Petr MikulBSek*, Petr PospiSil, Petr DoleCek, Jifi Cakl

Department of Chemical Engineering, Faculty of Chemical Technology, University of Pardubice,
ncim. 6. leg-ii 565, 532 IO Pardubice, Czech Republic
Tel. +420 (40) 603-7130; Far +420 (40) 603-7068; email: Petr.Mikulase@upce.cz

Received 1 February 2002; accepted 15 February 2002

Abstract
An application of the gas-liquid two-phase flow for the flux enhancement during the microfiltration of aqueous
titanium dioxide dispersions on an ahuninium oxide tubular membrane has been studied. The results of experiments
showed a positive effect of the constant gas-liquid two-phase flow on the flux. It might be concluded from the analysis
of experimental results based on the dead-end filtration model that a two-phase flow seemed to expand the particle cake
as it increased both the cake porosity and thickness, thus allowing higher fluxes. A mathematical model for the flux
prediction during two-phase gas-liquid microfiltration has been developed. The results showed a good agreement
between experimental data and model prediction.

Keywords: Microfiltration; Two-phase flow; Dispersion; Flux enhancement; Mathematical model

1. Introduction
increases the energy consumption for required
The rapid permeate flux decrease at the begin- separation. Therefore, there is a tremendous
ning of filtration is a general problem of cross- unused potential in reduction and control of con-
flow microfiltration (MF) and ultrafiltration centration polarisation and fouling in membrane
(UF). The deposition of particles on the mem- processes and hence an alleviation of these
brane surface and inside the pores makes MF limitations. Many techniques for reduction of
ineffective since it diminishes the flux and particle deposition and concentration polarisation
have been studied. A survey of these methods is
*Corresponding author. given in MikuliSek [l]. There are at least three

Presented at the International Congress on Membranes and Membrane Processes (ICOM), Toulouse, France,
Jury 7-12, 2002.
30 l l-9164/02/$- See front mat -‘..0 2002 Elsevier Science B.V. All rights reserved
PII: SO0 11-9 I64(02)00498-8
104 M. Petr et al. /Desalination
possible approaches to reduction or control ofthe
concentration polarisation and fouling: changes
in surface characteristics of the membrane; pre-
treatment of the feed; and fluid management
methods.
Recently, some studies have dealt with the use
of gas-liquid two-phase flow techniques in the
concentrate stream during UF with the aim of
enhancing the flux for different applications
(biological treatment, drinking water production,
macromolecules separation) and different mem-
brane geometries (hollow fibre, flat sheet or
tubular). At present, studies of the two-phase
gas- liquid flow in membrane filtration processes
have mostly experimental character and are goal-
directed to UF. Only very little research has been
focused on theoretical aspects of the process. Cui
et al. [2-4] have shown that air injection can
reduce the concentration polarisation in UF of
macromolecules (dextran, dyed dextran and
bovine serum albumin) in the case of flat-sheet
modules and hollow-fibre membranes. The expla-
nation given for the flux enhancement is that air
sparging into the liquid stream increases turbu-
lence near the membrane surface as well as the
cross-flow velocity, thus limiting the boundary
layer thickness. Mercier et al. [5,6] reported a
significant flux enhancement (200% of flux
increase) by air sparging in UF tubular inorganic
membranes with two kinds of suspension (bento-
nite and yeast).
Cabassud et al. [7,8] presented results con-
cerning two-phase gas-liquid flow for particle
suspensions (clay suspensions) inside hollow
fibres. For all the concentrations studied, signifi-
cant increases in permeate flux have been
observed even at a very low air velocity. The air
injection processes lead to an increase of up to
155% at specific conditions. However, good
results were obtained for very low air velocities
(under 0.2 m s-l). Lee et al. [9] used air slugs
entrapped in cross-flow stream to prevent the flux
decline during filtration of bacterial cell suspen-
sions. UF and MF flat sheet membranes were
I46 (2002) 103-109
used and the best performance was obtained for
UF (maximum enhancement of 200% is
reported).
An accurate model that would enable a
prediction of the permeate flux during MF with a
two-phase flow has not been proposed yet. Vera
et al. [lo] expressed a steady-state flux of gas-
sparged MF and UF using two dimensionless
numbers: generalised shear stress and resistance.
The validations of graphic relations between
them and explanation of the line slopes have to
be confirmed by other experiments. Experiments
by Vera et al. [lo] were carried out with dextran,
wastewater effluent, tap water and ferric hydrox-
ide suspensions. A maximum flux enhancement
of 200% was achieved. The UF model proposed
by Ghosh et al. [l l] was based on a diffusion
mechanism of permeate transport through the
membrane surface and gave predicted flux values
lower than the experimental ones. The model
consisted of dividing the two-phase flow in
membrane into three zones enclosed in one gas
slug.
The aim of this study is to explain the
influence of the two-phase gas-liquid flow on the
flux, determine which operating parameters are
involved in the flux enhancement and propose a
semi-empirical model for the time-dependent flux
prediction. The validation of this model by
laboratory experiments is also presented.
2. Theoretical
Cakl et al. [ 121 developed a semi-empirical
model describing the time-dependent decrease of
permeate flux modified for backflushed cross-
flow MF. Their model was derived from a dead-
end filtration model in which the cake resistance
was determined by the mass accumulated during
the time of initial flux decrease. This procedure
has been shown to yield a very good approxima-
tion to the exact solution for a time variable
permeate flux, J [ 131.
The particle mass balance adapted for the
 M. Petr et al. /Desalination I46 (2002) 103-l 09 105

