processes

Article
A Computational Fluid Dynamics Approach for the
Modeling of Gas Separation in Membrane Modules
Salman Qadir, Arshad Hussain and Muhammad Ahsan *
School of Chemical and Materials Engineering (SCME), National University of Sciences and Technology, (NUST),
Islamabad 44000, Pakistan
* Correspondence: ahsan@scme.nust.edu.pk; Tel.: +92-51-9085-5125




Received: 1 May 2019; Accepted: 28 June 2019; Published: 3 July 2019


Abstract: Natural gas demand has increased rapidly across the globe in the last decade, and it is set to
play an important role in meeting future energy requirements. Natural gas is mainly produced from
fossil fuel and is a side product of crude oil produced beneath the earth’s crust. Materials hazardous
to the environment, like CO2 , H2 S, and C2 H4 , are present in raw natural gas. Therefore, purification
of the gaseous mixture is required for use in different industrial applications. A comprehensive
computational fluid dynamics (CFD) model was proposed to perform the separation of natural
gas from other gases using membrane modules. The CFD technique was utilized to estimate gas
flow variations in membrane modules for gas separation. CFD was applied to different membrane
modules to study gas transport through the membrane and flux, and to separate the binary gas
mixtures. The different parameters of membrane modules, like feed and permeate pressure, module
length, and membrane thickness, have been investigated successfully. CFD allows changing the
specifications of membrane modules to better configure the simulation results. It was concluded that
in a membrane module with increasing feed pressure, the pressure gradient also increased, which
resulted in higher flux, higher permeation, and maximum purity of the permeate. Due to the high
purity of the gaseous product in the permeate, the concentration polarization effect was determined
to be negligible. The results obtained from the proposed CFD approach were verified by comparing
with the values available in the literature.

Keywords: computational fluid dynamics; membrane module; gas separation;

concentration polarization

1. Introduction
Natural gas is considered one of the significant fossil fuels. It is found in subsurface reservoirs and
mostly produced as a byproduct of oil production. The demand for natural gas has seen a considerable
rise in recent years [1,2]. As per the reports of the U.S. Energy Information Administration (EIA),
global natural gas consumption is increasing 4% annually. It is estimated that 10% of the world power
sector depends on natural gas [3]. By 2040, power production and industrial usage are expected to be
73% dependent on natural gas. Natural gas consists of several chemical species, including methane
(CH4 ), ethane, propane, butane, water vapor, nitrogen, and acidic gases such as carbon dioxide (CO2 )
and hydrogen sulfide (H2 S). The species comprising natural gas, like CO2 , N2 , water vapor, and H2 S,
are considered impurities [4]. The different concentrations of impurities in natural gas is in the range
4–50%, depending on the reservoir. The presence of these impurities can significantly affect pipelines,
in terms of corrosion, and raise health and safety concerns [5]. Therefore, typical pipeline specifications
usually mandate that the concentration of carbon dioxide in natural gas not exceed 2–5 volume percent,
making it necessary to treat natural gas and remove the impurities before it is transported. In recent

