The industry widely uses membrane gas separation as it
presents many advantages over other methods, such as
cryogenic distillation or adsorption [1]. In particular, the
economic efficiency of the method has been proven in natural
gas treatment [2, 3]. The main advantage is that membrane gas
separation does not involve a phase change, leading to less
energy consumption than cryogenic distillation [4]. On the
other hand, cryogenic distillation has about 90 % higher
energy consumption than membrane gas separation processes
[1]. Further advantages of membrane gas separation
technologies are their simplicity, small footprint, and ease of
scaling [1]. Nevertheless, designing a membrane application
involves experimental activities to generate the required data,
especially permeances [5].
Mathematical modeling in membrane gas separation is
already in use. Wala-wender et al. [6]. Furthermore, Pan et al.
[7] developed mathematical calculation models for different
flow patterns in the seventies. Many articles about
mathematical modeling in membrane gas separation have
been published recently [811]. Until now, a prediction of the
permeance is not available based on process conditions. Lee
et al. developed a model for permeability prediction [12]. This
mathematical model is based on the configurational entropy
of the membrane and allows for predicting a specific
membrane's permeability. Prabhakar et al. developed a model
to predict permeability depending on temperature and rubber
polymers' concentration [13]. This paper uses a mathematical
model to predict permeance and selectivity mainly based on
the process conditions. The prediction is based on the partial
pressure difference between the two sides of the membrane
since this is the driving force in membrane gas separation [14,
15].
The predicted selectivity is used in a countercurrent
model, which is solved with a finite element approach. It is
more efficient than solving differential equations to calculate
permeate mole fraction values than experimentally obtained
values from the literature [16]. Case Study 1 compares an
asymmetric high-flux membrane's values by Pan et al. that
separates helium from methane [17]. The second case study
compares the values from an air separation experiment by
Merrit et al. using nano-porous carbon as a membrane material
[18].
As the introduction mentions, the model is based on the
partial pressure difference ∆p. Equation 1 shows the basic
equation used to predict the permeance. The variables on the
left which describe the flux and consist of the permeate flow
rate VP, the permeate mole fraction yP, and the membrane
area Am must be known. The driving force is calculated by
the developed model and used with the known variable on the
left side of equation 1 to predict the permeance P
.

󰆄
󰆈
󰆈
󰆈
󰆈
󰆅
󰆈
󰆈
󰆈
󰆈

(1)
The partial pressure is calculated by the relation given in
equation 2, in which PA is the partial pressure of species A, p
is the total pressure, and xA is the mole fraction of species A.
(2)
The model is derived based on the countercurrent flow
pattern shown in Fig. 1 P1, A, P2, A, and P3, A, are the points at
which the partial pressure is calculated and represent the feed
inlet, reject outlet, and permeate outlet.
Computational Analysis of Permeance Prediction for Gas Separation
Membrane Using Countercurrent Flow Model
MUHAMMAD AHSAN1, THOMAS LETTENBICHLER2
1School of Chemical & Materials Engineering National University of Sciences and Technology, Islamabad 44000,
PAKISTAN
2Management Center Innsbruck – Department of Environmental, Process & Energy Engineering, Innsbruck, AUSTRIA
Abstract: - Gas separation polymeric membranes have gained significant attention in various industries, including gas
processing, petrochemicals, and environmental applications. Accurately predicting the permeance of these membranes is
crucial for optimizing their design and performance. This paper presented a numerical prediction model for the permeance
of a binary gas mixture under various process conditions, using only algebraic equations to minimize the calculation effort.
The model considers input parameters such as feed and permeate flow rates, feed pressure, feed and permeate mole fraction,
and membrane area. It demonstrates the behavior of permeance and selectivity in this study. The study also presented two
case studies that utilize predicted selectivity to model counter-current flow and compare the results with experimental data
from the literature. The first case study involves recovering helium from natural gas using an asymmetric high-flux
membrane. The second case study separates air using nano-porous carbon as the membrane material. The numerical
analysis successfully accurately predicted the permeance of gas separation polymeric membranes. The model accounted
for variations in membrane thickness, feed composition, and operating conditions, providing valuable insights into the
overall performance of the membrane system. It also allowed for the optimization of membrane design and operational
parameters to enhance separation efficiency and productivity. The study showcased the effectiveness of numerical
techniques in accurately predicting membrane performance. The developed model can be a valuable tool for membrane
designers and engineers, enabling them to optimize the design and operation of gas separation systems.
Key-words: - Permeance, Numerical Modeling, Membrane Gas Separation.
Received: March 12, 2024. Revised: August 5, 2024. Accepted: September 8, 2024. Published: October 9, 2024.
1. Introduction
2. Numerical Model
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
Muhammad Ahsan, Thomas Lettenbichler
E-ISSN: 2945-0519
32
Volume 3, 2024
Fig. 1. Countercurrent flow model for the derivation of the
equations
The following general assumptions are made for the
mathematical model:
Isothermal conditions
There is no interaction between the different gases
of the binary gas mixture
Plug flow on the permeate and the feed side
Steady-state conditions
Ideal gas conditions
The permeate is under atmospheric pressure
Only a slight pressure drop of approximately 3 kPa
occurs on the feed side
The model's basis is the overall mass and component
balances, equations 3 and 4. LF is the feed flow rate, xF is the
feed mole fraction, LR is the reject flow rate, xR is the reject
mole fraction, VP is the permeate flow rate and yP is the
permeate mole fraction.
(3)
(4)
The partial pressures are calculated on the high-pressure
side at the feed inlet and the reject outlet, equations 5 and 6.
On the low-pressure side, partial pressure is required at the
permeate outlet, equation 7.

