Review

Ceramic Membranes for Water Separation from Organic Solvents

By Peter Kölsch*, Melinda Szilµdi, Manfred Noack, Jürgen Caro, Levente Kotsis, Ildikó Kotsis, and Ina Sieber

Novel hydrophilic SiOx modified alumina membranes with high separation factors and flux rates have been prepared for the
separation of water from organic solvents. For the preparation of the membranes, SiOx networks are deposited inside the c-
Al2O3 layer of a commercial ultrafiltration membrane by hydrolysis of tetraethylorthosilicate in autoclaves at 250 C. The
transport resistances of the individual membrane layers for the permeation flux are described by a model. The membranes are
stable towards solvents to temperatures of at least 150 C. Pervaporation studies show that water can be separated from solvents
such as acetonitrile, tetrahydrofurane, 2-propanol, ethyl alcohol, dimethylsulfoxide, N,N-dimethylformamide, and phenol. The
separation performance of the membranes allows their use in technical separation processes, especially for the removal of water.

1 Introduction CVD/CVI techniques [9±11], by crystallization of zeolites

The use of membranes in separation processes is of interest
in the chemical and pharmaceutical industry in refinery
technology, food industry, medicine, and biotechnology due
to economical, technological, and ecological advantages [1,2].
A large number of technical separation processes were
realized in the last 30 years with polymer membranes. The
economical advantages of pervaporation plants can amount
up to 30 % in the investment and up to 50 % in the operating
costs in comparison to rectification plants [3]. Membranes are
generally used in established separating processes, they are
also frequently used in hybrid techniques. The development of
membranes with high separation factors and flux perfor-
mances supports this trend. The development of inorganic
membranes has been increasingly carried out over the last 10
years. Advantages of inorganic membranes in comparison
with polymer membranes are their higher chemical resistance
against dissolving and swelling and a higher temperature
resistance. Inorganic membranes can be chemically function-
alized and are thus ideally suited for separation problems.
Disadvantages of inorganic membranes in comparison with
polymer membranes are the presently higher production costs
of the membranes and modules. Currently, the costs to
produce inorganic membranes amount to 750±1250 Euro per
m2 of membrane plus the investment for the modules. With
increasing production volume of this type of membrane and of
the modules these costs will decrease.
At present, porous ceramic membranes are produced
commercially up to average pore diameters of ca. 1 nm
(nanofiltration). However, membranes with even smaller
pores are necessary to carry out molecular separations. Up to
now, such membranes were made only in research labs by
layering several thin functional layers with pore sizes of 1 nm
on top of a substrate layer. The separation layers can be
deposited on these membranes by a sol±gel method [4±8], by
± show that the SiOx networks are partly bound chemically to
[*] Dr. P. Kölsch, Dr. M. Noack, Dr. J, Caro, Institut für Angewandte Chemie
Berlin-Adlershof e.V., R.-Willstätter-Str.,12, 12489 Berlin, Germany;
M. Szilµdi, Prof. Dr. L. Kotsis, Prof. I. Kotsis, Universität VeszprØm,
Lehrstuhlf.AngewandteChemie,H-8201VeszprØm,P.O.Box158,Hungary;
Ina Sieber, Hahn-Meitner-Institut, KekulØstr. 5, 12489 Berlin, Germany.
[16±20] or by chemical modification of surface areas [12±15].
This contribution is dedicated to the latter membrane types,
i.e., membranes with chemically modified surfaces.
2 Experimental
2.1 Preparation of the Selective Membranes
Commercial ceramic flat filters with asymmetrical Al2O3
layers were the basis for the SiOx functional layers (producer:
Hermsdorfer Institute for technical ceramic (hitk)/inocermic
GmbH). Data for the layered structure are given in Table 1
[21]. Pore narrowing and hydrophilic functionalizations of the
c-Al2O3 layers were carried out by chemical modification of
Al2O3 ceramic membranes. The fabrication of the membranes
was achieved by in-situ hydrolysis of a metal/alcohol/
tetraethyl orthosilicate (TEOS) solution [22±24]. The pore
system of the starting ceramic was first saturated with water
(water loading of < 1 mg/g ceramic) through gas-phase
adsorption at 23 C. Then, the ceramic was spin coated with
a 50 % TEOS-ethyl alcohol solution and brought into an
autoclave [24]. A certain amount of liquid TEOS was added to
the autoclave, so that at 250 C a TEOS pressure of 1.75 bar
was reached. The temperature was ramped up to 250 C at a
rate of 10 C/min, the temperature was then kept constant at
250 C for 1 h. TEOS reacts with the accessible, reactive c-Al-
OH groups of the pore wall surface thereby forming Al-O-Si-
O. Simultaneously, SiOx precipitation by condensation reac-
tions of the partly hydrolyzed TEOS molecules occurs. The
pore wall surface of the supporting ceramic becomes hydro-
philic because of the formation of a network of finely
distributed SiOx with a high concentration of Si-OH groups.
The obtained membranes were characterized by means of
phase interference microscopy, FE-REM/EDX, NMR,
ESCA, and thermal analysis [16,25]. NMR and ESCA studies
the Al2O3 surface (Si-O-Al bindings).
The FE-REM (Fig. 1a) shows the cross section of a c-Al2O3
layer and the first a-Al2O3 layer. The line scan EDX (Fig. 1b)
represents the length-resolved distributions of the aluminum

