1418 Chem. Eng. Technol. 2007, 30, No.

10, 1418–1425

Maryam Peer1 Research Article

Seyyed Mehdi Kamali1
Mohammad Mahdeyarfar1
Toraj Mohammadi1
1
Research Laboratory for
Separation Processes,
Chemical Engineering
Department, Tehran, Iran.
Separation of Hydrogen from Carbon
Monoxide Using a Hollow Fiber Polyimide
Membrane: Experimental and Simulation
The separation of hydrogen from carbon monoxide (syngas ratio adjustment)
with polymeric membranes was investigated in this work. A polyimide hollow fi-
ber membrane module was used for hydrogen separation. This polymer has
shown large permeability and selectivity for hydrogen separation (selectivity of
ca. 30). Permeation tests were carried out at different feed conditions. Feed flow
rates were varied between 150–300 mL/min, temperature was varied in the range
of 20–80 °C and feed pressure was varied between 5–9 bar. Mixtures containing
0–50 % carbon monoxide were used when carrying out experiments. Measured
membrane permeances for hydrogen and carbon monoxide were about 70–
100 GPU (gas permeation units) and 3–5.5 GPU, respectively. In addition, a
mathematical model for simulation of gas separation in hollow fiber membrane
modules with all flow patterns (crossflow, countercurrent and cocurrent) was
presented. This model can be used for calculation of membrane performance or
its required surface area for a specific separation. Experimental results have
shown good correlation with simulation results. Plasticization, competitive sorp-
tion and concentration polarization effect of carbon monoxide on membrane
performance is shown with experimental results. This effect reduced hydrogen
permeances in mixed gas experiments.

Keywords: Membranes, Modeling, Multicomponent gas mixtures, Separation

Received: May 09, 2007; revised: July 11, 2007; accepted: July 25, 2007
DOI: 10.1002/ceat.200700173

1 Introduction Hydrogen separation from carbon monoxide has been inves-

In recent years, gas separation with membrane technology has
become an attractive alternative to traditional methods like
pressure swing adsorption and cryogenic separation. Some of
the industrial process applications of this technology are air
dehumidification, nitrogen production, hydrogen recovery
from refinery purge gases, natural gas sweetening and helium
separation amongst others [1]. Additionally, separation of hy-
drogen from carbon monoxide in a syngas mixture is another
application of membrane gas separation.
Syngas is commonly produced with a H2 : CO ratio between
1 and 3. In order to use a syngas mixture to produce acetic
acid, methanol, plasticizers and other valuable petrochemical
products, this ratio must be reduced.
– [10–12]. In Coker and Freeman’s model, the effect of being
Correspondence: M. Peer (m_p_ahang@yahoo.com), Research Labora-
tory for Separation Processes, Chemical Engineering Department,
Narmak, Tehran 16846-13114, Iran.
tigated by many researchers. Hinchliff and McCandless studied
separation of mixtures using different concentrations and dif-
ferent polymers as the membrane material [2, 3].
In addition to experimental work, many researchers have
tried to simulate membrane behavior. Binary gas mixture sepa-
ration, with some simplifying assumptions like perfect mixing,
has been simulated by some researchers [4, 5]. Sengupta and
Sirkar have studied the separation of ternary gas mixtures with
countercurrent and cocurrent flow patterns [6, 7].
A detailed model was developed by Pan for multicomponent
gas mixtures, but his method for solving the differential equa-
tions was very complicated [8]. Kaldis presented a model for
simulation of gas mixture separation with an orthogonal collo-
cation method [9]. Other researchers also tried to develop a
general model for the simulation of membrane gas separation
countercurrent or cocurrent in each membrane element was
considered [13]. This is the reason for the consistency of their
model with experimental data.

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Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425 Modeling 1419

