Journal of Membrane Science 497 (2016) 458471

Contents lists available at ScienceDirect

Journal of Membrane Science

journal homepage: www.elsevier.com/locate/memsci

Strategies for the simulation of multi-component hollow bre

multi-stage membrane gas separation systems
Michael Binns a, Sunghoon Lee a, Yeong-Koo Yeo a, Jung Hyun Lee b, Jong-Ho Moon b,
Jeong-gu Yeo b, Jin-Kuk Kim a,n
a
b

Department of Chemical Engineering, Hanyang University, Wangsimni-ro 222, Seongdong-gu, Seoul 133-791, Republic of Korea
Korea Institute of Energy Research, 152 Gajeong-ro, Yuseong-gu, Deajeon 305-343, Republic of Korea

art ic l e i nf o

a b s t r a c t

Article history:
Received 18 February 2015
Received in revised form
6 August 2015
Accepted 10 August 2015
Available online 13 August 2015

Gas separation membranes allow the preferential removal of certain gases from a mixture of gases. If the
separation objective is to obtain high product purity and either high removal efciency or high product
recovery it is often necessary to implement a multi-stage network of membranes. However, in the literature most modelling approaches consider the simulation of single-stage membranes. Hence, the aim
of this study is to identify stable and computationally efcient strategies for simulating complex multistage membrane systems. For this purpose a multi-stage membrane modelling framework is developed
and six different stable solution strategies are evaluated and compared in terms of the computational
effort required to solve the resulting sets of equations. These solution strategies vary according to the
sequence in which the individual membrane models are solved (sequential and simultaneous approaches) and the manner in which those membrane models are initialised. In all these strategies a
NewtonRaphson method is employed to solve the mass balance equations in both single-stage and
multi-stage membrane systems. Comparisons are made using example simulations of 10 different congurations of membranes containing 14 membranes with different numbers of connections and recycle
streams present.
& 2015 Elsevier B.V. All rights reserved.

Keywords:
Multi-stage membranes
Simulation strategy
NewtonRaphson method
Gas separation

1. Introduction
A single-stage membrane used for gas separation will typically
have a single stream of feed gas and two exit streams called the
permeate and retentate as shown in Fig. 1. The permeate stream
contains gases which have passed through the membrane and the
retentate contains any remaining gases from the feed.
For hollow bre membranes there is a choice to be made as to
whether to insert the feed into the bore side (inside the hollow
bre) or the shell side (outside the hollow bre). In either case the
hollow bres will generally be encased in a module containing
multiple bres so that the pressures of both sides of the membrane are contained and pressurised appropriately. Additionally
there are three basic congurations including co-current, countercurrent and cross-ow which vary depending on the direction of
ow, location of the exit streams and the inuence of permeateside mixing.
There have been a number of articles which describe methodology for the simulation of single-stage membranes. The
n

Corresponding author.
E-mail address: jinkukkim@hanyang.ac.kr (J.-K. Kim).

http://dx.doi.org/10.1016/j.memsci.2015.08.023
0376-7388/& 2015 Elsevier B.V. All rights reserved.

equations which are used to describe these systems normally form

a boundary value problem, i.e. sets of differential equations with
boundary conditions at the inlet and outlets. One of the most
commonly used and cited method for the simulation of multicomponent membrane separations is the work of Pan [1] and they
implement an iterative method (a shooting-type method [2]) to
solve this boundary value problem where they repeatedly integrate along the membrane until reaching convergence. However,
a number of authors have made simplifying assumptions and
modications which allow the conversion of this problem into an
initial value problem [3,4] which is simpler to solve.
Alternatively, authors such as Coker et al. [5] and Katoh et al.
[6] have tackled the boundary value problem directly by dividing
the membrane into a number of sections or tanks which is
equivalent to a nite-difference approach to solve the problem.
The methods for obtaining numerical solutions describing
these membrane separations can then be divided into those which
require initial values for ow rates, compositions and pressures
inside the membrane such as those of Pan [1] and Coker et al. [5]
and other methods which state that no initial values are required
[4,7] (methods which require no initial values should converge
starting from a poor/crude initial guess rather than requiring a
good initial values). The method of Kaldis et al. [7] uses collocation

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

459

Permeate outlet
Permeate

Retentate
Feed

Retentate outlet

Fig. 1. Tanks-in-series model representation of a hollow-bre membrane operated in the counter-current conguration.

together with the Brown method to solve the equations for a

single-stage membrane while the method of Kundu et al. [4]
converts the problem in to an initial value problem which is solved
through dynamic integration using Gears method incorporating a
variant of Newtons method. In both cases the authors state that
their methods are both stable and computationally efcient.
However, the accuracy and computational effort required by
these approaches and by the nite difference methods depend on
the size of the time steps for integration methods, the number of
collocation points for collocation methods and the number of
sections/tanks for nite-difference methods. These numbers are
typically chosen such that the models are sufciently accurate to
reproduce experimental results. For example Kaldis et al. [7] state
that only 6 collocation points are required to reproduce the experimental results of Pan [1] within an accuracy of 5% while Coker
et al. [5] suggest that 100 nite difference tanks are sufcient for
most modelling purposes.
Additionally, a major limitation of most membrane simulation
methodologies is that they consider only the solution of singlestage membranes. This is a signicant point because it is known
that multi-stage membrane systems are normally required to obtain high purity and high removal efciency. For example Baker [8]
suggests that due to pressure ratio and selectivity limits in commercial membranes a single-stage system may be unable to provide the required separation. Additionally Low et al. [9] show that
for CO2 capture a single-stage membrane is unable to simultaneously give high CO2 purity and recovery.
Hence, there are many articles in the literature such as that of
Ahmad et al. [10] which consider the simulation and optimisation
of multi-stage membrane systems. Although it is possible to use
single-stage methods to model multi-stage systems through the
sequential simulation of the different connected membranes this
can be a computationally inefcient approach. In particular for
cases where one or more of the outlet streams are recycled (e.g. to
enhance product recovery) this sequential solution strategy may
require a large number of iterations before it converges to a
steady-state solution for the whole system. This is shown by Makaruk and Harasek [11] who implement a methodology which
sequentially and repeatedly simulates single-stage membranes in
order to obtain solutions for multi-stage membrane systems. In
their results they show that for cases involving 2 membrane stages
with a recycle thousands of iterations are required to obtain a
solution. Hence, single-stage methods can be used to model multistage systems but depending on the membrane conguration and