Processes 2019, 7, 420; doi:10.3390/pr7070420 www.mdpi.com/journal/processes

Processes 2019, 7, 420 2 of 13

years, the membrane separation process has been widely used because it is more economical compared
to other methods [6].
Membrane gas separation can remove unnecessary species from a gas mixture. The membrane
allows only the desired components of a mixture to pass through because of its selectivity [7]. It is
a widely used process due to its reliability, separation performance, low maintenance, and easy
operation [8]. Moreover, membrane technology is used for the separation of various fuel mixtures in
different industries as a result of economic competitiveness and other current demanding situations
related to competitive environments [9]. It has many applications in industrial sectors, hydrogen
recovery from ammonia, hydrogen recovery in refineries, air separation for oxygen purification, sour
gas treatment, and carbon dioxide removal from natural gas [10]. These processes are integrated
with big industrial units to perform specific industrial operations. It is estimated that the use of
membrane gas separation will increase substantially in 2020 [11]. It is an essential fact that the use of
this technology will decrease the unit operation cost of gas separation and reduce the environmental
hazards [12].
The different mathematical models for the separation of gaseous mixtures using a membrane
were developed using altered assumptions [13]. Recently, it was found that the most commonly
available commercial membrane modules for gas separation were hollow fiber and spiral wound
membrane modules [14,15]. Many researchers have investigated flow behavior with different module
arrangements for gas separation and desalination processes [16,17]. Alrehili’s study [18] showed the
different arrangements of fibers with parallel feed channels that made a hybrid membrane module.
The simulation results of the hybrid module gave better membrane flux for both spiral wound and
hollow fiber membrane module configurations. Ahsan [19] applied computational fluid dynamics
(CFD) modeling to gas separation using a finite difference method in polymeric membranes. Saeed [20]
described laminar flow behavior in spacers with narrow channels, and mass transfer coefficient
calculated with different wire spacing. Karode [21] determined that pressure dropped with bounding
surfaces in a rectangular channel. The effect of shear stresses on both sides of the membrane was
also observed.
Other researchers developed a mathematical algorithm for flow behavior and membrane
surfaces, and investigated the concentration polarization phenomena in gas separation processes [22].
The transfer of CO2 gas molecules through the membrane increased due to higher flux on the feed
side, but rejected molecules of other gases that then accumulated on the membrane surface [23].
For this reason, concentration polarization occurs in membrane processes. Mourgues [24] showed the
effect of concentration polarization on membrane separation processes for both counter-current and
co-current patterns. The most important factors were analyzed based on feed pressure, permeability,
and selectivity of the mixture.
Several researchers developed membrane processes to study the influence of concentration
polarization on the feed side. Ahsan and Hussein [25], in their CFD model, studied energy transfer
phenomena in the membrane using permeation flux. Coroneo [26] developed a three-dimensional
single-tube membrane module to define flux, based on Sievert’s law, considering both membrane
sides. Recently, a non-isothermal model was developed to evaluate the effect of temperature on
permeance [27]. In another study, Chen [28] considered co-current and counter-current flow patterns
of the membrane process at different operating conditions using COMSOL Multiphysics 4.0a software.
Another study looked at plug flow and perfect mixing channel, commonly used for modeling
membrane gas separation, and reported the fluid behavior in permeate [29]. Flat sheet membrane
modules were widely used to evaluate membrane performance. The incompressible Navier–Stokes
model was used to improve the fluid chamber while the solid stress–strain model was used to enhance
the mechanical performance of the module [30].
In this study, the CFD technique was used to solve the model equations. The permeability of the
membrane was measured by introducing the species of interest into the feed gas. The effect of gas flow
profiles on gas separation in the membrane modules is reported. A three-dimensional (3D) model was
Processes 2019, 7, 420 3 of 13

established using CFD simulation in COMSOL Multiphysics software. The geometry of the flat sheet
and spiral wound membrane modules were determined, and co-current and counter-current models
were used to find the flow profiles. The effect of molar flux on species transported en mass through the
membrane was considered. The binary gas mixtures CO2 /CH4 and CH4 /C2 H6 were used for separation
in the flat sheet and spiral wound membrane modules, respectively. The investigated parameters,
permeability, feed pressure, permeate pressure, and feed gas concentration, were compared with the
data available in the literature.

2. Numerical Methods
The CFD technique (COMSOL Multiphysics®4.3, COMSOL, Inc., Burlington, MA, USA, 2012) is
used in simulations looking at flow profiles in the membrane module. In this study, the flat sheet and
spiral wound membrane modules were used for the simulations. The data used for the simulations
were taken from the literature and are shown in Table 1.

Table 1. Properties for membranes modules. Reproduced with permission from R. Qi, M.A. Henson,
Separation and Purification Technology; published by Elsevier, 1998.

Spiral Wound Flat Sheet Membrane

Parameters Units
Membrane Module [31] Module [32]
Feed Pressure 35 × 105 106.7 × 103 Pa
Permeate Pressure 1.05 × 105 1.1 × 103 Pa
Feed gas 0.20 CO2 0.395 CH4 Mole fraction
Permeance 1.48 × 10−9 2 × 10−7 mol/(m2 ·s·pa)
Selectivity 20 2.73
Module Diameter 0.3 6 × 10−3 m
Module Length 1 0.8 m
Thickness 2.84 × 10−3 15 × 10−6 m

The numerical simulations were performed using the COMSOL Multiphysics® package (COMSOL
Multiphysics®4.3, COMSOL, Inc., Burlington, MA, USA, 2012). The spiral wound and flat sheet
membranes were developed with 3D axisymmetric geometry. Fick’s law of permeation was used
for the main transport of diluted species through the membrane. The following assumptions were
made [13].

2.1. Assumptions
1. Steady-state and ideal gas conditions;
2. Isothermal conditions;
3. Solution–diffusion mechanism for permeation;
4. Permeance not dependent on the concentration of gas or the feed pressure;
5. No axial mixing of gaseous molecules;
6. Constant pressure drop on the feed and permeate side.

2.2. Mathematical Modeling of Mass Transport

The model accounts for diffusion transport in a unit cell of the structure sketched in Figure 1.
The unit cell is a small part of the membrane that is representative of the whole membrane. In this
model, the initial flux in the membrane was studied, and corresponded to the largest difference in
concentration between the two chambers on different sides of the membrane. The supporting structure
in the membrane consisted of a mesh structure made up of a dense and rigid polymeric material.
This system was used to classify the permeability properties of a membrane to certain species.
Processes 2019, 7, 420 4 of 13
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Figure 1. Membrane model unit.