In this work, hydrogen separation from carbon monoxide in
a syngas mixture (syngas ratio adjustment) was investigated by
a hollow fiber polyimide membrane module. Gas permeabil-
ities and selectivities in polyimide membrane using different
conditions of pressure, temperature, concentration and feed
flow were determined experimentally. Results showed an in-
crease in pure gas permeance by increasing pressure. In mixed
gas experiments, however, an increase in pressure reduced the
hydrogen permeance and increased the carbon monoxide per-
meance. The plasticization effect tended to increase both gas
diffusivities due to swelling of the polymer matrix.
There are other factors which effect mixed gas separations.
One of them is competitive sorption which tends to decrease
both gas permeances in mixed gas experiments, relative to
their pure state. Another factor is concentration polarization.
Concentration polarization refers to a concentration gradient
building up due to depletion of the more permeable compo-
nent and the accumulation of the less permeable species in the
boundary layer adjacent to the membrane. This causes a de-
crease in the separation efficiency. Usually in a gas membrane
system the concentration polarization may be significant in the
case of having a very large gas permeation rate [14]. Hydrogen
permeance in polyimide is very large relative to carbon mon-
oxide. Therefore carbon monoxide may accumulate at the
membrane surface and may cause the hydrogen permeance to
decrease due to concentration polarization [15].
Using experimental results of mixed gas separations, per-
meance can be evaluated as a function of temperature, pres-
sure, feed flow and feed concentration. A model was developed
for calculation of membrane performance, using Coker and
Freeman’s work as a foundation. This model was developed in
such a way that it can be used to determine the required mem-
brane area for a specific separation. It can estimate an initial
membrane area and calculate the correct required membrane
area for a specific separation. With this model the effect of flow
patterns, pressure losses, purge streams and variable permeance
for gases on membrane performance can be studied. Addition-
ally, the accuracy of the model was studied by comparison of its
results with experimental data for binary and multicomponent
gas mixtures. The authors of this model had not compared their
simulation results with experimental results. In this paper some
comparisons with experimental data of binary and multicom-
ponent gas mixtures have been carried out.
tion of constant permeance for each gas are not signifi-
cantly different from experimental results.
If axial dispersion is also considered, plug flow certainly
changes into a parabolic profile and X and Y in Eq. (10) (de-
tailed later) would not be dependent only on length; and so
their changes with radius should be considered when deriving
the governing equations1). In that case there would be two di-
mensional concentration distribution profiles in both shell and
bore side of the fibers. In fact the driving force for permeation
would also be changed.
For simulation each fiber was divided into N equal stages
and differential mass balance equations were written for each
component in each stage. Then these coupled equations were
solved numerically and the crossflow pattern was chosen as an
initial estimate for solving these equations. However, when sol-
ving the resultant matrix, this assumption was modified for
countercurrent or cocurrent flow patterns. The solution proce-
dure was repeated until convergence was attained, i.e., when
total permeate and retentate flow rate were constant.
The same procedure has also been used for area calculations,
but in this case, an initial estimate for membrane area was re-
quired first. Then this initial estimate was changed until the re-
sultant retentate compositions reached the same level as the
given and desired retentate composition. After writing mass
balance equations for each component and a total mass bal-
ance equation in each stage, governing equations for counter-
current flow in all stages, except the first stage, were obtained
as follows:
l(K,i + 1) – l(K,i) + V(K,i – 1) – V(K,i) = 0 (1)
B(K,i) l(K,i – 1) + C(K,i) l(K,i) D(K,i) + l(K,i + 1) = 0 (2)
B, C and D are only simplifying parameters and are defined
as follows:
 
V…i 1† Q…K† DA Pf
B…K; i† ˆ 1‡ (3)
Pv DA Q…K† L…i 1†
V…i 1†
C…K; i† ˆ 1 ‡ ‡
Pv DA Q…K†
 
V…i† Q…K† DA Pf
1‡ (4)
Pv DA Q…K† L…i†

V…i†
D…K; i† ˆ 1 (5)
2 Modeling Pv DA Q…K†
In the first stage:
The assumptions made for developing this model are:
I. The membrane module operates at steady state. C(K,1) l(K,1) + D(K,1) l(K,1) – V(K,0) = 0 (6)
II. The gas on the shell side of the module and on the bore
side is in plug flow.  
III. All fibers have the same inner and outer diameter. V…1† Q…K† DA Pl
C…K; 1† ˆ 1 ‡ 1‡ (7)
IV. There is no axial mixing in the bore or shell side of the Pv DA Q…K† L…1†
module.
V. Permeabilities of the gases are constant. This assumption is V…1†
D…K; 1† ˆ 1 (8)
for simplifying the derivation of the governing equations. Pv DA Q…K†
In fact, permeance is dependent on pressure, temperature,
component composition (in mixed gas experiments) and –
membrane type. But simulation results with the assump- 1) List of symbols at the end of the paper.

© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.com

1420 M. Peer et al. Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425
2 3 2
32 3
C…K; 1† D…K; 1† l…K; 1† V…K; 0†
6 B…K; 2† C…K; 2† D…K; 2† 76 l…K; 2† 7 6 0 7
6 76 7 6 7
6 ::::: :::: ::::: ::::: :::::: 76 :::: 7 6 0 7
6 76 7 6 7
6 B…K; i† C…K; i† D…K; i† :::::: 76 l…K; i† 7 ˆ 6 0 7 (9)
6 76 7 6 7
6 :::::: ::::: :::::: :::::: :::::: 76 :::: 7 6 0 7
6 76 7 6 7
4 B…K:N 1† C…K; N 1† D…K; N 1† 54 l…K; N 1† 5 4 0 5
B…K; N† C…K; N† l…K; N† D…K; N† l…K; N ‡ 1†

The tridiagonal matrix, which can be solved by Thomas al- l(K,i + 1) + V(K,i + 1) – l(K,i) – V(K,i) = 0 (12)
gorithm is as Eq. (9).
In order to solve this matrix, a crossflow pattern was chosen The governing equation that must be solved in this case is as
as an initial estimate, and then this assumption was modified follows:  
V…i†
with matrix solving: V…K; i ‡ 1† ‡ 1 ‡ l…K; i†
Q…K† DA Pv

l…K; i† ˆ   (13)
Q…K† Pf XR…K; i† Pv Y…K; i† V…i† P V…i†
Y…K; i† ˆ0 (10) 1‡ ‡ f
PR

Q…K† DA Pv Pv L…i†
Q…K† Pf XR…K; i† Pv Y…K; i†
iˆ1 The solving procedure must be repeated for all flow patterns
For the R component in the gas mixture, there would be a until convergence. The convergence conditions are as follows:
set of R–1 independent nonlinear algebraic equations which    
DL…1†  
was solved by the Jacobian method. The initial estimates that  h10 8 and DV…N†h10 8 (14)
 L…1†   V…N† 
are needed to solve these equations in stage N are calculated
from the following equation: Visual Basic was used for solving all these equations. Eq.
(10) governs the crossflow patterns. This equation can be
Q…K† XR…K; N ‡ 1†
Y…K; N† ˆ (11) solved by the Jacobian method and an appropriate initial esti-
P
R
Q…m† XR…m; N ‡ 1† mate is provided by Eq. (11).
mˆ1
For all other stages, except stage N, the initial estimates for
component compositions are those compositions which are 3 Experimental
calculated at the previous stage.
For cocurrent flow in the membrane module, there was a In order to carry out the experiments, the gas permeation set-
simpler solving method and there was no need for matrix sol- up shown in Fig. 1 was used. An asymmetric polyimide hollow
ving. The assumptions are the same for this flow pattern. Only fiber membrane module with an effective area of 12.56 cm2
the total mass balance equation in each stage was changed as and measuring 1 m in length was used. It was prepared by Ube
follows: industries. In Fig. 2 the molecular structure of this polymer is

Figure 1. Experimental setup.

© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.com

Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425 Modeling 1421

Figure 2. Molecular structure of polyimide used in this study.

shown. Ar is an aromatic divalent radical. Pure gas permeation

tests were carried out with N2, H2 and CO, respectively. Mixed
gas experiments were carried with a temperature range for feed
of 20–80 °C. When investigating the effect of pressure on
membrane performance and gas permeances, feed pressure
was varied between 5–9 bar. Mixtures containing 0, 10, 25, 40
and 50 % CO with a flow of 150–300 mL/min were used for
carrying out the permeation tests. Feed was introduced at the
shell side and permeate was collected from the bore side of the
fibers. The flow pattern in the module was countercurrent.
Figure 4. Comparison between simulation and experimental re-
Permeate flow rate was measured by a bubble flow meter.
sults for a multicomponent gas mixture, effect of feed pressure
The permeate stream was linked to a GC with a TCD detector on retentate composition.

(a)
and a Molecular Sieve 5/A column. Column temperature was
100 °C and the TCD current was 35 mA.
Permeability and selectivity calculations for mixed gas mix-
tures were performed with the following equations:
V 1 1
Pi ˆ (15)
1 A …pf xi pv yi †
y1=
x
a…i;j† ˆ y2 1 (16)
=x
2
xi is the logarithmic mean of feed and retentate compositions
and is defined as follows:
…xif xir †
xi ˆ   (17)
ln xif=xir

(b)
4 Results and Discussion
In this section simulation results are compared with experi-
mental data from the literature, for binary and multicompo-
nent gas mixtures. Also, results of experimental tests which
were obtained from our permeation tests with binary mixtures
of H2 and CO are compared with simulation results.