the algorithm used this can be a computationally inefcient

approach.
Ahmad et al. [10] have developed methodology for the simulation of single-stage membranes which they use repeatedly
within a process simulator environment to simulate multi-stage
membrane systems. However, other authors including Khalipour
et al. [12] and Kundu et al. [4] have presented methodology for
simulation of single-stage membranes and state that their methodologies can be applied to multi-stage membrane systems but
they do not specify how their methodology should be extended to
these multi-stage membrane systems. Hence, it is presumed that
they use a similar approach as Ahmad et al. [10] repeatedly using
their single-stage membrane methodology.
This sequential approach has also been used inside optimisation with the LevenbergMarquardt method for the upgrading of
both biogas from natural gas [13] and for the extraction of hydrogen from biomass gasication [14]. However, in both cases it is
assumed that a large computational effort was required due to the
large numbers of iterations required for each simulation.
Additionally a number of authors have suggested methods for
the simultaneous solution of multi-stage membrane systems. For
example authors such as Qi and Henson [15] and Scholz et al. [16]
have included the equations for multi-stage membrane systems as
non-linear constraints inside their MINLP optimisation methods.
As these authors do not mention any convergence issues (e.g. due
to numerical stiffness) which might occur at high or low stage cut
it is assumed that implicit methods together with damping are
used which should be able to handle most cases without difculty.
Also, in both cases these authors have used either simplied or
shortcut models and they do not state the computational requirements of their multi-stage simulations or of the optimisations which are carried out with these models. Katoh et al. [6] have
also considered the simultaneous solution of multi-stage membrane systems, in their case using a dynamic relaxation method
which should be a stable method for solving such systems but may
require large numbers of small time steps to reach a steady-state
solution. Although the number of steps can often be greatly reduced using variable step-length methods the number of steps
required can still be very large in some cases (depending on the
stiffness of the problem, the algorithm used and tolerances specied). Hence, dynamic methods may be computationally slow
(generally much slower than steady-state methods), but they are
essential if the dynamic behaviour of the system is being studied.
So in summary for the solution of multi-stage membrane

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M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

systems there are three broad classes of solution strategies:

HagenPoiseuille equation.

Dynamic/relaxation-based methods

Sequential -&- repeated use of single-membrane based methods

Simultaneous solution of all membranes

Assumption 6. There is no concentration polarisation.

Process simulators which are used to simulate owsheets

containing multiple different process units (reactors, separators,
heat exchangers, pressure changing units, etc.) can also be used to
model multi-stage membrane systems. These process simulators
contain various sequential and simultaneous convergence methods for solving the different models used to represent each unit
and the various connections and recycle streams [19]. However,
despite the large number of studies which have linked membrane
simulation code/programmes with process simulators (e.g. [3,10])
none of these articles give serious attention to the method of
convergence used for multi-stage membrane systems. For example
Ahmad et al. [10] describe a single-stage membrane visual basic
s
routine which they have used inside Aspen HYSYS for the simulation of a number of different multi-stage congurations but do
not mention which convergence options they have used within
s
Aspen HYSYS .
The choice of convergence methods can have a big effect on the
stability and computational effort required for simulation of multistage systems. Hence, for the purpose of design and optimisation
of membrane systems which may require large numbers of simulations at various different conditions this choice becomes an
important issue (for simulation both inside and outside process
simulators).
The purpose of this article is to give a comparison of different
convergence strategies for the simulation of multi-stage membrane systems. In particular looking at the computational efciency (the CPU time required) and the stability of different initialisation and calculation sequences implemented. Hence, this
work aims to provide guidance as to the most appropriate initialisation and convergence strategies which can be used for simulation and optimisation of complex multi-stage membrane
systems.

2. Methodology
The modelling equations used here are based on those given by
Katoh et al. [6] and Coker et al. [5]. Hence a (nite difference type)
tanks-in-series model (similar to Katoh et al. [6]) is used here to
represent the two sides of the membrane (see Fig. 1). This can be
used to represent any of the common feed ow patterns (crossow, co-current, counter-current) or any of the less common ow
patterns such as those using a sweep gas stream on the permeate
side. In addition the following assumptions are made:
Assumption 1. Membrane permeances are xed, independent of
temperature, pressure and gas composition.
Assumption 2. The geometry of the hollow bres is unaffected by
high pressures.
Assumption 3. There is no temperature change within the
membranes.
Assumption 4. There is no pressure drop on the feed side of the
hollow bres (shell side).
Assumption 5. The bore side pressure drop is described by the

Assumption 7. The gases behave as ideal gases.

These assumptions largely neglect the inuence of non-ideal
effects which limit the accuracy of the model at very high pressures and for membranes with very high selectivity and permeances. However, a model based on these assumptions is still
sufciently accurate for the design of membrane processes. This
has been shown by various studies which have used similar assumptions for the design of membrane processes (e.g. for the
upgrading of biogas [16] and for the separation of CO2 from natural
gas [10]). It is also worth noting that the model presented here
could be modied to include these non-ideal effects, for example,
through the adoption of the equations presented by Scholz et al.
[17].
The approach for simulation of membrane separations requires
calculation of the volumetric ow (at standard conditions) of different gases passing through the membrane and here this is based
on Eq. (1)

Ji, j, n = Q i Am Pr, j xi, j Pp, n yi, n

(1)

where Qi is the permeance of component i, Prj and Ppn are the

retentate and permeate pressures of the jth retentate and the nth
permeate tank and Am is the area of the membrane connecting
those two tanks (see Fig. 1). Also, xij and yin are the mole fractions
of component i in the jth rentate tank and in the nth permeate
tank.
In addition to this permeation of gases through the membrane
the volumetric ow of gases passed between adjacent tanks must
also be considered. The total volume ow rate of gases (including
all components) passing from tank j to tank j 1 is given by Fr,j. If
the permeate is operated in a counter-current direction then Fp,n
represents the volume ow rate of gases passed from tank n to
tank n  1 (in the co-current direction this would be the volume
ow rate from tank n to tank n 1). The following set of Eqs. (2)
(5) are written assuming a counter-current ow pattern, to convert to either co-current or cross-ow would require only simple
modications of Eqs. (3) and (5). These equations are used to represent the separation of a mixture of Cn different gas components
(e.g. CO2, CH4, etc.) using a membrane with Sr tanks used to represent the retentate and Sp tanks used to represent the permeate
in the numerical tanks-in-series model. Typically, a hollow bre
membrane module will include multiple membrane bres (nbre)
and so the total feed should also be divided by the number of bres used. Subsequently Eqs. (2)(5) are used to simulate a single
bre and the total outlet ow rates should be calculated by multiplying by the number of bres used. Additionally, since these
equations are written in terms of the normal volume ow (e.g.
N m3 s  1) the feed ow rate provided should be converted to
these units.
For the rst tank (tank 1) in the retentate Fr,j  1 and xi,j  1 in Eq.
(2) should be replaced by Fr,feed and xi,feed which are the feed ow
rate and composition of the gas feed. Also, for the nal tank (tank
Sp) in permeate the terms Fp,n 1 and yi,n 1 are set equal to zero as
tank Sp is at the end of the membrane (in the counter-current
conguration).

