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A Modified Method for the Calculation of

the Humidity Adsorption Stresses Inside
Zeolite Films Using Magnetoelastic
Sensors
ARTICLE in SENSOR LETTERS APRIL 2012
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SENSOR LETTERS
Vol. 10, 879885, 2012

A Modied Method for the Calculation of the Humidity

Adsorption Stresses Inside Zeolite Films Using
Magnetoelastic Sensors
Theodoros Baimpos1 2 , Vassiliki Tsukala1 2 , Vladimiros Nikolakis1 3 , and
Dimitris Kouzoudis4
Foundation for Research and Technology Hellas, Institute of Chemical Engineering and High-Temperature
Chemical Process, P.O. Box 1414, GR 265 04 Patras, Greece
2
Department of Chemical Engineering, University of Patras, GR 265 04 Patras, Greece
3
Catalysis Center for Energy Innovation (CCEI), University of Delaware, Newark, DE 19816, USA
4
Department of Engineering Sciences, University of Patras, GR-26504, Patras, Greece

RESEARCH ARTICLE

(Received: 28 March 2012. Accepted: 28 April 2012)

A magnetoelastic sensor is comprised of a magnetoealstic substrate (Metglas) and an active layer
(zeolite). In this paper, a previous method that measures adsorption-induced stresses in Metglas
is modied. That method which was demonstrated for Metglas/FAU and Metglas/LTA sensors, was
based on tting the humidity adsorption data of each sensor with a phenomenological theory develTechnology
to: BIDS/ingenta
oped by Squire. TheDelivered
purpose ofby
thePublishing
current work
is twofold. The
previous method is modied with a
IP: 217.45.193.129
On:
10 Apr
08:29:17
more direct tting approach
and their results
areWed,
compared
to 2013
each other.
Also, a model developed
Copyright
American
Scientific
Publishers
by Hsueh is applied in order to correlate the stresses in the Metglas with the induced stresses in
the zeolite layers.

Keywords: Magnetoelastic Sensors, Zeolite Films, Metglas, Adsorption Induced Stresses.

1. INTRODUCTION
Quite often, when gas and vapor physical adsorption takes
place inside natural and synthetic adsorbents, it is assumed
that the physical properties of the adsorbent remain unaffected. Such an assumption is valid only for adsorbents of
small specic surface area but not for microporous adsorbents with an extremely developed porous structure-such
as zeolites. Toward this direction, the group of Noble and
Falconer has demonstrated that feeding small amounts of
gases or vapors can either expand or shrink the zeolite
unit cell,15 which in turn can affect the overall performance of the zeolite membrane.68 Our group has already
presented a method for measuring the elastic modulus of
zeolite lms9 10 upon gas adsorption, using magnetoelastic sensors. In a recent publication,11 we demonstrated
the remarkable exibility and elasticity of MFI zeolite
lms under the adsorption of volatile organic compounds
(VOCs). The adsorption caused notable bending (visible

Corresponding authors; E-mail: kouzoudis@des.upatras.gr

Sensor Lett. 2012, Vol. 10, No. 3/4

even to the naked eye) however without destroying the

cohesion and the continuity of the MFI lm.
Caro et al., studied the change of the unit cell dimensions for several zeolites (LTA, FAU, MOR and MFI) as
a function of temperature and water content by means
of in situ-heating XRD.7 A strong change was observed
for all the Al-rich zeolite types, as a result of the dewatering process upon heating. They attributed the difculty of preparing shape-selective FAU or LTA membranes
for gas separations, to the extreme expansions/shrinkages
of their unit cell during water removal.12 On the other
hand, such a behavior was not observed in the case of
hydrophobic zeolites (i.e., MOR, MFI).
The most commonly used techniques to calculate unit
cell size changes down to the ppm level upon gas
adsorption, are X-ray and Neutron Diffraction5 1315 and
dilatometry.1622 Independently of the technique used, all
results indicate that adsorption may cause both shrinkage
and swelling of the zeolite crystals depending not only
on the nature of the adsorbent, but also on the magnitude
of the loading. Despite the high accuracy offered by the

1546-198X/2012/10/879/007

doi:10.1166/sl.2012.2592

879

RESEARCH ARTICLE

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films

Baimpos et al.