4.1 Simulation Results

For model validation, simulation results for binary and multi-

Figure 3. Comparison between simulation and experimental re-
sults for a multicomponent gas mixture; Effect of stage cut on
(a) permeate composition, and (b) retentate composition.
component gas mixtures were compared with experimental
data from literature at first. A multicomponent gas mixture
containing 67.5 % H2, 11.5 % CO2, 16.7 % CH4 and 4.3 %
C2H6 which was used by Kaldis et al. in their experiment was
chosen for simulation. They varied the feed flow rates from
5–30 nL/h to investigate the effect of stage cut on membrane
performance. Pure gas permeability of each gas was obtained
experimentally. These values were 2.9 · 10–4, 0.93 · 10–4,
0.037 · 10–4, 0.0064 · 10–4 cm3/cm2 s–1cmHg–1 for H2, CO2, CH4

© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.com

1422 M. Peer et al.
and C2H6, respectively. According to Figs. 3 and 4, simulation
and experimental results were very consistent.
4.2 Comparison between Experimental and
Simulation Results
After carrying out the permeation tests, permeance, selectiv-
ities, permeate and retentate compositions were measured and
calculated. These tests were carried out at different feed flow
rates and pressures. The effect of these parameters on selectiv-
ity, permeance and permeate composition were investigated
and compared with simulation results at the same conditions.
At first, hydrogen, carbon monoxide and nitrogen pure gases
were used when carrying out the tests. Results of pure gas ex-
periments are shown in Fig. 5a). It shows that permeance of all
pure gases increased with increasing pressure and permselec-
tivity slightly increased. This was because of the increasing
driving force as pressure increased. In fact, carbon monoxide
showed accelerated plasticization effects and its permeance in-
creased with increasing pressure. In Fig. 5b), the effect of feed
pressure on hydrogen permeance for a mixture containing
75 % hydrogen and 25 % carbon monoxide is shown. A de-
crease in hydrogen permeance with increasing pressure can be
(a)
H2CO permselectivity
Permeance / GPU
Feed pressure / bar
(b)
H2 permeance / GPU
/ min-1
/ min-1
/ min-1
Feed pressure / bar
Figure 5. Effect of feed pressure on permeance in (a) pure gas
tests, and (b) mixed gas tests.
© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim
Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425
seen in all flow rates. Also plasticization effects tends to in-
crease both gas permeance, however, competitive sorption and
concentration polarization effects make the hydrogen per-
meance decrease with increasing pressure, as can be seen.
Mixed gas tests were performed using a mixture containing
a constant concentration of 75 % hydrogen and 25 % carbon
monoxide. The effect of pressure and feed flow rates were in-
vestigated with these tests. In some tests, pressure was kept
constant and feed flow rate was changed and in others, pres-
sure and feed flow rate were kept constant, but feed concentra-
tion was changed. The feed flow rate was changed within the
range of 150–300 mL/min. Feed pressure and concentration
were in the range of 5–9 bar and 10–50 % carbon monoxide,
respectively. Also a simulation was done for the same mixtures
with the same conditions, and results were compared with ex-
perimental data. This comparison can be seen in Figs. 6 and 7.
In Fig. 6, the effect of feed flow rate, i.e., stage cut, at differ-
ent feed pressures on hydrogen composition in the permeate
stream is shown. As expected, with increasing feed flow rate
and decreasing stage cut, permeate composition increased.
Comparing these three diagrams, it can be seen that the differ-
ence between simulation and experimental results was more
significant at higher pressures, i.e., 9 bar. At higher pressures
polyimide was plasticized by carbon monoxide. Carbon mon-
oxide permeance increased by increasing pressure as in the
pure gas case because of plasticization effect. In mixed gas
tests, however, hydrogen permeance decreased by increasing
pressure. As explained before, it was because of a concentra-
tion polarization effect introduced by carbon monoxide at the
membrane surface.
As a result, carbon monoxide concentration increased and
hydrogen concentration in the permeate stream decreased.
This effect was not taken into account for the simulation, so
this caused the larger difference between simulation and ex-
perimental results at higher pressures. All three diagrams have
the same dimensions to illustrate greater differences at higher
pressures.
In Fig. 7, test results with different feed concentrations are
shown. These tests were carried out at a constant feed flow of
300 mL/min. As expected, with increasing feed concentration,
permeate composition also increased. As seen in the previous
figure, as pressure increased the differences between simulation
and experimental results increased. Also, at all pressures, when
carbon monoxide concentration in the gas mixture was high,
i.e., more than 40 %, the difference between simulation and ex-
periment was a slightly larger. When carbon monoxide con-
centration increases, its effect on polyimide plasticization and
concentration polarization increases, and this is the main rea-
son for greater deviation from simulation results at high con-
centrations of carbon monoxide.
As shown above, the effect of feed pressure and partial pres-
sure of hydrogen on permeate composition are greater than
the effect of feed flow rate. Also, from the experimental data,
the effect of temperature on membrane performance was in-
vestigated. In Figs. 8a) and 8b) the effect of temperature on
hydrogen permeance and membrane selectivity, respectively,
are shown. Increasing temperature has a significant effect on
the diffusion coefficient of smaller hydrogen molecules. As a
result, temperature increase elevated membrane selectivity.
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Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425 Modeling 1423