Figure 1. Membrane model unit.
2.2.1. Convection and Diffusion Model
2.2.1. Convection and Diffusion Model
In the convection and diffusion model, the mass transport equation contained both phenomena.
In the convection
In chemical engineering, the convectionand diffusion model,
and diffusion the mass
model transportfor
is applicable equation contained
mass transport, both is
which phenomena.
In chemical engineering, the convection and diffusion model is applicable
described by Fick’s Law. In the 19th century, Fick gave the simplest definition of diffusion for mass for mass transport, which
is described by Fick’s Law. In the 19th century, Fick gave the simplest
transport. The mass flux of any species is directly proportional to the concentration gradient due definition of diffusion for mass
to diffusion.transport.
The rateThe mass flux
of change of of any species at
concentration is directly
a point in proportional to the concentration
space is proportional to the secondgradient due to
diffusion. The rate
derivative of concentration with space;of change of concentration at a point in space is proportional to the second
derivative of concentration with space;
∂Ca ∂Ca ∂Ca ∂Ca ∂ Ca ∂2 C ∂22 Ca 2
" 2 #
2a
+ vx + v∂Cy a +∂C vz = DAB ∂Ca + ∂ Ca+ ∂ Ca +
∂C ∂C Ra (1)
∂t ∂x ∂y+vx a +v ∂zy a +v z ∂x=DAB ∂y + ∂z + + Ra (1)
∂t ∂x ∂y ∂z ∂x ∂y ∂z
ConvectiveConvective
transport accounts
transportfor the bulk
accounts forflow
the of
bulkfluid due
flow oftofluid
velocity
due to v. velocity
This term v. vThis
canterm
be v can be
solved analytically or by solving the momentum equation with the mass balance equation.
solved analytically or by solving the momentum equation with the mass balance equation. All these All these
expressionsexpressions
include time (t), and
include timespatial andspatial
(t), and velocity andcomponents are used for
velocity components aremass
usedbalance
for mass with
balance with
convection.convection.
The vx , vy , The
and vvxz, are velocity fields in three dimensions. R a describes the rate of
vy, and vz are velocity fields in three dimensions. Ra describes the rate of reaction reaction
and it shouldandbeitequal
shouldto be
zero
equalas notoreaction
zero as no is involved
reaction is ininvolved
gas separation
in gas in membrane
separation in modules.
membrane modules.
2.2.2. Diffusion Term
2.2.2. Diffusion Term
The chemical species is transferred from high to low regions due to diffusion, and becomes a mass
The chemical species is transferred from high to low regions due to diffusion, and becomes a
transfer phenomenon with time and space. The chemical species is dissolved in a solvent or any gas
mass transfer phenomenon with time and space. The chemical species is dissolved in a solvent or any
mixture, for example as oxygen enrichment in the air. The evolution of species mass transfer depends
gas mixture, for example as oxygen enrichment in the air. The evolution of species mass transfer
on its concentration with respect to time and space. The gradient for diffusion occurs as a result of the
depends on its concentration with respect to time and space. The gradient for diffusion occurs as a
motion of the molecules. Due to the kinetic energy of molecules, they can collide with each other in
result of the motion of the molecules. Due to the kinetic energy of molecules, they can collide with
random directions. Then, flux Na for diffusion can be written as;
each other in random directions. Then, flux Na for diffusion can be written as;
∂ Ca ∂2 Ca∂2 C ∂2 C
" 2 #
2a 2
Na = −DAB N = + + a ∂ Ca ∂ Ca (2)
∂xa -DAB∂y ∂x +∂z∂y + ∂z (2)

where masswhere
transfer occurs
mass as a occurs
transfer result of
asdiffusion DAB
a result of .
diffusion DAB .

2.2.3. Membrane Model

2.2.3. Membrane Model
The unit cell is unit
The a small
cellpart
is a of the part
small membrane module that
of the membrane demonstrates
module the whole membrane
that demonstrates the whole membrane
module. The steady-state diffusion equation, which shows mass transport in a model with
module. The steady-state diffusion equation, which shows mass transport in a model diffusion,
with diffusion,
can be written as;
can be written as;
∂ Ca ∂2 Ca ∂2 Ca
" 2 #
DAB + +2 2= 0 2 (3)
∂x ∂y ∂ C∂z a ∂ Ca ∂ Ca
DAB + + =0 (3)
It can also be represented in terms of a nebula operator;∂x ∂y ∂z
It can also be represented in terms of a nebula operator;
D·∇2 Ca = 0 (4)
D · ∇ Ca = 0 (4)
Processes 2019, 7, 420 5 of 13

where Ca denotes concentration (mole/m3 ) and DAB is the diffusion coefficient of the diffusing species
(m2 /s). All boundaries are considered to be insulating

∂Ca ∂Ca ∂Ca

" #
DAB + + =0 (5)
∂x ∂y ∂z

D ∇Ca ·n = 0 (6)

The two faces are applied as boundary conditions where the concentration of the two components
is set from high to low. Boundary Condition 1 (B.C.1) is considered to be high concentrations on the
feed side and Boundary Condition 2 (B.C.2) is represented on the reject side in low concentrations.
B.C.1
C = C0 (7)

B.C.2
C = C0,1 (8)

2.2.4. Membrane Flux

Diffusion through the membrane was represented in terms of the initial boundary condition C0
and the final boundary condition C0,1 .