Fr, j 1xi, j 1 Ji, j, n Fr, j xi, j

dxi, j
=
dt
Vr /Sr
dyi, n
dt

(2)

Fp, n + 1yi, n + 1 + Ji, j, n Fp, n yi, n

Vp/Sp

(3)

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

Cn

Fr, j = Fr, j 1

Specify parameters:

Ji, j, n

(4)

i=1
Cn

Fp, n = Fp, n + 1 +

461

feed

d inner

Ji, j, n

feed

P outlet

feed

d outer

n fibre

(5)

i=1

Eqs. (2) and (3) are ODEs (ordinary differential equations) describing the rate of change of retentate and permeate mole fractions and Eqs. (4) and (5) are algebraic expressions for calculation
of the total gas ow rates Fr and Fp. If the numbers of tanks on each
side of the membrane (Sr and Sp) are not equal then the cross
membrane volume ow rates Ji,j,n should then be added together
appropriately in Eqs. (2)(5) to reect the ow rate of gases passing between adjacent tanks. For example Katoh et al. [6] recommend using a greater number of tanks on the permeate side
for a number of applications. It should also be noted that Eq. (5)
will change depending on the direction of the permeate ow rate.
In addition to the gas ow rates this model also requires
knowledge and calculation of pressures on both sides of the
membrane. Here it is assumed that there is no pressure drop on
the retentate side while the permeate side change in pressure
(from one tank to the next) is calculate based on the HagenPoiseuille relation [5] in Eq. (6).

Pn = 128 n ( L/Sp ) Fp, n 1/d 4 (1/ )

(6)

where in this equation L is the effective length of the membrane,

n is the viscosity in the nth tank and d here is the inner diameter
of the hollow bres.
In the work of Katoh et al. [6] the method of calculating viscosities is not specied while in the work of Coker et al. [5] they
specify that the mixing rules of Wilke are implemented but they
do not specify their method for the calculation of pure component
viscosities. The pure component viscosities are calculated here
using the correlations of Lucas and the mixing rules of Wilke
found in the literature [18].
Two different approaches for solving these equations for single-stage membranes are considered here: a relaxation method
and a NewtonRaphson method. These methods are programmed
s
in MatLab and CPU times are obtained for comparison of different
s
methods using an Intel i5 3.40 GHz desktop computer with 8 Gb
of memory.
2.1. Relaxation solution strategy for single-stage membranes
This study aims to nd steady-state solutions for the above set
of differential algebraic equations (DAEs). However, one of the
most stable and reliable methods for achieving this is through the
use of relaxation methods where the above equations are numerically integrated with respect to time until the system reaches
a steady-state. Unfortunately, this often requires a very large
number of small time steps in order to reach the solution without
introducing any large perturbations which cause the method to
either fail or reach an unphysical solution. Hence, this method may
be considered inappropriate for the purposes of optimisation due
to the CPU time required (typically between 5 min and 1 h using
the approach described here). This issue about heavy CPU times is
mentioned by Katoh et al. [6] with regard to the use of small time
steps, however they do not report the CPU times required for their
simulations.
The relaxation method implemented here follows the procedure given in Fig. 2 which is a modication of the explicit Euler
method of integration. This is a relatively simple method, which is
modied here to account for the algebraic equations for total ow
rates and permeate pressures which are recalculated after each

Initialise

x , y , F r , F p , Pp
for all tanks

Compute cross membrane fluxes ( J )

Calculate

Calculate

F r , F p , Pp

dx
dt

dy
dt

and

x = x + dx
dt

y = y + dy
dt

No
Converged?

Yes
Fig. 2. Relaxation-based solution strategy for simulation of gas separation
membranes.

time step.
Alternative more complex relaxation strategies such as that of
Kundu et al. [4] could also be implemented using backward differential methods which simultaneously solve the algebraic
equations while integrating the ODEs. This could increase the
computational efciency but would require the calculation of an
initial point which satises the algebraic equations. However, in
this study the modied explicit Euler method is used because our
goal when using relaxation is to obtain a solution in a simple
manner. Although explicit methods are less stable than implicit
methods small time steps can be used to make this simpler explicit
method more stable and reliable.
2.2. NewtonRaphson solution strategy for single-stage membranes
In order to obtain solutions in a quick and efcient manner we
consider the use of a NewtonRaphson algorithm in order to

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M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

directly solve the set of algebraic equations which are satised at

steady-state. At steady-state Eqs. (2)(6) become the following
algebraic Eqs. (7)(11) which can be solved directly.

0=

0=

x , y , F r , F p , Pp

Initialise

for all tanks

(e.g. using values previously generated by relaxation)

Fr, j 1xi, j 1 Ji, j, n Fr, j xi, j

Vr /Sr

(7)

Fp, n + 1yi, n + 1 + Ji, j, n Fp, n yi, n

Vp/Sp

= ( x , y , F r , F p , Pp )

Set

(8)

Cn

0 = Fr, j 1 Fr, j

Ji, j, n

(9)

i=1
Cn

0 = Fp, n + 1 Fp, n +

Specify parameters:
F

feed

feed

d inner

Ji, j, n

P outlet

feed

d outer

n fibre

Q
L

(10)

i=1

0 = Pn Pn + 1 + 128 n ( L/Sp ) Fp, n 1/d 4 (1/ )

(11)

These equations are solved using the procedure given in Fig. 3

which is the NewtonRaphson method where analytical derivatives of Eqs. (7)(11) are calculated. In this procedure Z represents
the set of unknown variables including x and Fr for each of the Sr
retentate tanks and y, Fp and Pp for each of the Sp permeate tanks.
Also, in Fig. 3 F(Z) is the right hand side of Eqs. (7)(11) and Jac is
the related Jacobian containing derivatives of the terms in F (i.e.
dF/dZ, see [2] for details of the NewtonRaphson method).
This is similar to the method of Coker et al. [5] except that in
their case the pressure drop equation is not solved simultaneously,
rather it is updated following the calculation of ow rates (requiring the subsequent re-calculation of ow rates), an iterative
process which should be repeated until both ow rates and
pressure values are converged. Authors including Chowdhury et al.
[3] and Kundu et al. [4] have pointed out that this approach
(sometimes referred to as a nite difference approach) requires
initial estimates of ow rates along both sides of the membrane.
Additionally estimates of the pressures along both sides of the
membrane are also useful. However, as mentioned by Kaldis et al.
[7] the sensitivity with respect to initial conditions (stability) is not
discussed in the work of Coker et al. [5].
While it is true that methods such as the approach implemented here require initial values for ow rates and pressures
along the membrane, in this study it was found that a single good
solution can be used as an initial point in order to start the process
and can be used to calculate a wide range of different conditions
using the NewtonRaphson method. Hence, using this single
starting point the fast NewtonRaphson method can be used repeatedly within an optimisation procedure to nd the optimal
process conditions.
For the purpose of obtaining this good starting point a
number of different initialisation options have been considered.
One option would be to obtain this initial starting point using a
relaxation-based simulation as described in Section 2.1. However,
additional initialisation options can also be considered using the
available knowledge of the feed (the feed volume ow rate Fr,feed
(for a single bre) and composition xfeed). Hence, the following
different options are considered:
1) Initialisation using the relaxation method