previously mentioned methods, data collection requires the

Hmin is the value of H at the minimum, and extract from
it the humidity-adsorption stresses from the minima of the
use of highly sophisticated and expensive scientic equipexperimental curves. In a subsequent paragraph it will be
ment (i.e., Synchrotron Radiation for Neutron or X-ray
shown that both approaches (the data t35 and the new
Diffraction), the use of large zeolitic single crystals (which
minima-calibration curve), lead to a fairly good agreement.
in general are hard to synthesize) or the use of powder in
The sensors signal results from magnetization changes
which case the data analysis might be rather cumbersome.
in the Metglas layer and thus the extracted stresses are the
Zeolites are commonly used in commercial separation
internal stresses s in this layer, due to the adsorption on
processes and VOCs recovery due to their molecular sievthe attached zeolite layer. However it would be of great
ing ability, i.e., to preferentially adsorb certain molecules
interest to calculate the stresses f developed in the zeolite
and to exclude others. They have attracted great interest
lm. This is achieved in this work by introducing a new
due to their catalytic and ion-exchange properties, emergmethodology which correlates s with f . The developed
ing as possible versatile adsorbents. The size and the strucmethodology is based on the model of Hsueh,36 is general,
ture of both the micropores and the molecular adsorbate,
and can be used for calculating stresses due to adsorption
determine the adsorption capacity and selectivity. On the
in any microporous (zeolite, MOF, ZIF etc.) lm as long as
other hand, ferromagnetic materials can alter their shapes
it can be deposited uniformly on a magnetoelastic ribbon.
when placed in an external magnetic eld (the magnetostrictive effect) and conversely, their magnetic properties might change when strains or stresses are applied
2. MATERIALS AND METHODS
to them (the so-called magnetoelastic effect). All magne2.1. Synthesis of the Zeolite/Metglas Sensor
tostrictive ferromagnetic materials are also magnetoelastic
materials. Magnetoelastic ribbons have often been used as
Zeolites were synthesized on both sides of 6 mm
sensors,2325 while the coating of their surface with appro20 mm 28 m Metglas 2826MBA (Fe40 Ni38 Mo4 B18 
priate analyte-responsive recognition layers enhances their
magnetoelastic ribbons (Allied Signal). Details concern26
27
28
detective ability on humidity, pH, microorganisms
ing the synthesis procedure like chemicals, temperature
etc. Our group has already shown that Metglas/zeolite
and duration of synthesis for each zeolite are described in
bilayers (Metglas is a known magnetoelastic material) can
our previous publications,9 10 30 revealing the formation of
Delivered
by Publishing
be used as selective sensors for
the detection
of lightTechnology to: BIDS/ingenta
zeolite
polycrystalline
lms on both sides of the strips.
On: Wed,
10 Apr
2013 08:29:17
gases,29 light hydrocarbons30 31 IP:
and217.45.193.129
VOCs.32 The detecCopyright American Scientific Publishers
tion of VOCs has also been reported using a polymeric
2.2. Experimental Set-Up
recognition layer in the place of the zeolitic recognition
layer.33
Recently, we introduced34 a new, relatively simple and
low cost method for measuring the internal stresses s
imposed on the Metglas resulting from humidity adsorption to neighboring zeolite layer. Two different zeolite layers of types FAU and LTA were used. That method was
based on the phenomenological theory of magnetolasticity
introduced by Squire,35 which relates the axial stresses in
a magnetoelastic ribbon to the ratio of two experimentally
measured quantities, the resonance fR and anti-resonance
fA frequencies. Shown in Figure 1 is a typical voltagefrequency signal on the pickup coil where both the fR and
fA frequencies are determined. The fR /fA 2 quantities are
plotted versus the intensity of an externally applied magnetic eld H , with the internal stress in the ribbon as a
parameter, generating different curves. In Ref. [34] these
theoretical curves were t to our experimental data in order
to extract the adsorption induced stress s (internal to the
Metglas layer) as a function of humidity levels.
In the current work, the s values are extracted via
another approach by noticing that both theoretical and
experimental fR /fA 2 versus H curves have a characteristic minimum which shift as a function of stress and humidity level correspondingly. From the theoretical curves, a
calibration curve Hmin versus s can be made, where
880