backflush [ 121 is given by where RM, RR and RIR are the membrane, rever-
sible and irreversible resistances, respectively.

1
The irreversible resistance represents the mem-

Ik-J, )t-db
dt
aF= a,--%
dt
(1) brane pore blocking due to particle size or
adsorption phenomena. When the particles can-
not enter the membrane pores, e.g., when there is
where J is the permeate flux, J, the steady-state a large gap between the biggest pore diameter
flux without backflushing, a,,+ aD, are the solid and the smallest particle diameter, the irrever-
volume fractions in the suspension and in cake, sible resistance can be neglected. Actually, the
respectively, and 8, is the cake layer thickness. reversible resistance is actually the cake resis-
The product J’@, is suggested to describe the tance (R,-), which could be expressed as a product
particle flux out of the membrane wall. This of specific cake resistance (R’,) and cake thick-
model has been experimentally proved for the ness. According to Darcy’s equation, the flux is
backflush MF of various suspensions and defined as
emulsions [ 121.
Considering that the transport of particles
from the membrane wall is proportional to the (5)
velocity gradient on the membrane surface in the
case of gas-liquid MF, the influence of gas flow Combination of Eqs. (2) and (5) gives the
velocity should be represented in the particle following differential equation:
mass balance. Then, the particle mass balance for
the MF with the gas-liquid two-phase flow is
expressed by