2) xi, j = xi, feed , yi, n = xi, feed , Fr, j = Fr, feed,

Fp, n = Fr, feed (i = 1, Cn; j = 1, Sr ; n = 1, Sp )
3) xi, j = xi, feed , yi, n = xi, feed , Fr, j = Fr, feed/2,
Fp, n = Fr, feed/2 (i = 1, Cn; j = 1, Sr ; n = 1, Sp )

F(Z)

Evaluate function values

Jac ( Z )

Evaluate Jacobian of derivatives

Gaussian elimination
Jac

Update

Z,

-F(Z)

including damping

Z = Z + ( damp

Z )

No
Converged?

Yes
Fig. 3. NewtonRaphson solution strategy for simulation of gas separation
membranes.

4) xi, j = xi, feed , yi, n = xi, feed , Fr, j = Fr, feed, Fp, n = 0 (i = 1, Cn; j = 1,
Sr ; n = 1, Sp )
5) xi, j = xi, feed , yi, n = 0, Fr, j = Fr, feed, Fp, n = Fr, feed (i = 1, Cn; j = 1,
Sr ; n = 1, Sp )
where options 25 are simple initial guesses and options 1 require
a relaxation-based simulation.
To quantify the stability of these different initialisation approaches the maximum allowed damping coefcient (damp, as
shown in Fig. 3) which can be used to converge to a real physical
solution is determined. The use of a smaller damping coefcient in
the NewtonRaphson method (in the range 0 odamp r1 ) allows
for a more stable convergence by reducing the size of the steps
taken. For example this is useful for cases where very high (0.9 4 )
or very low (0.1 o) stage cut ( total permeate outlet ow/total
feed ow) simulations (or any cases involving numerical stiffness)

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

are required. Hence, determining the maximum allowed damping

coefcient gives some empirical measurement of the stability of
the numerical method at each set of conditions. The maximum
value is determined here by testing values 0.1, 0.2, 0.3 ., 1.0 using
and recording the maximum value which converges to the correct physical solution. For cases where the simulation does not
converge even with a damping value of 0.1 the maximum damping
value is recorded as 0 (although it may be possible to converge
using an even smaller damping coefcient).
In general a smaller damping factor makes the convergence of
the procedure more stable however it also increases the computational time (as mentioned by Makaruk and Harasek [11]). Hence
a good strategy to employ is to initially set a small damping factor
(e.g. 0.1) then when the solution converges past a certain tolerance
increase this factor to 1 in order to accelerate the nal
convergence.
In comparison with the relaxation method, this Newton
Raphson solution strategy is very fast and direct, typically nding
a solution using a much smaller number of iterations (compared to
the large number of time steps used for relaxation). The CPU time
involved is typically under 1 s without damping or 46 s if
damping is employed.
2.3. NewtonRaphson solution strategies for multi-stage membrane
systems
As mentioned in the introduction this article aims to compare
different strategies for the simulation of multi-stage membrane
s
systems. In process simulators such as Aspen Plus there are sequential modular and simultaneous (equation-oriented) convergence strategies for the simulation of multi-unit systems [19].
The advantages of the sequential approach include simpler

463

initialisation and less effort required to formulate the problem [19]

but for more complex systems and for optimisation this approach
can become computationally expensive [19]. Alternatively, simultaneous approaches are can potentially be much faster but
require good initialisation [19].
As single-stage membrane models are very commonly used in
the literature the simplest method for the solution of a multi-stage
system would be a sequential modular approach where the singlestage membrane programme is called repeatedly. However, for the
purpose of achieving faster convergence simultaneous approaches
can also be considered at the expense of a more complex initialisation and formulation. Hence, a comparison of different
possible solution strategies is made in this study with the aim to
highlight the most computationally efcient and stable
approaches.
2.3.1. Sequential strategies
When there are multiple membranes present it would seem
natural to implement the NewtonRaphson method developed for
single-stage membranes sequentially for each membrane. Hence,
starting with simulation of the 1st membrane connected to the
feed stream, then simulation of membranes connected to the exit
streams of the 1st membrane, then simulation of membranes
connected to the outlets of those membranes and so on. However,
this can lead to large numbers of iterations required for convergence when there are recycle streams present (requiring repeated simulation of the membranes, updating the ow rates and
compositions of the recycle streams after each set of sequential
simulations). The general procedure for this type of simulation
strategy is shown as the sequential strategy in Fig. 4. When there
are recycle streams present a number of different strategies can be
employed for the updating of recycle stream properties after each

Multi-Membrane Simulation Strategies

Sequential
Set Recycle Flow Rates = 0

Simultaneous
Simple initialisation

Sequential initialisation
Set Recycle Flow Rates = 0

Set Recycle Flow Rates = 0

Steady-state Simulation
of 1st

Membrane
Steady-state Simulation
of 1st Membrane

Steady-state Simulation
of NM th

Membrane
Steady-state Simulation
of NM th

Membrane

Update Recycle Flow Rates

and Compositions using :
Direct substitution / Wegstein /
Newton-Raphson / Broyden

No

Converged?

Update Recycle Flow Rates

and Compositions

Simultaneous

Steady-state

Simulation of all NM membranes

Yes

( including connections and recycles )

Fig. 4. Multi-stage membrane simulation strategies.

464

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

sequence.
A. Direct substitution
B. Wegstein
C. NewtonRaphson
D. Broyden
The four methods considered here include the simple direct
substitution method where the recycle streams are set equal to the
relevant calculated membrane outlets. This method is the most
basic which generally requires large numbers of iterations and so
the other three methods are intended to accelerate convergence
by improving the estimation of these recycle stream conditions
after each sequence of calculations. In the Wegstein method this is
achieved using a simple set of equations which use the values
obtained from previous iterations to improve the estimation of
these unknown recycle stream conditions in subsequent iterations.
Alternatively the NewtonRaphson method can be implemented
for the calculation/convergence of these recycle streams (a nested
approach where the NewtonRaphson method is used twice: for
the solution of single-stage membranes and for the solution of
recycle streams). However, the calculation of the Jacobian for this
NewtonRaphson method requires the calculation of derivatives
using a numerical differences method (not shown in Fig. 4) which
is known to be computationally intensive. For this reason the
Broyden method is also considered which includes a simpler
method for the approximate calculation of the Jacobian allowing
for faster iterations. A description of these methods which are
commonly used in process simulators can be found in the book of
Turton et al. [19].