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0930-7516/02/0404-0357 17.50+.50/0 357
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Table 1. Asymmetrical layer construction of the used UF-Al2O3 ceramic membrane.

description layer thickness d50-value1) material

[lm] [nm]
support ca. 1000 3000 a-Al2O3
1. microfiltration(MF) layer intermediate layer 10 1000 a-Al2O3
2. microfiltration(MF) layer intermediate layer 10 200 a-Al2O3
3. microfiltration(MF) layer intermediate layer 10 60 a-Al2O3
4. ultrafiltration(UF) layer sol-gel layer 2±4 5 c-Al2O3

1) d50 data = pore diameters at 50 % of the pore volume of the respective layer.

and silicon across the membrane. The c-Al2O3 layer with a
thickness of about 2 lm shows that the SiOx network is mainly
deposited within the c-Al2O3 layer. Correspondingly, no
noticeable changes of the surface roughness of the membrane
after SiOx functionality could be observed with phase inter-
ference microscopy [25], as opposed to SiOx coating by the
sol±gel technique. By the storage of SiOx in the c-Al2O3 layer
this is mechanically and chemically protected. Therefore,
minor mechanical defects, such as scratches on the membrane
surface, do not reduce the membrane performance. The
hydrophilic qualities of the c-Al2O3 layer with the SiOx
network are used for the separation of water from solvent
mixtures. The following layer of a-Al2O3 (10 lm thick, d50 60
nm) has a lower Si concentration. Any hydrophilic effects from
this layer probably have a minor, if any, influence on the
separation process.
Hydrophobic or organophobic membrane characteristics
can be achieved in a similar way by using other chemical
reactants, e.g., fluorine or chlorosilanes [17,19,20], to chem-
ically modify the membranes. So, for a given separation
problem, a selective working membrane can be prepared.
2.2 Pervaporation Measurements
The pervaporation measurements were carried out under
vacuum on flat membranes, with diameters of 18 mm, which
were held in a permeation cell with Viton or silicone sealing
rings and were measured at constant temperature. The liquid
on the feed side was held in turbulence using a stirrer. On the
permeate side of the membrane, a vacuum of p < 10 mbar was
used. The permeate was frozen in a cool trap, then weighed
and analyzed by a GC/MS.