The diffusion coefficient of small hydrogen molecules in poly- controlled [16]. So with increasing temperature hydrogen per-
imide is much larger than carbon monoxide. In other words, meance increased. Since carbon monoxide permeation
the permeation of hydrogen through membrane is diffusivity through polyimide is solubility controlled, because of its large

(a)

H2 permeate composition / vol

Permeate composition / vol

(a)

H2 feed composition / vol

-1
Feed Flow / ml min

(b)
H2 permeate composition / vol
Permeate composition / vol

(b)
H2 feed composition / vol
-1
Feed Flow / ml min
(c)
H2 permeate composition / vol
Permeate composition / vol

(c)
H2 feed composition / vol

-1 Figure 7. Effect of feed composition on hydrogen permeate com-

Feed Flow / ml min
position and comparison with model at (a) feed pressure =
Figure 6. Effect of feed flow rate on hydrogen permeate compo- 9 bar, (b) feed pressure = 7 bar, and (c) feed pressure = 5 bar.
sition and comparison with model at (a) feed pressure = 9 bar,
(b) feed pressure = 7 bar, and (c) feed pressure = 5 bar.

© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.com

1424 M. Peer et al. Chem. Eng. Technol. 2007, 30, No. 10, 1418–1425

Simulation results have shown good consistency with ex-

perimental data, even when pure gas permeances were used.
However, because pure gas permeance were used in simula-
tion, at higher pressures differences between simulation and
experimental results, are a little greater. This is because of plas-
H2 permeate / GPU

ticization, competitive sorption and concentration polariza-

tion effects at higher pressures in mixed gas experiments,
which were not considered in simulation.
With this simulation and experimentally obtained per-
meances, required membrane area for a specific separation can
be calculated and optimum operational condition can be
found.
(a)

Symbols used
Feed Temperature / ºC
K [–] component number
i [–] stage number
pf [bar] feed pressure
pu [bar] permeate pressure
Q(K) [f t3/f t2h-1 bar–1] permeability of component K
m(K,i) [f t3/h] permeation rate of component K
Selectivity

in stage i
XR(K,i) [–] composition of residue side for
component K in stage i
Y(K,i) [–] composition of permeate side
for component K in stage i
D(A) [f t2] membrane area in each stage
(b)
y i, xi [–] permeate and retentate
composition of component i,
Feed Temperature / ºC
respectively
Vi [f t3/h] total permeate flow rate of
Figure 8. Effect of temperature cut on (a) H2 permeance, and component i
(b) membrane selectivity. A [f t2] total membrane area
V(i) [f t3/h] total flow rate of permeate
solubility coefficient in polyimide [16], temperature increase leaving stage i
did not increase carbon monoxide permeance very much. In L(i) [f t3/h] total flow rate of residue leaving
total, membrane selectivity increased with increasing tempera- stage i
ture. V(K,i) [f t3/h] permeate flow of component K
leaving ith stage
l(K,i) [f t3/h] residue flow of component K
5 Conclusions leaving ith stage
xif, xir [–] feed and retentate compositions
This study showed that polyimide has good potential as a of component i, respectively
membrane material for separation of hydrogen from carbon
monoxide. Also it was found that the results of pure gas per-
meation tests are not suitable for simulation. This is because References
with a mixed gas there are some deviations from the pure gas
case, which may result in large differences in membrane per- [1] R. R. Zolandz, G. K. Fleming, Gas Permeation, Membrane
meance for gases and required membrane area. It was shown Handbook (Eds.: W. S. W. Ho, K. K. Sirkar), Van Nostrand
that in mixed gas experiments, hydrogen permeance decreased Reinhold, New York 1992.
with increasing pressure, because of concentration polarization [2] A. B. Hinchliff, Ph. D. Thesis, University of Aston, Birming-
and competitive sorption effects, and domination of these ef- ham, UK 1991.
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however, increased in both pure and mixed gas experiments (4), 470.
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tion to the plasticization effect on the membrane had a larger J. Membr. Sci. 1996, 118 (2), 289.
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so increased the permeance of both gases, especially hydrogen. [6] A. Sengupta, K. K. Sirkar, AICHE J. 1987, 33 (4), 529.

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© 2007 WILEY-VCH Verlag GmbH & Co. KGaA, Weinheim http://www.cet-journal.com