(i kJ-J, 1+-d%T
dt 1
aQ=
db
a+--
dt
(2) For the integration of Eq. (6), the following
conditions are considered: the initial flux is equal
to the pure water permeate flux (J= Jo; t = 0); the
where J, is the steady-state flux during MF specific cake resistance is constant over the
without the two-phase flow. The quantity k period of filtration, and the filtration cake is
indicates the influence of gas sparging on the incompressible.
immediate permeate flux. The following expression for the time-
The resistance model is expressed by dependent permeate flux results from the
integration
J= BP (3)
%RT
where AP is the transmembrane pressure, qOthe
dynamic viscosity of the permeate, and R, is the
total resistance to permeate flow, which can be where Jo is the pure water permeate flux, J, the
defined as steady-state flux during MF without two-phase
flow, t is time, and IJ,,is the dynamic viscosity of
(4) the permeate. Two experimental measurements
106 M. Petr et al. /Desalination
have to be made before the calculation. First,
with pure water for& and R, evaluation; second,
a MF experiment without two-phase flow to
obtain the values of J, and specific cake resis-
tance calculated from the dead-end filtration
model (R’& [14]. The value of @, was
substituted by the maximum solid volume
fraction in filtration cake (0.65), reported in [ 141.
The gas flow, k, as an exponential function of
injecting factor, Y,was estimated from previous
measurements [ 151:
k= exp(-v) (8)
The injecting factor, r, is defined as
(9)
u’d+rJL.
where u’~ and u L are superficial gas and liquid
flow velocities, respectively.
The expression of specific cake resistance
during MF with the two-phase flow is based on
the specific cake resistance during MF without
the two-phase flow (R> &. The relationship
between R’, and R’,,, is a function of k valid for
the whole gas flow velocity range,
R’, = kR’,,,
(10)
Then, the flux, J, for various gas flow velocities
during MF with the two-phase flow could be
predicted. Eq. (7) is implicit in J and can be
solved, e.g, in MS Excel with the Solver
program.
3. Experimental
The MF experiments were performed with an
aqueous dispersion oftitanium dioxide (Versanyl
B-K7020) obtained from Ostacolor a.s.,
Pardubice, Czech Republic. The mean diameter
of particles was 443 nm; however, the distribu-
tion of particle size was very wide (from 2 10 nm
146 (2002) 103-109
to 850 nm). The solids content in the dispersion
was 1 mass % and 5 mass % during the MF
experiments. During concentration experiments,
the dispersion solids content increased from 5
mass % to 18 mass %. The dispersion of titanium
dioxide was stable during the experiments.
The membranes used in the experiments with
two-phase gas-liquid flow were asymmetric
multi-layered ceramic membranes (Terronic a.s,
Hradec Kralove, Czech Republic). Composed of
a thin alumina layer deposited on the internal
surface of the alumina support, the membranes
were configured as a single 0.1 m long, 6 mm ID
and 10 mm OD cylindrical tubes. The MF mem-
branes with the 91 nm mean pore diameter were
used in MF experiments. The pore size distribu-
tion of the membrane was determined by the
liquid displacement method [ 161.
The two-phase gas-liquid apparatus used in
our experiments was shown schematically in
MikuldSek and PospiSil [ 141. The stainless-steel
circulating loop contained a 5-L retentate tank, a
diaphragm pump, the membrane module and a
flow control valve at the module outlet. The loop
was also equipped with a thermal regulating
system, and a pressure, temperature and flow
monitoring systems. The velocity and pressure in
the retentate loop were varied independently by
means of a pump controller and an appropriate
needle valve. Air was added to the liquid stream
through a capillary at the inlet of the membrane.
The airflow rates were controlled by means of a
flowmeter.
The flux through membrane was measured by
weighing the permeate collected during a chosen
period of system operation (using a computer-
interfaced balance). Both the retentate and
permeate were recirculated back into the retentate
container. Therefore, the concentration in the
recirculation loop remained virtually constant.
After each set of experiments was finished, the
circuit and membrane were rinsed with water and
the pure water flux was measured again under the
conditions of initial testing until the steady state
 M. Petr et al. /Desalination
was obtained. The differences between
subsequent steady-state pure water fluxes were
taken as a measure of the membrane fouling
tendency.
4. Results and discussion
The effects of the gas-liquid two-phase flow
on permeate flux were measured at various
experimental conditions keeping constant the
liquid flow velocity of 1 m s-’ and the trans-
membrane pressure difference of 100 kPa. The