3 Results
3.1 Influences of the Membrane Arrangement on the Flux and
the Separation Factors

In applied technology the separating layers of asymmetric

Figure 1. a) Field emission (FE)-REM of the cross section of the SiOx modified
membrane with the c-Al2O3 and a-Al2O3-layer; b) Energy dispersive X-ray
spectroscopy (EDX) line scan of the Al-Ka and Si-Ka intensities of the
approximately 2 lm thick c-Al2O3 layer and the following first 10 lm thick
a-Al2O3-layer.
membranes are normally installed in the direction of the flow.
From pervaporation and gas permeation measurements,
respectively, Rautenbach [26,27] and Seidel-Morgenstern
[28] found that the permeation flux through asymmetrically
built membranes depends on the direction of the flux
(see Fig. 2). In this work, we found that the flux rate for
inorganic membranes at steady state function depends on
whether the fine or rough porous layer of the asymmetrically
built ceramic points to the feed or permeation side. When the
liquid on the feed side is in contact with the rough porous
membrane support, the flux is approximately twice as high as
when the c-Al2O3 layer is in contact with the liquid. By
intensive stirring of the liquid in the feed volume the flux
doubles itself due to the improved heat transport and a
minimizing of the concentration gradients. The influence of
the two orientations of the asymmetric membrane remains
unchanged. For the tests with stirrer in the liquid feed and
c-Al2O3 membrane layer pointing to the permeation side,
nearly 3.5 times higher fluxes were reached in comparison
with the tests where the c-Al2O3 layer pointed to the feed side

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 Review

10000 1,4 Al2O3 layers under the SiOx separation membrane water
exists in the gas phase. This water vapor has a more than
[Wasser/Isopropanol]
1,2
1000
1 1200 times greater volume than the liquid phase. Since a

Fluss [kg/m2h]
Trennfaktor

0,8
vacuum (1 mbar) is applied to the permeation side a further
100
0,6
volume increase to around thousand times the liquid
volume is reached. The total volume increase is 1.2
0,4
10
million-fold. The transport resistance increases due to the
0,2
increase in the free path lengths of gas or steam molecules at
1 0
ohne Rührer mit Rührer ohne Rührer mit Rührer
low pressures and due to more collisions with the walls. For
this type of membrane structure, a reduction of the partial
pressure difference, which is reflected in reduced fluxes, is
case 1 case 2 seen.

3.2 Estimation of the Resistances of the Membrane Layers

Figure 2. Effect of the flux direction (arrow) through the assymmetrically built
ceramic membrane on the permeation flux and the separation factor (p = 1 bar,
T = 25 C).
The dependencies on the fluxes on the orientation of the
asymmetrically built membrane were reason to carry out an
estimation of the relative resistances of the substance flux in
and the feed was not stirred. Even with stirring only half the the single layers.
flux rate is reached when the c-Al2O3 membrane layer is Since the separating performance of the membrane for
pointing to the feed side. water is high, the low flux rate of the solvent mixture
Depending on the structure of the effective c-Al2O3/SiOx component can be neglected. Therefore only the water flux
layer, different transport resistances are responsible for the is looked at in the following estimation. The calculations were
water flux. These are discussed in the following section. The carried out using data of the pervaporation of a 2-propanol/
separating characteristics do not depend on which structure of water mixture (50/50 %, v/v).
the membrane touches the feed, they are influenced exclu- Since the water flux rates were strongly dependent on the
sively by the c-Al2O3/SiOx layer. In the following the installation direction of the c-Al2O3 side of the membrane, the
influence of the transport resistances on the total flux and two installation possibilities, i.e., to the feed or to the
the separating characteristics are studied for the various permeation side, are looked at separately. Three layers of
membrane structures. the membrane are included in the consideration (see Figs. 3a
and b):
Case 1: Transport resistances and separation characteristics,
if the c-Al2O3/SiOx layer points to the permeation side and the (i) the 1000 lm thick a-Al2O3 support (d50 3000 nm)
liquid solvent±water mixture is in contact with the porous (ii) the three 10lm thick Al2O3 micro-filtration layers with
supporting layer (see Fig. 2). d50 1000, 200, and 60 nm
(iii) a 3±5 lm c-Al2O3 layer (d50 5 nm) with the pore-
l The transport resistances of the porous a-Al2O3 layers of
narrowing SiOx network.
the membrane (3 layers are 10 lm thick and 1 layer is 1 mm
thick) are small as opposed to the c-Al2O3/SiOx layer (see
Case 1: The c-Al2O3 layer points to the permeation side
Section 3.2). Therefore, the complete transport resistance of
For the c-Al2O3 layer the validity of a linear adsorption
the water flux is defined mainly by the c-Al2O3/ SiOx layer
isotherm is assumed1):
of the membrane.
l Inside the porous a-Al2O3 layers, a fast heat exchange takes cs;f ˆ K1 cf cs;g ˆ K2 cv
place due to convection of the liquid (stirring). At each
point of the layer, the same concentration of the solvent±
water mixture exists, i.e., there is no concentration gradient.
At the surface of the c-Al2O3/SiOx membrane layer, which
yields the water separation, a maximum water concentra-
tion exist. The separating characteristics are therefore not
very different with or without stirring.