The experimental set-up used for humidity adsorption

is shown in Figure 1. The gure also shows a typical
frequency-amplitude signal of the sensor measured with
a magnetoelastic resonator, as a magnied screen shot
of the PC monitor, where the quantities fR and fA are
marked with dotted lines. The sensor is placed in a glass
tube (cell) around which a sensing coil is wrapped. The
edges of the coil are connected to the magnetoelastic resonator (provided by Sentech Corp.). The cell is placed
in an oven for the control of the operating temperature.
Before each measurement, the sensors surface is degassed
at 200  C overnight under the ow of 50 cc/min of synthetic air. The humidity concentration is controlled using
the following procedure: a stream of synthetic air is fed
to a saturator (bubbler) in order to become saturated with
H2 O. The concentration of the H2 O is adjusted by diluting
it with a second stream of pure synthetic air. The ows of
both streams are adjusted using two mass ow controllers
(AERA 7700C).
2.3. ResonanceAnti-Resonance Frequency
Measurements
The magnetoelastic materials deform when placed inside
a magnetic eld. For a thin ribbon placed in a constant
Sensor Letters 10, 879885, 2012

Baimpos et al.

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films
1.6
1.4

1.0
0.8

Amplitude [V]

Amplitude [V]

1.2

0.6

1.6
1.4
1.2
1.0
0.8
0.6
0.4
0.2
0.0

fR

fA

106 108 110 112 114

Frequency [kHz]

0.4
fA

0.2
fR

0.0
106

108

PC
110

112

114

Frequency [kHz]

RESEARCH ARTICLE

Resonator

Glass
cell Coils
MFC

AIR

Vent
H2O
Sample

Oven

Delivered
byused
Publishing
Technology
BIDS/ingenta
Fig. 1. Schematic drawing of the experimental
set-up
in the detection
experiments.to:
A typical
voltage-frequency signal on the pick up coil where
IP: 217.45.193.129
On: Wed, 10 Apr 2013 08:29:17
fA frequencies are determined.
both the resonance fR and the anti-resonance
Copyright American Scientific Publishers

magnetic eld H along its long axis, the relative length

change (strain) is called magnetostriction and is given
in ppm (parts per million, typically 550 for Metglas
ribbons). When an AC magnetic eld is added to the constant magnetic eld (the latter also known as the bias),
the ribbon vibrates in an effort to follow the AC variations.
Because Metglas is a magnetic material (the bias magnetizes it), its vibrations cause variable magnetic ux which
can be sensed by a nearby detection coil. The coils voltage
reaches a maximum when the ribbon vibrates at its resonance (natural) frequency fR . Similarly, there is an antiresonance frequency fA where the ribbons oscillations are
out of phase and the coils voltage reaches a minimum. For
the sensors tested (FAU/Metglas, LTA/Metglas) the measurements of fR and fA were recorded as a function of
humidity concentration P/Ps, where P is the water pressure and Ps the corresponding saturation pressure at room
temperature.

3. RESULTS AND DISCUSSION

As it was mentioned in the Introduction section, a new
method was introduced by our group which extracts the
internal stresses s in a Metglas substrate resulted from
gas adsorption in the zeolite layer. This method,34 which
Sensor Letters 10, 879885, 2012

is based on the theory of magnetoelasticity and a phenomenological model developed by Squire, was demonstrated for a FAU/Metglas and a LTA/Metglas sensors upon
humidity adsorption. A slight variation of this approach
and their comparative results will be presented in this
work. The common steps of the two approaches are the
following:
(1) Measure the fR /fA 2 changes of the bare Metglas
ribbon (before zeolite synthesis) as a function of the magnitude of the applied magnetic eld H .
(2) Estimate the values of the Metglas magnetic properties, by tting the experimental data to the Squires model
and assuming that the ribbon is at a stress free state
 = 0. The tting process is a minimization procedure
in which all the magnetic parameters vary within their
physically acceptable range, until the minimum difference between the experimental and the theoretical curves
[fR /fA 2 vs H ] is achieved. In Figure 2(a), representative
theoretical curves of Squires phenomenological model are
presented with respect to the axial stress (6  6
MPa). Their common feature is a minimum with respect
to H . With increasing stress, this minimum shifts to lower
H values.
(3) After synthesizing zeolite on the Metglas strip, measure experimentally the fR /fA 2 ratio as a function of
H at different humidity levels for each Metglas/zeolite
881

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films

3.1.1. First Approach

In the rst approach, the experimental data are t by the
theoretical curves of Squires model over a broad range
of magnetic elds H . Their results of the whole process
which has already been demonstrated in detail34 are presented in Figure 3(a).