D
Na = (C0 − C0,1 ) (9)
δ

where D δ is a barrier with a corresponding thickness.

The permeability (P) of gas can be defined as a product of the diffusion coefficient (D) and solubility
coefficient (S),
P = D·S. (10)

The relationship between partial pressure and concentration is defined as

C = S·p. (11)

The flux through the membrane can be presented in terms of permeability and partial pressure,

P
S
Na = (S·pf − S·ph) (12)
δ
where feed pressure pf and permeate pressure ph are used for calculating gradient across the membrane.
Solubility is obtained using a ratio of the concentration gradient and partial pressure difference for the
binary mixture. The solubility S can be calculated as

∆p
S= . (13)
∆C
This membrane model was used to study gas separation in flat sheet and spiral wound
membrane modules.

2.3. Geometry
A sketch of the geometries of flat sheet and spiral wound membrane modules is shown in Figure 2.
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Figure2.2.Schematic
Figure Schematicdiagram
diagramof
ofthe
theflat
flatsheet
sheetand
andspiral
spiralwound
woundmembrane
membranemodule.
module.

2.4.Meshing
2.4. Meshing
Figure 2. Schematic diagram of the flat sheet and spiral wound membrane module.

Thesubdomains
The subdomainsare areoften
oftencalled
calledelements
elementsororcells,
cells,and
andthe
thecollection
collectionofofall
allelements
elementsor
orcells
cellsisis
2.4. Meshing
calledaamesh
called mesh(Figure
(Figure3).3).In
Inthis
thisprocess,
process,aaphysics-controlled
physics-controlledmesh meshwaswasapplied.
applied.An Anextremely
extremelyfine
fine
The
grid subdomains
gridelement
elementwas are
wasused, often
used,while called elements
whilea afurther
further or
increase
increase cells,
did
did and
notnot the
affect
affect collection
thethe model
model of all elements
results.
results. TheThe or
mesh
mesh cells is
consisted
consisted of
called a mesh
of 1,324,604
1,324,604 (Figure
domain
domain 3).elements,
In this
elements, andprocess,
and
46,750 aboundary
46,750 physics-controlled
boundary mesh
elements,
elements, and and
900was
900applied.
edge edge An were
extremely
elements
elements were finethe
usedused
for for
grid element
the
flat sheet was used,
flat membrane
sheet while amodule.
membrane
module. further
The meshincrease did not
Theconsisted
mesh of affect
consisted the
of model
3,257,454 results.
3,257,454
domain domainThe 413,420
elements, mesh consisted
elements, 413,420
boundary
of elements,
1,324,604 domain
boundaryand elements,
elements, and
andelements
3439 edge 3439 edge46,750 boundary
elements
used for theused elements,
forwound
spiral and
the spiral 900 edge elements
wound module.
membrane were
membrane module. used for
the flat sheet membrane module. The mesh consisted of 3,257,454 domain elements, 413,420
boundary elements, and 3439 edge elements used for the spiral wound membrane module.