Case 2: Transport resistances if the liquid solvent±water

mixture is in contact with the c-Al2O3/SiOx membrane layer Figure 3. Schematic concentration profiles (ci), layer thickness (di) and
diffusion coefficients (Di); case 1: c-Al2O3-layer on the permeation side, case
(Fig. 2): 2: c-Al2O3-layer on the feed side.

l It is known that in capillaries the resistance for gas transport ±

is higher than that for liquid transport [29]. In the porous a- 1) List of symbols at the end of the paper.

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 Review

The flux according to Eq. (1) is then: The mass-transfer coefficient of the second and third
layers is:
cs;f cs;g K c K2 c
j ˆ D ˆD 1 f (1) D
1
dg dg  0.26 m / s  

Case 2: The c-Al2O3-layer of the membrane points to the
feed side DM
 0.55 m / s   M
Again the validity of a linear adsorption isotherm is M
assumed:
The total resistance can then be calculated from the mass-
transfer coefficients using Eq. (8):
cs;f ˆ K1 cf cs;g ˆ K2 cg
1 1 1 1
ˆ ‡ ‡ (8)
The water flux is then given by: b bg b bM
The relative resistance of the single layers can be calculated:
cs;f cs;g K c K2 cg
j2 ˆ D ˆD 1 f (2)
dg dg b
100 % ˆ 72:2 %
bg
cg cg;k
j2 ˆ e D (3)
d b
100 % ˆ 18:9 %
bl
cg;k cg;v
j ˆ eM DM (4)
2
dM b
100 % ˆ 8:9 %
bM
From Eqs. (3) and (4) one can calculate and compare cg,k
and cg with the experimental data. From this modeling, it can be seen that the Al2O3 membrane
j2 = 0.00995 mol/m2s T = 353 K layer with the inlayed SiOx network causes the main transport
Dl = 6.44 10±6 m2/s d l = 2.5 10±5 m resistance (72 %) for the pervaporation. The three 10 lm
±4 2 layers and the 1 mm thick rough porous Al2O3 support cause
DM = 5.37 10 m /s d M = 9.75 10±4 m
fundamentally smaller resistances.
e l = e M = 0.38 pv = 1 torr
r
4 2RT
D ˆ r
3 M
3.3 Separation Factors and Fluxes for the Separation of
We obtained the following values: cg,k = 0.093 mol/m3 and Solvent/Water Mixtures by Pervaporation
cg = 0.195 mol/m3.
To obtain the mass-transfer coefficients, the assumption In Tab. 2 the separating factors and fluxes for pervaporation
that K1/K2 = g is constant must be made. From Eqs.(1) and (2) measurements at a Al2O3/SiOx membrane layer are pre-
the following equations are then obtained: sented. A first report was given in [30].