(a) 1.000

increasing
stress

0.996

=6 MPa
=4 MPa
=2 MPa

0.992

=0 MPa
=2 MPa
=-4 MPa
=-6 MPa

0.988
0.984
0.980

3.1.2. Second Approach

0.976

The second approach makes use of only the characteristic

0.0000
0.0004
0.0008
minima which are present on both the experimental and
H [T]
Delivered
Publishing
to: BIDS/ingenta
the theoretical curves. A calibration
curve isbymade
(inset inTechnology
(b) Apr
1.000 2013 08:29:17
IP:minima
217.45.193.129
On: Wed, 10
increasing
Fig. 3(b)) from the H values at the
of the theoretiCopyright American Scientific
Publishers
humidity
0.995
cal curves (Fig. 2(a)) as a function of stress. The resulting
P/Ps
linear equation (also shown in the inset), can be used as
0.990
a calibration factor to convert Hmin shifts to corresponding
0.985
s changes. Applying this equation to the minima of the
0.980
experimental data of Figures 2(b) and (c) for the two sen0.975
sors, the corresponding s are calculated and their values
are presented in Figure 3(b).
0.970
(fR/fA)2

0.0012

P/Ps
0
0.009
0.019
0.029
0.056
0.107
0.166
0.23
0.285
0.423
0.6

FAU
0.965

3.2. Interpretation of the Results

0.0004

0.0006

0.0008

0.0010

H [T]

The s results of the two approaches as a function of

humidity levels P /Ps, are shown in Figures 3(a) and (b)
correspondingly and they are plotted with the same vertical
y-scale for easier comparison. The close quantitative and
qualitative similarities between them certify the validity
and reliability of the two approaches. Hence, the discussion on the interpretation of the results in the next paragraph is common to both approaches. However, it should
be mentioned that the second approach is more direct since
it requires only the H value of the minima of the theoretical curves, whereas the rst one is more exact since
it requires a satisfactory t between the experimental and
theoretical curves over a broad range of H . Also note that
for FAU at high humidity, a few points are missing in
Figure 3(a) with respect to Figure 3(b). This is because it
was impossible to obtain satisfactory curve-tting results
at these high humidity values.
882

(c) 1.000
0.996
0.992

(fR/fA)2

RESEARCH ARTICLE

3.1. Extraction of the Optimum Internal Stress

Values as a Function of P/Ps

In the cases of FAU and LTA sensors, the estimated s

values show a minimum at low humidity levels, whereas
s increases at higher ones. This result indicates that at low
values of humidity the FAU and LTA lms tend to contract.
The contraction is maximized (at the curve minimum)
and as the humidity level increases, the initial contraction
is followed by relaxation and nally leads to expansion.
This behavior is in qualitative agreement with literature
studies for the same adsorbate/adsorbents systems, using
dilatometry19 21 22 37 or XRD.5 7
It should be noted that the calculated s shown above,
are the stresses developed on the Metglas strip as a result
of the adsorption induced stresses on the zeolite lm. This

(fR/fA)2

sensor, as shown in Figures 2(b), (c) for the FAU and LTA
sensor correspondingly (for simplicity, from now on, these
sensors will be referred to as FAU and LTA). The shift
of the experimental curves with P/Ps, shows a remarkable similarity with the shift of the theoretical curves of
Figure 2(a) as a function of stress. The numbers next to
each experimental curve indicate different humidity levels (0 P /Ps 1). The two approaches for the calculation of internal stresses differ in their nal step, which is
described separately in the next section.

Baimpos et al.

0.988
P/Ps

0.984
0.980
LTA

0.976
0.0004

0.0006

0.0008

0
0.004
0.008
0.016
0.09
0.33
0.66
1

0.0010

H [T]
Fig. 2. (a) Plot of (fR /fA 2 values as a function of the applied magnetic
eld H as predicted by Squires model for different stress values .
Plot of fR /fA 2 values as a function of the applied magnetic eld H .
Experimental data for different humidity levels (P /Ps ) in the (b) FAU
and (c) LTA sensor.

Sensor Letters 10, 879885, 2012

Baimpos et al.