Figure 3. Meshing of membrane module. (a) flat sheet; (b) spiral wound.
Figure 3. Meshing of membrane module. (a) flat sheet; (b) spiral wound
3. Results
3. Results Figurewas
CFD analysis 3. Meshing of membrane
performed for themodule. (a) flatand
flat sheet sheet; (b) spiral
spiral wound
wound membrane modules.
The simulation
CFD analysiswas was
carried out using
performed forCOMSOL Multiphysics
the flat sheet and spiral software
wound5.2a. Fluxes modules.
membrane of gases and
The
3. Results
concentration variations were found across the length of membrane modules.
simulation was carried out using COMSOL Multiphysics software 5.2a. Fluxes of gases and Various parameters like
feed pressure,
CFD
concentration concentrations
analysis was performed
variations across
were forthe
found length
the
across of the
flat the
sheet module,
and
length permeability,
spiral
of wound modules.
membrane and feed
membrane were considered
modules.
Various The
parameters
in this study.
simulation was carried out using COMSOL Multiphysics software 5.2a. Fluxes of gases and
concentration variations were found across the length of membrane modules. Various parameters
Processes 2019, 7, x FOR PEER REVIEW 7 of 13
Processes 2019, 7, 420 7 of 13
like feed pressure, concentrations across the length of the module, permeability, and feed were
considered in this study.
3.1. CH4 /C2 H6 Separation
3.1. CH4/C2H6 Separation
The flat sheet membrane module is usually used for pilot plant testing or lab scale testing.
Theseparation
The flat sheet membrane
of methanemodule is usually
and ethane used for pilot
was considered forplant testing
the flat sheetormembrane
lab scale testing.
module The
in this
separation of methane and ethane was considered for the flat sheet membrane
study. The simulation of a flat sheet membrane module was performed to check the concentration module in this study.
Thechange
simulation ofreject
on the a flatand
sheet membrane
permeate module
sides. The feed wasgasperformed
entered the to membrane
check the concentration
module and the change
permeate
on the reject at
collected and
thepermeate
bottom of sides. The feedAgas
the module. entered model
cross-flow the membrane module
with specific and theconditions
boundary permeate was
collected
used. at Thetheboundary
bottom ofconditions
the module. A cross-flow
included a high model with specific on
feed concentration boundary
the rightconditions
side and low was feed
used. The boundary
concentration on conditions
the left side. included
Figure a4ahighshowsfeedtheconcentration
concentration onvariation
the rightofsideCHand4 onlowthe feed and
concentration
permeate sides.on theTheleftcontour
side. Figure
shows4athe shows the concentration
concentration variationvariation
of gas on of CHsides
both 4 on the feed
of the and
membrane.
permeate sides. The contour shows the concentration variation of gas on both sides
The slice centration shows the gas variations in the center of the module. Figure 4b shows the differing of the membrane.
Theconcentration
slice centration showsfrom
variation the gas variations
the feed side to inthethe center side.
permeate of theThe module.
gas moved Figure 4b shows
through thesheet
the flat
differing concentration variation from
module and permeate collected at the bottom. the feed side to the permeate side. The gas moved through the
flat sheetFigure
module and permeate collected at the bottom.
4c shows the concentration gradient of CH4 present in the flat sheet membrane module.
Figure 4c shows
Streamlines the concentration
were used for concentration gradient of CH
gradient 4 present in the
representation inflat sheet
Figure 4c.membrane module.from
The lines moving
Streamlines were used for concentration gradient representation in Figure
high to low and passing through the membrane represent the gas diffusion through the membrane. 4c. The lines moving from
highTheto low and passing through the membrane represent the gas diffusion through
membrane is located in the center of the module and the permeate is shown on the bottom surface. the membrane.
TheThe membrane is located
results verified thatin the center
a gradient wasofpresent,
the module andgas
and that thediffused
permeate is shown
through on the bottom
the membrane. The flux
surface. The results verified that a gradient was present, and that gas diffused
was calculated for the given parameters using COMSOL Multiphysics software. The contour in through the membrane.
TheFigure
flux was 4dcalculated
indicates the forflux
the given parameters
variations using
in the flat COMSOL
sheet membrane Multiphysics
module. The software.
color barThe contour
shows the flux
in Figure 4d indicates the flux variations in the flat sheet membrane module.
magnitude in the module. The flux calculated in the module can be explained by Fick’s law. The color bar shows the
flux magnitude in the module. The flux calculated in the module can be explained by Fick’s law.

Figure 4. (a) CH4 gas concentration variation in the flat sheet membrane module; (b) slice shows CH4
Figure 4. (a) CH4 gas concentration variation in the flat sheet membrane module; (b) slice shows CH4
gas variation in the
gas variation in center of the
the center of module; (c) line
the module; shows
(c) line the concentration
shows gradient
the concentration variation
gradient in thein the
variation
membrane module and (d) diffusive flux variation for CH 4 in a flat sheet membrane module.
membrane module and (d) diffusive flux variation for CH in a flat sheet membrane module.
4
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3.2. CH4 /CO2 Separation
3.2. CH4/CO2 Separation
The simulation of a spiral wound membrane module was presented to show the concentration
of The
feedsimulation
CO2 on the of reject
a spiral wound
and permeatemembrane
sides. module
The feed wasgaspresented
entered theto show the concentration
membrane module from the
of central
feed COtube2 on the reject and permeate sides. The feed gas entered the membrane module from the
and moved through to the end. The module shows that the concentration of CO2 changed
central tube andFigure
throughout moved5a. through to the
The high end. The module
concentration wasshows
appliedthat
tothe
theconcentration
first wrapped ofsheet
CO2 changed
as a boundary
throughout Figure 5a. The high concentration was applied to the first
condition, permeate collected in the permeate channel, and a low concentration was wrapped sheet as a boundary
applied to the
condition, permeate collected in the permeate channel, and a low concentration was applied to the
second plate of the membrane module.
second plate of the membrane module.
The contour shows that the gas concentration varied along the membrane on the permeate and
The contour shows that the gas concentration varied along the membrane on the permeate and
reject sides. Figure 5b shows the slice concentration of CO2 in a spiral wound membrane module.
reject sides. Figure 5b shows the slice concentration of CO2 in a spiral wound membrane module. The
The result shows the concentration variation in the center of the module. It verifies that the gas diffused
result shows the concentration variation in the center of the module. It verifies that the gas diffused
through the membrane from the feed channel and collected in the permeate channel. Figure 5c shows
through the membrane from the feed channel and collected in the permeate channel. Figure 5c shows
thethe concentration
concentration gradient
gradient present
present in spiral
in the the spiral
woundwound membrane
membrane module module
for CHfor CH4 /CO2 separation.
4/CO2 separation.