(5)
 󰇛 󰇜
(6)

(7)
The variables P1,A is A's partial pressure at the feed inlet,
P2, A's partial pressure at the reject outlet, and P3, A's partial
pressure on the permeate side.
With the definition of stage cut θ, the ratio between VP
and LF and equations 1 and 2, the reject concentration xR
needed in equation 9, can be calculated via the component
balance. The calculation of the partial pressures of
component B follows the same scheme; since this model
deals only with binary gas mixtures, the concentration of B in
the feed is defined by 1 xF, and so on for permeate and
reject. This procedure leads to equations 8, 9, and 10, which
calculate B's partial pressures.
 󰇛 󰇜
(8)
 󰇛 󰇜 󰇛 󰇜
(9)
 󰇛 󰇜
(10)
As the next step, the differences between A and B's
partial pressures are calculated separately because these are
the driving forces in membrane gas separation. Thus,
equations (11) and (12) are the pressure differences between
P1 and P3 and P2 and P3, respectively.

(11)

(12)
The mean driving force across the membrane is
calculated using the average of equations 11 and 12.

(13)
󰇛 󰇜

(14)
Since the permeate flow, the membrane area, and the
permeate mole fraction are input parameters, and the
developed model calculates the mean partial pressure
difference, all variables from equation (1) are known. Hence,
the permeance for A and B can be calculated with equations
13 and 14, respectively. P
A is the permeance of component A,
P
B is the permeance of component B. The selectivity or ideal
separation factor α* is calculated using the ratio between
equations 13 and 14.
Since some approximations are applied to the model,
such as atmospheric pressure on the low-pressure side, the
permeate mole fraction used in the mass balance and an input
parameter cannot be directly used to calculate the
permeances. Also, the permeate mole fraction at the right
edge of the membrane application is unknown and must be
first estimated. Therefore, an additional permeate mole
fraction variable y'P is introduced, calculated by multiplying
yP the permeate mole fraction used initially with a factor
c. Factor c is varied from 0 to 1. At the end of each calculation
loop after the permeances and the selectivity are calculated
with a certain y'P the selectivity is used as input in the
quadratic equation (general solution in membrane gas
separation) to calculate the corresponding permeate mole
fraction. As the last step, the difference between the result of
the quadratic equation and y'P is calculated. This difference is
the loop criteria. As soon as the difference is smaller than 10-
3, the loop stops, and the calculation is completed.
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
Muhammad Ahsan, Thomas Lettenbichler
E-ISSN: 2945-0519
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Volume 3, 2024
Fig. 2. Flow chart for feed flow rate loop.
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
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Volume 3, 2024
Fig. 3. Flow chart for feed pressure loop.
Applying an additional loop in which the previous loop is
nested, the behavior of permeance and selectivity under
changing process conditions can be investigated to the feed
pressure or feed flow rate. The flow charts of these two
programs are shown in Fig. 2 and Fig. 3, respectively. After
predicting the permeance and selectivity, it is used as input for
a countercurrent flow model. The countercurrent flow model
is taken from Ahsan et al. and Geankoplis [16, 19]. As a result,
the model's permeate mole fractions and the reference values
are compared.
The input parameters for the problem are taken from the
literature [5]. In the reference, the permeability of species A is
given with 500×10-10 cm³cm/(scm²cm Hg) and the
selectivity with 10. A comparison of the reference and the
simulated values is shown in Table I.
The feed pressure used for this comparison is 253 kPa, and
the feed flow rate is 106 cm³/s. Also, a feed mole fraction of
3. Results and Discussion
3.1 The behavior of permeance and selectivity
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
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Volume 3, 2024
0.209, a stage cut of 0.4, a membrane area of 6.9×108 cm² and