Considering for example the 3-stage membrane system shown

in Fig. 5 it can be seen that there are three sets of unknown
variables (Z1, Z2 and Z3) which need to be calculated based on
three sets of equations (F(Z1), F(Z2) and F(Z3)). Also it should be
noted that for the rst tank Eqs. (7) and (9) must be modied to
include: the gas feed from the recycles added to the feed and
passed into membrane 1 (F(Z1)), the outlet of membrane 1 passed
into membrane 2 (F(Z2)) and the outlet of membrane 2 passed into
membrane 3 (F(Z3)). For this example the resulting set of equations
which are solved as part of the NewtonRaphson method are
shown in matrix format in Fig. 6 including derivative terms for
each of the three membranes in addition to derivatives related to
the various connections. It should be noted that the Newton
Raphson method is robust and it will still converge to a solution
even if these derivatives related to connections between membranes and recycles are neglected and set equal to zero. In fact,
setting these derivatives equal to zero can increase the stability of
the method since it is effectively removing terms which have the
potential to introduce stiffness into the problem (i.e. due to the
different scales of operating conditions inside the different connected membranes). However, the inclusion of these terms can
also accelerate convergence reaching a solution using fewer
iterations.
The stability and rate of convergence of this simultaneous approach depend on:

the method used for initialisation.

the level of damping employed in the multi-stage Newton
Raphson method.

the inclusion or exclusion of connection/recycle terms in the

Jacobian.

2.3.2. Simultaneous strategies

Alternatively, the NewtonRaphson method can be extended to
solve all the membranes simultaneously, including all connections
and recycles. This is known as the equation-oriented approach
when used in process simulators [19]. In this way a system with
multiple membranes can be simulated in a quick and efcient
manner provided that it is appropriately initialised.
This multi-stage membrane NewtonRaphson method follows
the same procedure shown in Fig. 3, except that now there are one
set of Eqs. (7)(11) included for each membrane (with additional
sets of equations for each of the multiple tanks used in the model
for each membrane). Hence, if there Nm membranes used to separate a gas mixture with CN components, using Sr tanks to model
the retentate and Sp tanks to model permeate, the total number of
equations to be solved will be Nm  [(CN  (Sr Sp)) Sr Sp Sp].
Additionally there will now be an augmented set of unknown
variables Z* (Z1, Z2 ZNm) and subsequently an augmented Jacobian of derivatives Jacbian* containing terms corresponding to
each membrane and to the various connections and recycles.

Here two different initialisation strategies are considered:

1. Sequential initialisation
2. Simple initialisation
In the sequential initialisation approach each membrane is simulated in sequence as shown in the Sequential initialisation
strategy in Fig. 4 providing initial values for the recycle streams
which are subsequently used in the simultaneous methodology
described above. This provides a good initial point from which
the simultaneous method can be used with or without damping.
Alternatively, a Simple initialisation method can also be considered in which all the recycle streams are set to zero ow rate
and these initial values are used directly in the simultaneous
methodology. This gives a lower quality initial point which means
that the method may fail to converge. However, this can be compensated for by using a small damping value inside the multistage NewtonRaphson method and/or by excluding (setting to
P3
R3

P2

Membrane 3

Membrane 2

P1

R2

Z 3 = ( x 3 , y3 , Fr 3 , F p 3 , P p 3 )

Z 2 = ( x 2 , y2 , F r 2 , F p 2 , P p 2 )

Membrane 1

R1

Z 1 = ( x 1 , y1 , Fr 1 , F p 1 , P p1 )

Fig. 5. Example of a multi-stage membrane system with three membranes including recycle streams.

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

Recycle Terms
Membrane 2

465

Recycle Terms

Membrane 1

Membrane 3

Membrane 1

Membrane 1
Derivatives

Z1

F Z1

Membrane 2
Connection Terms
Membrane 1

Z2

Derivatives

F Z2

Membrane 3

Connection Terms
Membrane 2

Membrane 2

Z3

Derivatives

Membrane 3

Jacobian

F Z3

Fig. 6. NewtonRaphson method for simultaneous solution of multi-stage membrane system (in this case using 3 counter-current membranes with recycles).

zero) the connection/recycle terms inside the Jacobian (e.g. see the
connection/recycle terms in Fig. 6).
Hence, two different multi-stage simulation strategies are
recommended:
E. Simultaneous Sequential initialisation
(without damping and including all connection/recycle terms in
the multi-stage Jacobian)
F. Simultaneous Simple initialisation
(with damping and excluding all connection/recycle terms in
the multi-stage Jacobian)
Where strategy E takes advantage of the good initialisation
point provided by the sequential initialisation and hence does not
require any further steps to enhance stability. While Strategy F
starts from a simpler initial point and uses both the stability enhancing modications mentioned above.

Table 1
Parameters used for validation cases.
Number
of bres

Case 1a
20
Case 2b 368
*
a
b

To validate the above equations and modelling approach two

different sets of experimental data from the literature are considered. This validation involves the comparison between model
and experimental results from single-stage membranes. Hence, an
additional assumption made here is that these models can be
extended to multi-stage systems without loss of accuracy. Firstly,
considering the removal of CO2 from natural gas and the experiments carried out by Pan [1]. Secondly, considering the separation
of air and related experiments carried out by Feng et al. [20].
The details of the experimental conditions are given in
Tables 1 and 2 including the feed and permeate outlet pressures,
the numbers of hollow bres, the membrane geometries, the
permeances of each component and the feed composition.
For the case of removal of CO2 from natural gas Pan [1] gives
results based on a counter-current ow pattern provided at different stage cuts (stage cut Permeate ow/Feed ow). For the airseparation case Feng et al. [20] give results based on both countercurrent and co-current ow patterns.
The model results calculated with the procedures in Figs. 2 and
3 (single-stage membrane relaxation and steady-state strategies)
are used to simulate both cases and the comparisons of experimental values from the literature and model predictions are given
in Figs. 7 and 8. It can be seen that the model very accurately

Outer
diameter
(m)

Inner diameter
(m)

Feed
pressure
(kPa)

Permeate
outlet
pressure
(kPa)

0.15
0.25

200
160

80
80*

3528.0
690.0

92.8
100.0

Assumed value.
Pan [1].
Feng et al. [20].