The arrows show that the gas passes through the membrane from the feed side to thepermeate
The arrows show that the gas passes through the membrane from the feed side to the permeatecollector
of the module. The results prove that a gradient was present, and that
collector of the module. The results prove that a gradient was present, and that the gas diffusedthe gas diffused through the
membrane.
through Figure 5d
the membrane. shows
Figure the diffusive
5d shows flux magnitude
the diffusive flux magnitudein the spiral
in the wound
spiral wound membrane
membranemodule
for COfor
module 2 . The
CO 2diffusive
. The flux
diffusive magnitude
flux in
magnitude the membrane
in the module
membrane was
module obtained
was using
obtained concentration
using
concentration and permeability parameters. The flux through the membrane was calculated in separation
and permeability parameters. The flux through the membrane was calculated in the gas the
gasprocess and process
separation depended and on gas diffusion
depended on gas in the perm-selective
diffusion membrane,
in the perm-selective due to the
membrane, due pressure
to the and
pressure and concentration
concentration gradient. that
gradient. It illustated It illustated that mass
mass transport transport
occurred through occurred throughinthe
the membrane the spiral
membrane in the spiralmodule.
wound membrane wound membrane module.

Figure 5. (a) CO2 gas concentration variation in the spiral wound membrane module; (b) slice shows
Figure 5. (a) CO2 gas concentration variation in the spiral wound membrane module; (b) slice shows
CO4 gas variation in the center of the module; (c) line shows concentration gradient variation in the
CO4 gas variation in the center of the module; (c) line shows concentration gradient variation in the
membrane module and (d) diffusive flux variation for CO4 in the spiral wound membrane module.
membrane module and (d) diffusive flux variation for CO4 in the spiral wound membrane module.
Processes 2019, 7, x FOR PEER REVIEW 9 of 13

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3.3. Parametric Study of the Spiral Wound Membrane Module

Feed
3.3.Pressure and
Parametric Permeate
Study Pressure
of the Spiral Wound Membrane Module
The membrane length was considered for the spiral wound membrane module, and the results
Feed Pressure and Permeate Pressure
were verified via the literature. Figure 6 shows that permeate pressure was a function of membrane
length The
for membrane length was
different values. considered
Basically, the for the spiral
permeate wound membrane
pressure module,
was less than theand
feedthepressure.
results
were verified via the literature. Figure 6 shows that permeate pressure was a function
Therefore, it was necessary to calculate the changes in permeate pressure according to length. of membrane
length forthe
Increasing different values.module’s
membrane Basically,length
the permeate
decreasedpressure was less than
the permeate the feed
pressure pressure.
because Therefore,
of the gradient
it was necessary to calculate the changes in permeate pressure according to length.
changes throughout the module from the feed side to the reject side. Therefore, less mass transfer Increasing
the membrane
occurred module’s
as a result of less length decreased
gradient the permeate
in the module. It was pressure
observedbecause of pressure
that feed the gradient
hadchanges
a reverse
throughout the module from the feed side to the reject side. Therefore, less mass
effect on permeate pressure. An increase in the feed pressure produced more gradient across the transfer occurred
as a result of less gradient in the module. It was observed that feed pressure had a reverse effect on
membrane, which resulted in higher mass transfer through the membrane. Figure 7 represents the
permeate pressure. An increase in the feed pressure produced more gradient across the membrane,
feed pressure variation with methane recovery in the spiral wound module. The results show that
which resulted in higher mass transfer through the membrane. Figure 7 represents the feed pressure
higher amounts of methane permeate were obtained in the end because a high gradient was
variation with methane recovery in the spiral wound module. The results show that higher amounts of
produced, and gas diffusion through the membrane was very high.
methane permeate were obtained in the end because a high gradient was produced, and gas diffusion
through the membrane was very high.

Figure
Figure6.6.Permeate
Permeatepressure
pressurevariation
variationwith
with module
module length in aa spiral
length in spiral wound
woundmembrane
membranemodule
module
compared with published values [31].
compared with published values [31].

Figure 7. 7.
Figure CH 4 gas
CH variation
4 gas with
variation withfeed
feedpressure
pressurein
inthe
thespiral
spiral wound
wound membrane modulecompared
membrane module comparedwith
with
published
published values
values[31].
[31].