permeate flux obtained in the presence of gas was
always larger than that without gas flow. Fig. 1
shows the results of experiments realised with
and without two-phase flow in the feed stream.
Typical behaviour for cross-flow MF was
observed, viz., that the permeate flux without
injecting air in the feed stream decreases with
time. During the first few minutes, the flux
decreased sharply due to a particle deposit forma-
tion that constituted additional flow resistance.
6000 7000 8000
Fig. 1. Influence of a constant gas-liquid flow on imme-
diate permeate flux for u i = 1 m s-‘, AP = 100 kPa, wF
= 0.01, and gas injecting capillary ID 1.08 mm. u k /
(m s-l): 0, 0; 0.25, 0; 0.53, 0; 0.81, W; 1.11, A; 1.70,
A; 2.36, 0.
146 (2002) 103-I 09 107
Then the flux seemed to level off. The deposit
behaved like a second membrane, with a flow
resistance constant in time.
The values of the normalised steady-state
permeate flux are plotted as a function of
injecting ratio, r, in Fig. 2. The normalised
permeate flux first increased with the air velocity
until it reached a limit corresponding to I = 0.45.
That is to say that a further increase in air
velocity would not result in any significant
improvement in the permeate flux until the
change of flow conditions. For r = 0.3-0.55,
large bubbles were observed with size of the
order of the internal diameter of the tube (Taylor
bubbles). Due to reduction in the available cross-
section for the liquid phase, a thin liquid film
always remained over the surface of the
membrane and moved in the opposite direction
with respect to the main flow. This phenomenon
induces a highly variable large shear rate against
the pipe wall. It should be noted that for a given
liquid flow rate, the presence of the gas increases
the mean longitudinal velocity of the fluid, which
in association with the great variations in the wall
0 0.1 0.2 0.3 0.4 0.5 0.6 0.7 0.8
Fig. 2. Normalised steady-state permeate flux against
injecting ratio for 1.08 mm (0) and 2.31 mm (0) ID
capillaries (u i = 1 ms-‘, AP = 100 kPa, wF = 0.01).
108 M. Petr et aL / Desalination 146 (2002) 103-109
~2, | |
10
~"~ 8 ' i ~
41
2 ~ i I H I I f f H I I I I I ~ ] I i l i
0 I I I I I I I
0 ~000 2000 3000 4000 5000 8000 7000 8000
#s
Fig. 3. Comparison of experimental fluxes with model
prediction for u ~ = 1 ms-~, u ~ = 0.8 ms-~, and Ap =
100 kPa and for we = 0.01 (O, experiment; doaed line,
model) and we = 0.05 (El, experiment; solid line, model).
shear stress and the turbulence e x i ~ g in the
churn flow (r = 0.6-0.7), can improve the
performance.
Model v~idation: A typicfl plot of flux vs.
time showing a comparison of experiment~
resuks and the model prediction is shown in
Fig. 3. The model developed in this g u d y
d e s c r i e d expefiment~ filtration behav~ur.
HoweveL an overestimation of the initifl flux
could be observed. Still, the predict~n of the
steady-state flux v~ues is more impo~ant for
indu~ri~ a p p l ~ n s of two-phase g a s - l ~ u ~
flow in MF processes.
Fig. 4 shows the v~ues of the s ~ a d y - g ~ e
perme~e flux experiment~ly measured and
predicted by the model. The values are predi~ed
for an operation time of 2 h when stab~ condg
tions for t~anium dioxide d i s p e ~ n s filtration
could be considere& The difference between
experim~nt~ and model resuRs varied ~om
+20% to -7%. While for the low value of gas
flow velocity (r = 0.2~ the model overestimated
the permeate f l u ~ for higher gas vdocities (r =
i ~ | | !
5 O
~ ~ S~
~~ 4 0 ~0 ~
~ ~
~ ~
~ ~
~ a ~
~
'~ O
2' I I I I I I I
0 ~4 ~2 0.3 ~4 0.5 0.6 ~7 0.8
i
F~. 4. Comp~son of expefime~N (o) ~ d p~di~ed
vNues ~o~ed l~e) of ~ e ~ e ~ e a t e flux ~r
v~ous ~ e ~ n g ratios and ~ r u~ = 1 m s-~, ~P =
100 kP~ ~ = 0.01, and g~ ~ e ~ n g c ~ a ~ ID
1.08 mm.
0.3-0.7), the model was near~ c o ~ e ~ or slight~
undere~im~ed the fluxes. The overestimation ~
the range of r = 0.1-0.3 can be a~ribu~d to un-
~able flow condK~ns of the bubb~ flow paRern
observed.
5. C o n d u s ~ n s
The experiment~ resuRs demons~ated that in
cros~flow MF of dispersions, the gas-liquid two-
phase flow is able to m~ntain the permeate flux
~ a constant and high ~vel during the e n t r e
experiment~ run. The hydrodynam~ regime
induc~g the larger enhancement in flux is slug
flow ~ the case of aqueous t~ania dispersion
where a permeate flux pl~eau is reached at the
beginn~g o f the slug flow regime. A p p l ~ i o n o f
slug flow paUern is a good comprom~e between
the flux enhancement and the a~ consumpt~n
during the MF process. The resuRs showed
agreement between modal prediction and experg
ment~ observation. Since other factors may
~fluence the permeate flu~ more experiments
should be done ~ order to optimise and v ~ e
this model for ~s application in a wider area of
process condR~ns and tested suspensions.
 M. Petr et al. /Desalination I46 (2002) 103-l 09 109