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films

is because the measured signal originates from the Metglas substrate and not from the recognition zeolite layer
in which the adsorption process takes place. However, for
zeolite applications such as membranes, the stresses of
interest are the ones developed in the zeolite recognition
lm, which from now will be denoted as f . Thus, there is
a need to quantitatively correlate f to s . This is achieved
through the analysis of Hsueh,36 which as will be shown
in the next section, deals with stress distribution in bilayer
materials.

(a)
f

Zeolite, Young modulus Ef

Metglas, Young modulus Es

(b)
z=tf
z=0
z=tb

z=-ts

3.3. Correlation of the Adsorption Induced Stresses

on the Substrate and the Recognition Film

4
3
FAU
2
1
0
1
2

Stress s [MPa]

3
4
5
4
3

FAU

2
1
6

0
Stress s [MPa]

1
2
3

2
0
2

Fig. 4. (a) Schematic representation of zeolite/Metglas sensor a assuming a two-layer system and (b) strains of the zeolite lattice due to adsorption mismatch.

and the Young moduli E which in our case are taken

from the values shown in Table I. The t values have been
measured with Scanning Electron Microscopy, while the
E values of the zeolite lms have been taken from our
previous publication9 for FAU and from the literature38 for
LTA. The value of Es = 131 GPa for Metglas has been
estimated by tensile testing.
The basic assumption of Hsuehs analysis is that the
strain  along the two layers increases linearly with z
accordingto:toBIDS/ingenta
Delivered by Publishing Technology
(a)
z tb
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On:
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10 Apr 2013 08:29:17
=c+
(1)
LTA
r
Copyright American Scientific Publishers
where c tb and r are three key parameters which are
determined from the boundary conditions. The geometrical
interpretation of Eq. (1) is shown in Figure 4(b). The strain
 consists of two terms. A uniform expansion c like the
one shown in the gure, and on top of that, a z-dependent
term, which is zero at z = tb , positive above and negative
below that. Hence the nal shape is a trapezoid.
The c tb and r parameters of Eq. (1) depend on the Es ,
ts , Ef , tf values, and the thermal expansion strain aT,
(b)
where a is the thermal expansion coefcient and T the
LTA
temperature variation. In our case, the operating temperature is maintained constant (at 30  C) and thus this term
is not taken into account. However, we introduce a simi = 12158.6*H +8.88
lar term aP due to the humidity pressure variation P ,
R = 0.9937
where a is a corresponding adsorption coefcient. Thus
in all Hsuehs equations, the af T term is being replaced
by af P , and the corresponding Metglas term with zero
2

6
0.0004

5
0.0

0.2

0.4

0.0006 0.0008 0.0010

H [T] of minimum

0.6

0.8

0.0012

1.0

P/PS of H2O
Fig. 3. Adsorption stress on the Metglas substrates of the FAU lm
(open squares), LTA (open stars) versus humidity calculated from
(a) Squires model and (b) the calibration curve in which the minimum
of the curve is presented.

Sensor Letters 10, 879885, 2012

Table I. Numerical values of our metglas/zeolite sensors for the application of Hsuehs model and the calculation of the (f /s ) ratio.
Substrate (metglas)
ts
Zeolite (m)
FAU
LTA

14
14

Film (zeolite)

Model parameters

Es
(GPa)

tf
(m)

Ef
(GPa)

131
131

6
14

38
46

tb
2
f /
(m) (m1 ) s

0.11 5
9
0.26 3
4

0.040
0.050

4.4
4.5

883

RESEARCH ARTICLE

The analysis of Hsueh36 deals with bilayers, while our sensor is a three layer system: zeolite lm-Metglas substratezeolite lm. However, since the two zeolite lms are of
the same synthesis and thickness, we can work on half
of the sensor (one zeolite lm plus the half of the Metglas substrate) and assume a mirror symmetry thus effectively having a bilayer system as shown in Figure 4(a).
Following the authors notation, we will use the subscript
s (substrate) for the Metglas ribbon and f (lm) for
the recognition layer (zeolite in our case). The material
parameters needed for this analysis are the thicknesses t