3.4. Parametric Study for the Flat Sheet Membrane Module

Processes 2019, 7, 420 10 of 13

Processes2019,
Processes 2019,7,7,xxFOR
FORPEER
PEERREVIEW
REVIEW 10 of
10 of 13
13
3.4. Parametric Study for the Flat Sheet Membrane Module
FeedPressure
Feed Pressureand andLength
Length
Feed Pressure and Length
ItIt was
was observed
observed that that the
the permeate
permeate concentration
concentration changed
changed along along the
the length
length of of the
the module.
module. The The
more It was observed
permeable that the permeate
components passed concentration
through the changed along
membrane theother
while lengthcomponents
of the module. wereThe more
left as
more permeable components passed through the membrane while other components were left as
permeable
rejects.The components
TheCH CH44gasgaswas passed
wasmore
moresuitablethrough
suitablefor the membrane
forpermeation
permeationthrough while
throughthe other components
themembrane.
membrane.Figure were left as
Figure88demonstrates rejects.
demonstrates
rejects.
The
thatCH the 4 gas
mole was more suitable
fraction of CH for permeation
increased on thethrough
permeatethe side
membrane.
across Figure
the 8 demonstrates
length of the module thatand
the
that the mole fraction of CH4 increased on the permeate side across the length of the module
4 and
mole fraction
decreased
decreased on of
theCH
onthe 4 increased
reject
reject side,with
side, withon the permeate
respect
respect tolength.
to length. side
Theacross
The ethanethe
ethane gaslength
gas of the
increased
increased onmodule
on thereject
the reject and
side
side decreased
because
because
on the reject
the permeation
the permeation of side, with
of ethane respect
ethane through to
through the length. The
the membrane
membrane wasethane gas
was very increased
very low. on
low. Therefore, the
Therefore, the reject side
the maximum because
maximum possiblepossiblethe
permeation
purityof
purity ofthe ofgas
the ethane
gas wasthrough
was achieved.
achieved. the membrane was very low. Therefore, the maximum possible purity
of theFigure
gas was
Figure 9 achieved.
shows that increasing
9 shows that increasing the the feed
feed pressure
pressure causes
causes the the gradient
gradient to to increase.
increase. Due Due toto high
high
Figure
feed pressure,
feed 9 shows
pressure, the that
the permeationincreasing
permeation of the feed
of components pressure
components through causes
through the the
the membrane gradient
membrane increased to increase.
increased whenwhen the Due to high
the driving
driving
feed
forcepressure,
force increased.
increased. the permeation
Therefore,
Therefore, ititwas
wasofestimated
components
estimated thatthrough
that thehigher
the higherthethe
the membrane
feedpressure
feed pressureincreased
thebetter
the when
better the driving
theseparation.
the separation.
force
This was also true for methane recovery on the permeate side because increasing feed separation.
This increased.
was also Therefore,
true for it
methanewas estimated
recovery that
on the
the higher
permeate the feed
side pressure
because the better
increasing the
feed pressure
pressure
This was
resulted in
resulted also true
in more for methane
more pressure
pressure gradientrecovery
gradient and on the permeate
and turbulence
turbulence for side
for mass because
mass transfer. increasing
transfer. Therefore, feed
Therefore, thepressure
the gas resulted
gas passed
passed
in more pressure
through
through themembrane.
the gradient
membrane. The
The and turbulence
permeate
permeate values
values forcalculated
mass transfer.
calculated theTherefore,
bythe
by numericalmodel
numerical the
model gasfor
passed
for through
thespiral
the spiral wound
wound the
and
membrane.flat sheet
The membrane
permeate modules
values are
calculated shown
by the in Table
numerical 2 for
and flat sheet membrane modules are shown in Table 2 for comparison with published data. Amodelcomparison
for the with
spiral published
wound and data.
flat A
sheet
maximum
membrane
maximum modules difference
difference of 10.8%
areofshown
10.8% in and
and 8.7%
Table
8.7% was
2 for found
wascomparison for
found for the the spiral
withspiral wound
published
wound and
data. flat
andAflat sheet
maximum membrane
difference
sheet membrane
ofmodules,
10.8% and
modules, respectively.
8.7% was found for the spiral wound and flat sheet membrane modules, respectively.
respectively.

Figure8.8.8.Mole
Figure
Figure Molefraction
Mole fractionof
fraction ofmethane
of methanewith
methane withfeed
with feedpressure
feed pressurein
pressure inthe
in theflat
the flatsheet
flat sheetmembrane
sheet membrane module
membranemodule compared
modulecompared
compared
with published
withpublished
with values
publishedvalues [32].
values [32].
[32].