6. Symbols References

J - Permeate flux, m s-i (dm3 mm2h-‘) PI P. Mikulsek, Collect. Czech. Chem. Commun., 59
Jo - Pure water permeate flux, m s-’ (dm3 (1994) 737.
m-’ h-‘) PI Z.F. Cui and K.I.T. Wright, J. Membr. Sci., 117
Js - Steady-state permeate flux without (1996) 109.
intensification, m s-’ (dm3 m-* h-l) [31 Z.F. Cui, S.R. Bellara and P. Homewood, J. Membr.
Sci., 128 (1997) 83.
Steady-state permeate flux with in-
tensification m s-’ (dm3 me2 h-l) [41 Q.Y. Li, Z.F. Cui and D.S. Pepper, Chem. Eng. J., 67
(1997) 71.
K - Gas flow velocity factor, Eq. (8)
PI M. Mercier, C. Fonade and C. Lafforgue-Delorme,
AP - Transmembrane pressure difference Biotechnol. Techniq., 12 (1995) 853.
Pa 161 M. Mercier, C. Fonade and C. Lafforgue-Delorme, J.
R - Injecting ratio, Eq. (9) Membr. Sci., 128 (1997) 103.
R - Resistance, m-’ [71 C. Cabassud, S. Laborie and J.M. Lain& J. Membr.
R’ - Specific resistance, mm2 Sci., 128 (1997) 93.
T - Time, s PI S. Laborie, C. Cabassud, L. Durand-Bourlierand J.M.
4 - Superficial liquid flow velocity, m s- ’ Lain& Fihr. Sep., 34 (1997) 887.

4
- Superficial gas flow velocity, m s-’ [91 Ch.K. Lee, W.G. Chang and Y.H. Ju, Biotechnol.
Bioeng., 41 (1993) 525.
wF - Mass fraction of dispersion in feed
PO1 Vera, S. Delgado and S. Elmaleh, Chem. Eng. Sci.,
L.
55 (2000) 3419.
Greek
1111 R. Ghosh and Z.F. Cui, J. Membr. Sci., 162 (1999)
Cake thickness, m 91.
6, -
- Permeate viscosity, Pa s WI J. Cakl, I. Bauer, P. DoleEek and P. Mikulgek,
Desalination, 127 (2000) 189.
kc - Maximum solid volume fraction in
the cake [I31 R.H. Davis, Sep. Purif Methods, 21 (1992) 75.
[I41 P. Mikul&ek and P. PospiSil, Sci. Pap. Univ.
@F - Solid volume fraction in the feed
Pardubice Ser. A, 6 (2000) 79.
WI P. PospiSil, DiplomaThesis, University ofpardubice,
Acknowledgements 1999.
The Grant Agency of the Czech Republic, [I61 P. Mikul#ek and P. Dol&ek, Sep. Sci. Technol., 29
(1994) 1183.
Grant Project No. 104/00/0794, provided the
financial support for the research described.