Table 2
Membrane permeance values and feed composition used in validation.
Permeances (GPU)
CH4

C2H6

C3H8

0
0
40.0478
1.8
9.3
0
Feed composition (% volume)

1.1124
0

0.3059
0

0.0596
0

N2

O2

CO2

CH4

C2H6

C3H8

0
79.5

0
20.5

48.5
0

27.9
0

16.26
0

7.34
0

N2

3. Single-stage membrane model validation and stability

analysis

Effective
length
(m)

Case 1a
Case 2b

Case 1
Case 2b
a
b

O2

CO2

Pan [1].
Feng et al. [20].

predicts the outlet concentrations of all components for the

counter-current simulations of both cases. For the air-separation
co-current conguration the model clearly shows a different result
from the counter-current case and despite the small deviation
from experiment the model can still be used to accurately predict
membrane performance with reasonable accuracy.
For the case given by Pan [1] the stabilities of the 5 different
single-stage initialisation options mentioned in Section 2.2 are
tested. For this purpose the maximum damping coefcient is determined for each of the 5 initialisation options for a range of
different feed ow rates / stage cuts (as discussed in Section 2.2).
This is shown in Fig. 9 where it can be seem that initialisation
options 4 and 5 did not converge for any of the conditions tested
(possibly requiring a damping coefcient smaller than the minimum 0.1 tested here) suggesting that these two options are the

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M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

100

100
CO (model)
CO (experiment)
2

Permate composition (% vol)

98

N 2 composition of retentate outlet (% vol)

95

90

85

80

75

96
94
92
90

86
84

70

65
0.35

82

0.4

0.45

0.5

0.55

0.6

0.65

Countercurrent (model)
Countercurrent (experiment)
Cocurrent (model)
Cocurrent (experiment)

88

0.7

0.1

0.2

0.3

0.4
0.5
Stage cut

0.6

80
N2 recovery

Permeate composition (% vol)

20

CH4 (experiment)
C2H6 (model)
C2H6 (experiment)

15

0.9

Countercurrent (model)
Countercurrent (experiment)
Cocurrent (model)
Cocurrent (experiment)

90
25

0.8

100

Stage cut

CH (model)

0.7

70
60
50
40

C H (model)
3 8

30

C H (experiment)
3 8

20
82

84

86

10

88
90
92
94
96
N2 composition of rententate outlet (%vol)

98

100

Fig. 8. Comparison of model predictions against experimental data of Feng et al.

[20].

0.4

0.45

0.5

0.55

0.6

0.65

0.9

0.7

Stage cut

Fig. 7. Comparison of model predictions against experimental data of Pan [1].

least stable. The most stable initialisation options are two of the
simpler options (2 and 3) which are shown to require little or no
damping allowing the maximum damping coefcient to be used
for a wide range of conditions. However, all methods are shown to
require smaller damping coefcients in order to converge at very
high stage cuts. In principle the initialisation using a solution from
the relaxation method calculated at conditions close to those being
simulated with the NewtonRaphson method should be a very
stable approach. However, it is shown here in Fig. 9 that the initialisation using a single solution from the relaxation method is
less stable at feed conditions with stage cut much higher and
much lower than that used to provide the initialisation. So for
example initialisation option 1 which is calculated here at conditions giving stage cut 0.53 is less stable for much lower and
much higher stage cut simulations. Hence, for this reason and
because the relaxation method requires more computational effort
it is only recommended if convergence issues are found using
options 2 or 3 at some certain feed conditions.

4. Example calculations: multi-stage CO2 removal from natural

gas
In order to compare the computational efciency of the six
different strategies considered here (four different sequential
methods and two different simultaneous methods) example calculations have been performed using the ten different membrane
congurations shown in Fig. 10.
For these example calculations a natural gas feed has been

Initialisation option 1
Initialisation option 2
Initialisation option 3
Initialisation option 4
Initialisation option 5

0.8
Maximum damping coefficient

0
0.35

0.7
0.6
0.5
0.4
0.3
0.2
0.1
0

0.1

0.2

0.3

0.4

0.5
0.6
Stage cut

0.7

0.8

0.9

Fig. 9. Comparison of the maximum damping coefcient for different initialisation

options used in the single-stage NewtonRaphson membrane solution method.

selected with composition given by Pan [1] and with a ow rate of

500 Nm3/s (a ow rate similar to that of ue gases from power
plants, another example where membranes are being considered
[21]). In addition the feed pressures of all membranes have been
changed to 400 kPa and the permeate outlet pressures of all
membranes have been changed to 100 kPa. Also, isothermal conditions have been assumed with a temperature of 10 C. Pressure
changing units have not been included in Fig. 10 and it is assumed
that the necessary compressors are used to create this pressure
difference across each of the membranes. In a subsequent step
after the convergence of membrane simulations the costs and
energy requirements of the required compressors and vacuum
pumps can be calculated if required (e.g. for the design of a
membrane system).
Given these feed conditions, pressures and using the permeances given by Pan [1] it is necessary to estimate the required
membrane area which is required to give a signicant separation
of the feed gas. Here the signicant separation mentioned can be

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

467

Fig. 10. Ten congurations used to test multi-stage membrane simulation strategies.

dened as giving a stage cut (fraction of total gas feed permeating

through the membrane) between 0.1 and 0.9 and hence avoiding
extreme situations where all or none of the gas is permeating
through the membrane. For this purpose a modied version of Eq.
(1) can be used to obtain a crude estimate of the membrane area
required based on these conditions (Eq. (12)).

( )

A estimate m2 =

Ffeed N m3 s1

Q max (GPU)7.501 1012P (Pa)

(12)

In this equation Qmax is the largest magnitude permeance value

(from the set of components in the feed) in units of GPU, P is the
pressure difference across the membrane in Pa, Ffeed is the feed

ow rate in N m3 s  1 and Aestimate is an estimate of the membrane

area required in m2. This equation will give a good crude initial
estimate provided that the component of the gas mixture having
the largest magnitude permeance makes up a large fraction of the
total feed. Alternatively for cases where this is not valid Eq. (12)
can be modied to include the average permeance (Qav) of the gas
feed (weighted according to the component fractions) as shown in
Eqs. (13) and (14).