a permeate mole fraction of 0.45 are input parameters for the
calculation. The main challenge is that the permeate mole
fraction on the right edge of the membrane application is
unknown; therefore, this value is initially estimated. The
mathematical algorithm described in section 2 shows that the
permeate mole fraction on the right edge is calculated
iterativelyfinally, the feed flow rate and the feed pressure
increase after each calculation loop.
The effect of increasing the feed flow rate on the
permeances is shown in Fig. 4. Again, a linear influence on
both permeances is observed. Whereby the permeance ratio
remains constant, leading to a constant selectivity. This
behavior is consistent because selectivity is assumed to be a
membrane material property. By changing the feed pressure,
the behavior differs from changing the feed flow rate. The
variation of the feed pressure has a potential influence on the
permeances and selectivity. The results are shown in Fig. 5
and Fig. 6 for the permeances and the selectivity, respectively.
TABLE I. PERMEANCE AND SELECTIVITY VALUES WERE OBTAINED
WITH THE DEVELOPED MATHEMATICAL MODEL
Variable
Unit
Model result
Literature [5]
Difference
(%)
P
A
Barrer/cm
2.2 × 10-5
2.0 × 10-5
10.0
P
B
Barrer/cm
1.8 × 10-6
2.0 × 10-6
10.0
α*
-
12.4
10.0
24.0
Fig. 4. The permeance of A and B over Feed flow rate, with
xF=0.209, pF=253 kPa, θ=0.4, Am=6.9×108 cm2, and yP=0.45.
Helium is mainly required for its chemically inert
properties, low density, and cryo-genic applications [20].
These properties make it worth separating it from natural
gas. Helium-rich natural gas consists of up to 4 % Helium
[20]. This case study deals with separating a binary
mixture of helium and methane. The other components of
natural gas are not considered in the simulation. The
selectivity is first predicted and then used as input in a
countercurrent model. The numerically calculated
permeate mole fraction values obtained by the developed
mathematical model are compared with the generated
values from Pan et al. [17]. The developed model predicts
the selectivity with 66.4 and uses these values as input in
the countercurrent flow model, solved using a finite
element approach [5, 16]. As input parameters, a stage cut
of 0.23, a permeate mole fraction of 0.9863, a pressure
ratio of 0.05, and a feed mole fraction of 0.6 is used [16].
A pressure ratio of 0.05 leads to a feed pressure of 2027
kPa because on the permeate side, 1 atmosphere is
assumed. The result is shown in Fig. 7; the solid line is the
mathematical model, and the triangles refer to the
reference values from Pan et al. [17].
The developed model's result fits the experiment's
data quite well. However, in the end (at low xR values),
the experimental data are slightly higher than those
calculated with the developed mathematical model. A
comparison is shown in Table II.
Fig. 5. The permeance of A and B over feed pressure, with
xF=0.209, LF=1×106 cm³/s, θ=0.4, Am=6.9×108 cm2, and yP=0.45.
Fig. 6. The selectivity of A and B over feed pressure,
with xF=0.209, LF=1×106, θ=0.4, Am=6.9×108 cm2, and
yP=0.45.
TABLE II. COMPARISON BETWEEN THE MATHEMATICAL MODEL AND
REFERENCE VALUES.
xR
yP model
yP [17]
Difference (%)
0.03
0.9415
0.9211
2.2
0.06
0.9573
0.9414
1.7
0.085
0.9636
0.9512
1.3
0.12
0.9689
0.9602
0.9
0.24
0.9779
0.9754
0.25
0.48
0.9863
0.9863
0.0
The calculation assumes that the feed mole fraction of O2
and N2 are 0.198 and 0.802, respectively. Thus, all other
components usually present in the air are neglected in the
simulation. The experiment is carried out by Merrit et al. at a
feed pressure of 413.7 kPa and uses nanoporous carbon as
membrane material [18].
The developed model predicts a selectivity of 6.3 and is
used as input in the countercurrent model. As input values for
predicting a stage cut of 0.01, a permeate mole fraction of
3.2 Case Study I: Helium recovery
3.3 Case Study II: Air separation
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
Muhammad Ahsan, Thomas Lettenbichler
E-ISSN: 2945-0519
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Volume 3, 2024
0.479 and a feed mole fraction of 0.198 are used. The results