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films

since the Metglas ribbon is non-adsorptive. These replacements lead to:

c=

E f tf
a P = 1 af P
Ef tf + Es ts f

(2a)

tb =

Ef tf2 Es ts2
2Ef tf + Es ts 

(2b)

where the 1 and 2 terms have been introduced for simplicity. Note that tb , 1 and 2 depend only on the materials
parameters Es , ts , Ef , tf . Using the numerical values given
in Table I, these three terms have been calculated and their
results are shown in the same Table.
The stress-strain relationships in each layer are:
(3)

f = Ef  f P  = Ef  Ef f P = Ef  f a

(5)

(4)

1  tf
E  tf
f dz = f
 af P dz
ts z=0
ts z=0
t
= Ef  1 2 tb 2 f 1f P
2

f =

(6)

However, we are interested only on the adsorption-stress

contribution f a :
f a = Ef f P

(7)

The ratio of Eqs. (5) and (7) leads to:

f a
Ef
=
s
Es  1 2 tb 22ts 

(8)

This ratio can be calculated from the numerical values

where we have introduced f a as the adsorption-stress
of the last column of Table I. From this ratio and the Metcontribution. Since the stress in both layers varies with z,
glas stress-humidity curves in Figures 3(a), (b), the correthe average stresses on each material (s and f  have to
sponding zeolite stress-humidity curves are calculated in
to: BIDS/ingenta
be calculated. For the Metglas: Delivered by Publishing Technology
Figures 5(a),
(b). Since these curves are quantitatively simIP: 217.45.193.129 On: Wed,
10
Apr
08:29:17
ilar to the 2013
original
zeolite curves in Figures 3(a), (b), the
Copyright American Scientific Publishers
physical
interpretation
is the same as the one described in
16
LTA
Section 3.2.
FAU
12
8
4

4. CONCLUSIONS

0
4
8
12

Stress f [MPa]

RESEARCH ARTICLE

(2c)

s = Es 

1u
E u
s dz = s
dz
ts z=ts
ts z=ts
t
= Es  1 2 tb 2 s f P
2

s =

For the zeolite lm:

1
6Ef tf Es ts tf + ts af P
= 2 4
r
Ef tf + Es2 ts4 + 2Ef tf Es ts 2tf2 + 2ts2 + 3tf ts 
= 2 af P

Baimpos et al.

16
20

(a)

24
16

(b)

FAU

12

LTA

8
4
0
4
8
12
16
20
24
0.0

0.2

0.4

0.6

0.8

1.0

A new calibration technique is introduced as a modication to our previous method which extracted the resulting
stresses in the Metglas ribbon due to humidity adsorption
in the zeolite layer. Additionally, the current work introduces an analysis that makes it possible to convert these
stresses to the corresponding adsorption induced stresses in
the zeolite layer. The modied method has been applied to
FAU, and LTA types of zeolite. The results for FAU show
that the as-synthesized lms are tensile but the introduction of even the slightest amount of humidity, reverses the
state to compressive. Further increase of humidity relaxes
the stresses until the stress-free state is obtained at relative
water pressure of P /Ps = 0
05 and subsequently the lm
becomes tensile again until saturation is reached. The LTA
behavior is similar but with smoother changes and a stressfree state around P /Ps = 0
35. The results are in great
agreement to the FAU and LTA results of other measuring
techniques in the literature.

P/PS of H2O
Fig. 5. Adsorption stress on the FAU lm (open squares), LTA (open
stars) versus humidity calculated from (a) Squires model and (b) the
calibration curve in which the minimum of the curve is presented.

884

Acknowledgments: The authors would like to thank

Georgia Tsoukleri for her valuable contribution. Part
of the current work was supported financially by the
KARATHEODORI 2010 grant.
Sensor Letters 10, 879885, 2012

Baimpos et al.

A Modied Method for the Calculation of the Humidity Adsorption Stresses Inside Zeolite Films

References and Notes

1.
2.
3.
4.
5.
6.
7.
8.

10.
11.
12.
13.
14.
15.
16.
17.
18.

Sensor Letters 10, 879885, 2012

885

RESEARCH ARTICLE

9.

19. V. F. Kononyuk, A. I. Sarakhov, and M. M. Dubinin, Phys. Chem.

8, 1691 (1972).
S. G. Sorenson, E. A. Payzant, R. D. Noble, and J. L. Falconer,
20. A. L. Pulin, A. A. Fomkin, V. A. Sinitsyn, and A. A. Pribylov, Russ.
J. Membr. Sci. 357, 98 (2010).
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