The pervaporation examinations of the mixtures show that
j ˆ D K2 gcf cv (5)
1
dg SiOx-modified membranes are advantageous for the water
  separation from solvent±water mixtures compared to polymer
K2 gcf cg membranes. polymer membranes cannot always be used
j ˆD (6)
2
dg because of their low chemical resistance towards solvents such
as acetonitrile and tetrahydrofurane.
From these equations g can be calculated:
The tested membranes were constant in continuous opera-
  
j2 
c  cg j1c  j2 c tions up to temperatures of 150 C. Examinations of up to 600
 1.23 . 105
f g v

 hours were carried out. The results show that pervaporation

c f  cv    
j1  j1  j2  c f can achieve separations of solvent-water mixtures that form

azeotropic mixtures, which can not be separated with
The used values are: cf = 2.778 104 mol/m3 for a 50/50 % technically relevant separating factors and flux performance,
2-propanol/water-mixture, j 1 = 0.02019 mol/m 2 s and by simple rectification.
cv = 0.044 mol/m3. Essential differences in the separating factors and the flux
From Eq. (6) one can calculate the substance transition rates are obtained depending on the composition of the
coefficient: mixtures. The flux rates become smaller at high separating
 factors, as expected. Separating factors of more than 1000
DK2 j2 (7) could be obtained at 25 C. At small concentrations of organic
  0.068 m / s   g
g
c f  cg solvents in the mixtures, high permeation flux rates of water

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Table. 2. Separation factors and flux rates of a SiOx modified Al2O3 membrane at Dp = 1 bar.

mixture temperature composition separation factor flux rate

solvent (A)/water (B) C A/B vol.-% awater/organica kg/m2 h

5/95 145 0.15

25 50/50 2295 0.10
acetonitrile - water 95/ 5 9625 0.02

5/95 64 3.65
80 50/50 18 0.30
95/ 5 17 0.25

5/95 29 0.15
25 50/50 115 0.05
tetrahydrofurane - water 95/ 5 9860 0.05

5/95 21 1.90
60 50/50 420 0.20
95/ 5 1275 0.10

5/95 380 0.30

25 95/ 5 >10000 0.25
isopropanol ± water
5/95 185 4.15
80 50/50 885 1.35
95/ 5 >10000 0.15

5/95 72 0.10
25 50/50 2160 2.40
ethanol ± water 95/ 5 24 0.50

5/95 2 2.50
80 50/50 520 4.85
95/ 5 42 0.90

5/95 9 1.15
95 50/50 115 1.15
dimethylsulfoxide-water
5/95 1820 0.10
25 50/50 2 0.02

5/95 2 1.20
dimethylformamide-water 95 50/50 95 0.40

phenol - water 80 5/95 6 1.30

are obtained near the boiling-point of the mixtures. The
performance parameters show that SiOx-modified ceramics
are comparable with the best polymer membranes.
4 Conclusions
Asymmetrical UF membranes can be modified by in-situ
hydrolysis with TEOS in an autoclave so that hydrophilic
separations by pervaporation and steam permeation with
these membranes are possible. The SiOx network, which
causes the molecular separation, is located in the ultrafiltra-
tion layer (c-Al2O3) of the membrane.
The surface modification technically is not expensive and it
is easily applied to greater membrane surfaces or pipes.
The SiOx-modified membranes show high separating
performances and flux rates and could be used as competitors
to polymer membranes. In comparison to the polymer
membranes the SiOx membranes can be used at high
temperatures (at least up to 150 C).
For the effective use of asymmetrically built membranes,
the influence of the flux direction on the flux rates is very
important. Theoretical modeling showed that the flow
resistance is determined mainly by the c-Al2O3/SiOx layer.
The complete resistance of the membrane can be reduced
further by using thinner c-Al2O3 layers.
The presented membranes create possibilities for the
separation of solution mixtures for which polymer membranes
do not offer an adequate stability. The advantage of the
ceramic membranes is that these are sterilizable and thus can
be used in the presence of germs. To reach large membrane
areas, as necessary for technical interests, the ceramic
membranes must be fabricated in suitable modules.
Acknowledgement
The Federal Ministry for Education and Science provided
the financialsupportforthisprojectas well as the Stateof Berlin
(grants 03 C30120 and UNG02197). We thank P. Toussaint,
M. Stöhr, G. Georgi, and I. Sieber for technical assistance.

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 Review

We also thank the co-workers of HITK: Dipl.-Chem. References

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This paper was also published in German in Chem. Ing. Tech. 72 (2000) No. 10,
pp. 167±173.

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