( )

A estimate m2 =

Ffeed N m3 s1

Q av (GPU)7.501 1012P (Pa)

(13)

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M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

Q av (GPU) =

Table 3
Membrane areas used for the simulation of 10 different membrane congurations.

i =n 1 Q ixi, feed
C
i =n 1 Q i

(14)

Hence, for the conditions in these example calculations the

estimated area required is approximately 5.548  106 m2 based on
Eq. (12) or 1.123  107 m2 based on Eqs. (13) and (14). Based on the
bre geometry the number of bres required can then be simply
calculated. As mentioned above these are crude estimates and the
exact membrane area and/or pressure values should be chosen
following simulation and optimisation using the modelling
methodology presented here. However, these crude estimates are
useful as a starting point for such simulation and optimisation
studies.
For simulation purposes these two areas (calculated by either
Eq. (12) or Eqs. (13) and (14)) are used for the 1st membrane
connected to the feed. Each subsequent downstream membrane is
arbitrarily given an area 90% smaller than the preceding upstream
membrane (to reect the fact downstream membranes will typically have feed ow rates smaller than those fed to the connected
upstream membranes). Hence, two cases have been considered
using the different membrane areas for the simulation of the different congurations as shown in Table 3. A small membranes
case based on areas calculated with Eq. (12) and a large membranes case based on areas calculated with Eqs. (13) and (14).
Considering the two different sets of membrane areas, each of
s
the ten congurations were simulated within MatLab using an
s
Intel i5 3.40 GHz desktop computer with 8 Gb of memory following the strategies given in the methodology section. In particular the following 6 simulation strategies are tested:
A. Sequential Direct substitution
B. Sequential Wegstein
C. Sequential NewtonRaphson
D. Sequential Broyden
E. Simultaneous Sequential initialisation
F. Simultaneous Simple initialisation
For congurations 14 where there are no recycle streams and
so simulation strategies AE operate in exactly the same manner
giving identical CPU times (strategies AE vary only when there
are recycle streams present). The simultaneous solution step in
strategy E is not needed if there are no recycle streams present and
in such situations the system is solved using only the sequential
initialisation. The remaining 6 congurations include recycle
streams and these are simulated using strategies AF until they
converge to a steady-state which satises the mass balances inside
all membranes, as well as all connections and recycles.
In all strategies the single-stage membrane simulations are
carried out using damping together with initialisation using option
3 from Section 2.2. Inside each single-stage membrane simulation
damp is initially set equal to 0.1 and later changed to 1 when the
method reaches a certain convergence criteria (norm (Z) divided
by the number of unknown variables o0.1; where the norm of a
vector B is dened as norm(B)(B12 B22 .)1/2). Complete
convergence is assumed for single-stage membranes when this
value becomes smaller than 1  10  6.
As mentioned in Section 2.3.1 the details of strategies AD can
be found in the literature [19]. For these calculations in the Wegstein method used in strategy B the acceleration parameter is
constrained between  5 and 0.
Strategy E is implemented using single-stage membrane simulations together with damping as described above for the sequential initialisation. Additionally, the multi-stage Newton
Raphson method is implemented in this strategy without damping
(damp 1) and including all connection/recycle terms inside the

Area (m2)

Memb
Memb
Memb
Memb
Memb

1
2
3
4
5

small membranes case (m2)

large membranes case (m2)

5.548  106
5.548  105
5.548  105
5.548  104
5.548  104

1.123  107
1.123  106
1.123  106
1.123  105
1.123  105

Jacobian. This is found to be a stable strategy because the sequential initialisation provides a good initialisation.
Alternatively, strategy F uses only a simple initialisation of the
recycle streams which is a relatively poor initial starting point.
Hence this strategy is implemented initially using damping in the
multi-stage NewtonRaphson method and excluding the connection/recycle terms from the Jacobian. As with the single-stage
damping damp is initially set equal to 0.1 and later changed to
1 when the method reaches a certain convergence criteria (norm
(Z*) divided by the number of unknown variables o0.1). After
meeting this criterion the connection/recycle terms are also reinserted into the Jacobian to accelerate convergence. Complete
convergence for the multi-stage simulations (in strategies E and F)
is assumed when norm (Z*) divided by the total number of unknowns in all membranes is less than 1  10  6.
The above strategies (AF) were found to be stable converging
to the same physical solutions for each of the ten congurations.
However, it is worth noting that there are a number of alternatives
strategies which are less stable. In particular it was found that:
Strategy D using a unity matrix as an initial Jacobian (a common practise when using the Broyden method) leads to convergence problems and hence the implementation used here involves the calculation of a Jacobian for the rst step using a numerical difference method.
All strategies using single-membrane NewtonRaphson method failed without damping (i.e. if damp 1 starting from the initial
point).
Also, the multi-stage NewtonRaphson method used in strategy F failed to converge for all cases without damping and for
some cases if the connection/recycle terms in the Jacobian are
included from the start.
Example simulation results are given for conguration 9 in
Fig. 11. These example results show that with this conguration a
very high purity of CO2 is achieved with a ow rate of approximately 10% of the feed.
The resulting CPU times required by each strategy for each of
the 10 congurations are shown in Figs. 12 and 13 for the sequential and simultaneous strategies using the small membranes
case and in Figs. 14 and 15 for the sequential and simultaneous
strategies using the large membranes case. It is clear from these
gures that while the sequential strategies are shown to be fast for
congurations 14 which do not contain any recycles they are an
order of magnitude slower than the simultaneous strategies for
congurations 510.
Considering the different sequential strategies the Wegstein
and Broyden methods are shown to give the best computational
efciencies for these cases. The NewtonRaphson method is slow
here mainly because of the computational effort required for the
calculation of the Jacobian derivatives using numerical differences
which increases the computational effort required, in particular for
cases with multiple recycles. The direct substitution method is also
shown to be relatively slow, due to the large number of iterations
required.
The two simultaneous methods are shown to give relatively

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

F
x CO
x CH

47

0.9989

0.0011

x C2 H =
6
xC H =
3

Nm s

469

-1

F
x CO

0.0000

x CH

0.0000

x C2 H

100

P2

kPa

xC

0.9711

x CH

0.0245

0.0040

3H 8

0.0003

100

=
=

0.0322

0.0052

3H 8

0.0005

400

-1

kPa

-1
400

x C2 H
xC

Nm s

190

Nm s

0.9621

F
x CO

143

kPa

R2
Membrane 2

P1

kPa

400

0.9536

x CH

0.0394

x C2 H

kPa

P3

xC

R1

x CH

500

0.4850

Nm s

0.2790

0.1626

3H 8

0.0734

400

x C2 H
xC

Nm s

0.0065

3H 8

0.0006

100

-1

kPa

Membrane 3

Feed

F
x CO

14

P
Membrane 1

F
x CO

F
x CO

-1

x CH

Nm s

467

-1

F
x CO

2
4

0.4472

x CH

0.2998

x C2 H

x C2 H =
6
xC H =
3

kPa

R3

0.1743

xC

0.0786
400

453

0.4318

Nm s

0.3078

0.1794

3H 8

0.0810

400

kPa

-1

kPa

Fig. 11. Sample calculation results based on conguration 9 shown in Fig. 10.