are shown in Fig. 8 and Table 3. The values calculated with
the model are compared with the experimentally determined
values of Merrit et al. [18]. However, the result is somewhat
worse than the results of Case Study I. This is mainly due to
the higher feed pressure in Case Study I. The higher feed
pressure compensates better for the assumed atmospheric
pressure on the low-pressure side.
Fig. 7. The selectivity is predicted with a stage cut of 0.23,
a permeate mole fraction of 0.986, a pressure ratio of 0.05, and
a feed mole fraction of 0.6. The solid line is the developed
mathematical model's solution, and the triangles are the
reference values [17].
TABLE III. COMPARISON BETWEEN THE MATHEMATICAL MODEL AND
REFERENCE VALUES.
θ
yP model
yP [18]
Differences (%)
0.01
0.449
0.479
6.3
0.13
0.421
0.421
0.0
0.27
0.385
0.363
6.1
0.31
0.375
0.347
8.1
0.40
0.351
0.326
7.7
0.47
0.332
0.302
9.9
0.65
0.283
0.266
6.4
Fig. 8. Results of Case Study II. The triangles refer to the
experimentally obtained permeate mole fractions by Merrit et
al. [18].
The comparison in the Case Studies shows that the
developed model calculates permeate mole fractions
comparable to those given by Pan et al. and Merrit et al. [17,
18]. The results obtained in Case Study 1 are slightly better
than those obtained from Case Study 2. This is mainly due to
the higher feed pressure in Case Study 1. The higher feed
pressure compensates better for the assumption of
atmospheric pressure on the permeate side, leading to better
results in Case Study 1. In part 1, the behavior of permeance
and selectivity was investigated by changing the feed flow rate
and pressure. The results show that increasing the feed flow
rate leads to a linear increase in permeance. The ratio between
the two permeances remains constant, which results in a
constant selectivity. This behavior is expected, as selectivity
is assumed to be a material property of the membrane and
should not be influenced by the feed flow rate. A change in
the feed pressure leads to a potential behavior of both
permeances and selectivity. The selectivity decreases with
increasing feed pressure. The examination of equations 13 and
14 shows a 1/∆p relationship that leads to the observed
behavior observed in Fig. 5 and Fig. 6. Since the molar
fraction of the permeate is an input parameter and must be
known in advance, an experiment to determine the permeate
composition is necessary; therefore, it would be great to
improve the model to eliminate the permeate mole fraction
parameter. This model is only able to deal with binary gas
mixtures. However, dealing with multi-component mixtures
for industrial applications would be interesting because most
gas streams consist of more than two components. Therefore,
extending this model to a multi-component mixture would be
meaningful. Also possible would be a coupling of different
mathematical models, like the thermodynamic model from
Lee and coworkers [12] or the temperature dependency model
of Prabhakar et al. [13], to improve the accuracy and scope of
the mathematical models.
LIST OF ABBREVIATIONS
LF
Feed flow rate
LR
Reject flow rate
VP
Permeate flow rate
xF
Feed mole fraction
xR
Reject mole fraction
yP
Permeate mole fraction
P1
Partial pressure at the feed inlet
P2
Partial pressure at the reject outlet
P3
Partial pressure on the permeate side
Δp
Partial pressure difference
Δpav
Mean partial pressure difference along
the membrane
pF
Feed pressure
pP
Permeate pressure
ploss
Pressure drop on the high-pressure side
P
Permeance
α*
Selectivity
θ
Stage cut
Am
Membrane area
4. Conclusion
International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
Muhammad Ahsan, Thomas Lettenbichler
E-ISSN: 2945-0519
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Volume 3, 2024
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References
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Conflict of Interest
The authors have no conflicts of interest to declare
that are relevant to the content of this article.
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International Journal of Chemical Engineering and Materials
DOI: 10.37394/232031.2024.3.5
Muhammad Ahsan, Thomas Lettenbichler
E-ISSN: 2945-0519
38
Volume 3, 2024