Figure9.
Figure
Figure 9.9.Mole
Molefraction
fractionof
ofmethane
methanechange
methane changewith
change withaaalength
with length of
lengthof the
ofthe flat
theflat sheet
flatsheet membrane
sheetmembrane module
membranemodule compared
modulecompared
compared
with
with published
withpublished values
publishedvalues [32].
values [32].
[32].
Processes 2019, 7, 420 11 of 13

Table 2. Comparison of the model results with the published data for CH4 (permeate) at different
values of selectivity.

Spiral Wound Membrane Modules Flat Sheet Membrane Module

CH4 (Permeate) CH4 (Permeate)
Selectivity Difference Selectivity Difference
PA /PB Published This (%) PA /PB Published This (%)
[31] Model [32] Model
20 0.881 0.786 10.8 2 0.457 0.417 8.7
40 0.936 0.903 3.5 4 0.672 0.635 5.5
60 0.952 0.913 4.1 6 0.749 0.718 4.2
80 0.967 0.929 3.9 8 0.891 0.829 6.9

4. Discussion
Computational fluid dynamics simulations were used to study mass transport in spiral wound
and flat sheet membrane modules. Three-dimensional geometrics were considered to analyze the
membrane-based gas separation for the binary gas mixture. Counter-current and cross-flow membrane
models were used to verify the results. The simple Fick’s law was used to explain mass flux transport
of the binary gas mixture through the membrane. The membrane model was defined using COMSOL
Multiphysics software for the separation of the binary mixture. The membrane model was applied as
a thin diffusion barrier, which allowed certain species to pass through the membrane. The effect of
molar flux for species in mass transport through a membrane was considered. In the present model,
the different parameters were investigated to verify the models in the literature. Different gas mixtures,
like CO2 /CH4 and CH4 /C2 H6 , were investigated in different membrane modules.
A spiral wound membrane module was discussed for CH4 /CO2 membrane separation. The module
geometry consisted of three flat sheets that wrapped around a central tube. The membrane collector
was present at the center of the feed and reject sides. The cross-flow model was applied to verify the
literature results. In the spiral wound membrane module, the increase in membrane length showed
a considerable decrease in concentration polarization. When the length of the membrane increased,
an increase in the residual mole fraction was observed. An increase in the permeate purity was also
observed, which indicated that the concentration polarization was negligible.
A flat sheet membrane module was considered for the separation of CH4 /C2 H6 . The model
showed a variation of membrane results that have been discussed. This was novel work describing
the flow profiles of gases in different membrane modules. The contour also showed the total flux,
concentration gradient, and diffusive flux magnitude of different membrane modules. The investigated
parameters were compared with published results. It was observed that in a flat sheet membrane
module with increasing feed pressure, the pressure gradient also increased, which resulted in higher
flux, higher permeation, and maximum purity of the permeate. The concentration polarization was
observed to be negligible. Furthermore, with increasing module length in the flat sheet membrane
module, a decrease in concentration polarization was observed because the increase in the module
length resulted in more permeation of the desired component and an increase in permeate purity.
In the spiral wound membrane module, increasing the membrane length resulted in a considerable
decrease in concentration polarization. When the length of the membrane was increased, an increase
in the residual mole fraction was observed. An increase in the permeate purity was also observed,
which indicated that the concentration polarization was negligible.

5. Conclusions
The membrane modules were modeled using CFD to obtain the maximum possible value of the
desired gas in the permeate. The effect of concentration polarization on gas separation performance
was negligible. Different parameters were studied in the membrane modules, such as feed pressure,
module length, permeate pressure, and feed concentration. Increasing feed pressure in the membrane
modules caused the pressure gradient to increase. Therefore, maximum mass transfer occurred through
Processes 2019, 7, 420 12 of 13

the membrane. Moreover, the length was considered to show gas variation in the permeate. In the
end, the contours of gas flow profiles in the membrane modules were successfully reported. Modeling
predictions were compared with the published data and validated, and it was found that there was
good agreement between them for the different values of selectivity. The comparison indicated that
the membrane modules were very efficient in terms of the separation of the desired gas at a higher
pressure gradient.

Author Contributions: A.H. proposed the main idea and methodology; S.Q. performed the CFD analysis and
wrote the manuscript; M.A. and A.H. provided key suggestions and improved the manuscript.
Funding: This research received no external funding.
Conflicts of Interest: The authors declare no conflicts of interest.

List of symbols
C Concentration of a (mol/m3 )
DAB Diffusion coefficient (m2 /s)
C0 Initial concentration (mol/m3 )
C0,1 Final concentration (mol/m3 )
P Permeance (mol/(m2 ·s·pa))
S Solubility in the membrane (mol/(m3 ·pa))
pf Feed pressure (Pa)
ph Permeate pressure (Pa)
∆ Membrane thickness (m)
∆C Difference in concentration (mol/m3 )
∆p Gradient of the partial pressure of gases (Pa)
Na Diffusive flux (mol/m2 ·s)

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