104

35
Simultaneous - Sequential initialisation
Simultaneous - Simple initialisation

CPU time (seconds)

30

CPU time (seconds)

103

102
Sequential - Direct substitution

20

15

10

Sequential - Wegstein
Sequential - Newton-Raphson

101

100

25

Sequential - Broyden

5
6
7
Membrane configuration

10

Fig. 13. Comparison of CPU times required for the simulation of 10 different congurations the small membranes using different simultaneous strategies.
1

5
6
7
Membrane configuration

10

Fig. 12. Comparison of CPU times required for the simulation of 10 different congurations the small membranes using different sequential strategies.

fast convergence for all 10 congurations and for both of the different membrane area cases (large and small). However, it is
shown that the strategy with sequential initialisation method is
faster for most of the congurations with the exception of conguration 6. It is presumed that the simple initialisation approach
is faster only for this conguration because conguration 6 has a
very small recycle ow rate compared to the other congurations.
Hence, the simple initialisation which uses a starting point with
zero ow rate is a good initial point for this conguration (under
the operating conditions used here).
For all other congurations the sequential initialisation approach is shown to give slightly faster convergence for the small
membranes case. Considering the large membranes case (excluding conguration 6) the sequential initialisation is shown to

give signicantly faster convergence for congurations which include one or more recycle streams. Hence, the simultaneous
strategy with sequential initialisation is considered to be the most
computationally efcient approach for use in the design and optimisation of complex multi-stage membrane systems.

5. Discussion and conclusions

A modelling framework including equations necessary to simulate membrane separations is presented here based on expressions taken from the existing literature. However, the existing
literature typically does not include details of the strategies employed for the solution of such membrane systems and in particular strategies for the solution of multi-stage membrane systems
have only been considered by a small number of different authors.
Hence, in this article six different strategies are considered for
the solution of multi-stage membrane systems. In the simpler

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M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

10 4

CPU time (seconds)

10 3

10 2
Sequential - Direct substitution
Sequential - Wegstein
Sequential - Newton-Raphson
Sequential - Broyden

10 1

10 0

10

Membrane configuration
Fig. 14. Comparison of CPU times required for the simulation of 10 different congurations the large membranes using different sequential strategies.

55
50
Simultaneous - Sequential initialisation
Simultaneous - Simple initialisation

45

CPU time (seconds)

40
35
30
25
20

modications in the simultaneous solution step as the sequential

initialisation provides a good initialisation. Alternatively, a second
strategy (strategy F: Simultaneous simple initialisation) is also
considered in which sequential initialisation is bypassed and the
simultaneous method is implemented starting from a relatively
poor initial point. Hence, this strategy requires stability enhancing
modications (damping and excluding connection/recycle terms
from the Jacobian of the multi-stage NewtonRaphson method
employed) which allow the strategy to converge but also slow
down the rate of convergence. In the set of example calculations
performed it was found that strategy E required lower CPU times
for nine out of the ten membrane congurations tested. Strategy F
was found to be faster only for the conguration and conditions
where there is a relatively small recycle ow rate in which case the
simple initialisation gives a better starting point.
For these reasons (fast and stable solution strategy) it is recommended that the simultaneous strategy with sequential initialisation should be used for simulation and optimisation of
multi-stage membrane systems. This strategy and modelling framework can be extended to any number of membranes with any
number of physically feasible complex connections and recycles.
Due to the shorter simulation time optimisation (which may require thousands of simulations carried out at different conditions)
also becomes substantially quicker and should give results within
a shorter timeframe.
This simultaneous strategy is also important when considering
the simulation of membranes connected to chemical or biochemical reactors, distillation columns, condensers and various
other pieces of equipment that need to be simulated at a gas
processing plant (or renery or petrochemical plant). If the model
equations are available for those other units then the same simultaneous strategy with sequential initialisation can be extended
to include all the process units. Alternatively, the membrane network can be simulated in sequence with the other processes
which may be simpler to implement (but potentially requiring
more computational effort to converge).

15
10
5

Acknowledgements
1

5
6
Membrane configuration

10

Fig. 15. Comparison of CPU times required for the simulation of 10 different congurations the large membranes using different simultaneous strategies.

sequential strategies any existing modelling methodology for the

solution of single-stage membranes can be implemented repeatedly until an overall converged solution is obtained. However,
it is shown in this study that while these strategies can obtain
feasible solutions, they may require a large computational effort
(e.g. using large numbers of iterations). Four different sequential
strategies are considered and it is found that among these sequential strategies the Wegstein and Broyden methods gave the
best performance (lowest CPU times) for the set of example calculations tested.
The more complex simultaneous strategies are shown to give
much faster (approximately 10 times faster) convergence than
sequential strategies for the simulation of multi-stage membrane
congurations containing recycles. Two different simultaneous
strategies are considered here which vary according to the way
they are initialised and the stability enhancing modications
which are implemented. The strategy (strategy E: Simultaneous
sequential initialisation) giving the best overall performance involves the sequential initialisation of individual membranes followed by the simultaneous solution of all membranes, connections
and recycles. This strategy does not require any stability enhancing

This work was supported by the Korea CCS R&D Center (KCRC)
grant funded by the Korea government (Ministry of Science, ICT &
Future Planning) (No.2014M1A8A1049338)

Nomenclature
Am

membrane effective surface area between two adjacent tanks (m2)

Cn
number of components (dimensionless)
d and dinner inner diameter of the hollow bre (m)
douter
outer diameter of the hollow bre (m)
damp
damping parameter (dimensionless)
F
total volumetric ow rate to adjacent tank on the
same side of the membrane (N m3 s  1)
F
set of functions including Eqs. (7)(11) (for all
membrane tanks)
J
Volumetric ow rate across the membrane
(N m3 s  1)
L
Effective length of the hollow bre (m)
Nm
number of membrane stages (dimensionless)
nbre
number of hollow bre tubes (dimensionless)
P
pressure (Pa)
Qi
permeance of component i (N m3 m  2 s  1 Pa  1)

M. Binns et al. / Journal of Membrane Science 497 (2016) 458471

S
t
T
V
xi
yi
Z

number of tanks used for modelling the retentate/

permeate (dimensionless)
time (s  1)
temperature (K)
volume of the retentate/permeate (m3)
retentate mole fraction of component i
(dimensionless)
permeate mole fraction of component i
(dimensionless)
set of unknown variables (x, y, Fr, Fp, Pp) (various
units)

Greek characters

n
Pn

dynamic viscosity of the gas mixture in the nth

tank of the permeate (Pa s)
Change in pressure between tanks n 1 and n (Pa)

Subscripts
i
j
n
p
r
feed
total
outlet

ith component
jth permeate tank
nth retentate tank
permeate
retentate
membrane feed (in the retentate)
total gas ow (considering all the membrane bres
combined)
membrane outlet (in the permeate)

[4]

[5]

[6]

[7]

[8]
[9]

[10]

[11]
[12]

[13]

[14]

[15]

[16]
[17]

References

[18]
[19]

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AIChE J. 32 (1986) 20202027.
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C: The Art of Scientic Computing, second ed., Cambridge University Press,
New York, 1992.
[3] M.H.M. Chowdhury, X.S. Feng, P. Douglas, A new numerical approach for a

[20]
[21]

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