World Academy of Science, Engineering and Technology
International Journal of Chemical and Molecular Engineering
Modeling and Parametric Study for CO2/CH4
Vol:4, No:12, 2010
Separation using Membrane Processes
Faizan Ahmad, Lau Kok Keong, Azmi Mohd. Shariff
Abstract—The upgrading of low quality crude natural gas (NG)
is attracting interest due to high demand of pipeline-grade gas in
recent years. Membrane processes are commercially proven
technology for the removal of impurities like carbon dioxide from
NG. In this work, cross flow mathematical model has been
suggested to be incorporated with ASPEN HYSYS as a user
defined unit operation in order to design the membrane system for
CO2/CH4 separation. The effect of operating conditions (such as
feed composition and pressure) and membrane selectivity on the
design parameters (methane recovery and total membrane area
required for the separation) has been studied for different design
configurations. These configurations include single stage (with and
International Science Index, Chemical and Molecular Engineering Vol:4, No:12, 2010 waset.org/Publication/9428
without recycle) and double stage membrane systems (with and
without permeate or retentate recycle). It is shown that methane
recovery can be improved by recycling permeate or retentate stream
as well as by using double stage membrane systems. The ASPEN
HYSYS user defined unit operation proposed in the study has
potential to be applied for complex membrane system design and
optimization.
Keywords—CO2/CH4 Separation, Membrane Process,
Membrane modeling, Natural Gas Processing
I. INTRODUCTION
M ETHANE is the major component (75%-90%) of
natural gas but it may also contain significant amounts
of ethane, propane, butane and traces of higher hydrocarbons
depending upon the source [1]. In some deposits, it may have
contaminants such as CO2, H2S, CO which constitutes
environmental hazards and also causes hindrance in natural
gas processing. The upgrading of low quality crude natural
gas is attracting interest due to the high demand for pipeline-
grade gas in recent years. CO2 must be removed in order to
serve the following purposes; increase the heating value of
the gas, prevent corrosion of pipeline and process
equipments and crystallization during liquefaction process
[2, 3].
CO2 contents can vary from 4% to 50% in NG depending
upon the gas source. It needs to be pre-processed before the
transportation to meet the typical pipeline specification of
2%-5% CO2 [4]. Most of the NG, produced in the lower 48
states of USA, contains more than 5% CO2.As a result, many
natural gas wells are unexploited due to their low production
rate and low quality (i.e., high CO2 and/or H2S content) [5].
Faizan Ahmad is with the Chemical Engineering Department, Universiti
Teknologi PETRONAS, Bandar Sri Iskandar, 31750 Tronoh, Perak
Malaysia. (Ph. No: 0060-13-4056022: e-mail: faizan615@gmail.com).
Lau Kok Keong is with the Chemical Engineering Department,
Universiti Teknologi PETRONAS, Bandar Sri Iskandar, 31750 Tronoh,
Perak Malaysia. (e-mail: laukokkeong@petronas.com.my).
Azmi Mohd. Shariff is with the Chemical Engineering Department,
Universiti Teknologi PETRONAS, Bandar Sri Iskandar, 31750 Tronoh,
Perak Malaysia. (e-mail: azmish@petronas.com.my).
International Scholarly and Scientific Research & Innovation 4(12) 2010
In Malaysia, NG from Tangga Barat Cluster fields of
PETRONAS contains relatively high amount of CO2 [6].
Therefore, it is necessary to develop efficient processes for
the removal of CO2 from NG [5, 6].
There are different processes for the removal of CO2
considering the factors of; capital and operating costs, gas
specifications and environmental concerns. The major
processes can be grouped as absorption Processes (chemical
and physical absorption), adsorption processes (solid
surface), hybrid solution (mixed physical and chemical
solvent) and Physical Separations (membrane and cryogenic
Separation) [7, 8, 9].
For natural gas processing applications, membranes
processes are commercially proven technology. For a gas to
permeate through a membrane surface, the gas must first
dissolve in the high-pressure side of the membrane, diffuse
across the membrane wall, and evaporate from the low-
pressure side. The working principle of gas separation is
therefore that some gases are more soluble in, and pass more
easily through polymeric membrane than other gases [7, 10,
11].
In membrane process, feed gas is pretreated before
entering the membrane system in order to ensure efficient
operation. It mainly controls the fouling, plasticization and
condensation of hydrocarbons in the membranes [1, 11].
Moreover, the temperature control system is provided to
maintain the gas at the desired operating temperature of the
membrane fibers. Finally, the heated gas is entered into the
membrane gas separators where it gets separated into two
streams; the permeate, a low pressure CO2 stream and the
non-permeate or residue, a high pressure hydrocarbon rich
stream [7].
Gas separation by membrane technology has become a
major industrial application only during the last few decades
but the study of gas separation has a long history [10].
Graham measured the permeation rates of all the known
gases of that time using different diaphragms [10, 12]. Barer,
Amerongen and Stern played an important role in the
development of solution diffusion model for the explanation
of gas permeation [13, 14, 15]. The success of Monsanto, the
first membrane company, encouraged other companies like
Cvnaoi, Separex and Grace Membrane Systems to produce
membrane plants for removal of CO2 from natural gas [10,
16].
Datta and Sen worked on the optimization of the gas
processing cost for a membrane unit. It is shown that the
optimum configuration might be unique within certain
ranges of CO2 concentration and the minimum gas
processing cost could only be achieved by adjusting the
number of modules in each stage and the compressor power
[4].
766 scholar.waset.org/1307-6892/9428
 World Academy of Science, Engineering and Technology
International Journal of Chemical and Molecular Engineering
Lee et al. investigated the effects of the operating variables 3. It represents the
Vol:4, No:12, 2010 whole membrane module and will
of pressure, feed flow rate, and the carbon dioxide not involve the details inside the module.
concentration in the feed. Additionally, computer models 4. Pressure drop on both sides of the membrane is
were applied for the separation of gases under perfect mixing negligible.
and cross flow conditions to the analysis of the field data [5]. 5. The concentration polarization is assumed to be
Wang enhanced operational flexibility and adaptability of negligible.
membrane process using an optimal method in which auto-
controlling of the permeate gas flux was applied for the first yp
Vp
time [17].
Qi and Hensen presented the optimal design strategy for
spiral membrane networks for gas separations [18] whereas Pl yn
Lababidi developed the mathematical model to optimize Xf
three configurations including single stage, two stages, and X0
the continuous membrane column (CMC) [19]. Lf Ph x x-dx
The permeability and selectivity variations of the CO2/CH4 Lr
system have been studied by Safari, Ghanizadeh and Rehmat
that included both temperature and pressure effects dAm
simultaneously [20]. Hau et al. studied process design, Fig. 1 Schematic diagram of cross flow membrane
economics, and sensitivity of membrane stage with recycle separation
streams [21].
International Science Index, Chemical and Molecular Engineering Vol:4, No:12, 2010 waset.org/Publication/9428

There are limited studies on the design of membrane The local permeation rate at any point in the stage over a
system using commercial process simulator. The advantages differential membrane area dAm is
of using commercial simulator involve the accurate modeling
PA
of thermodynamics properties and auxiliary equipment in the ydV p x py (1)
membrane system. In this paper, different design parameters
are analyzed for membrane gas separation under different PB
ydV p 1 x p 1 y (2)
configurations using ASPEN HYSYS. As membrane unit is
not a pre-defined unit operation in ASPEN HYSYS, a cross
flow model is proposed to predict the membrane Dividing eq (i) by eq (ii), we get
performance in the removal of CO2 from natural gas. Finally,
α
the proposed model is included in the process simulation as (3)
user defined unit operation along with other available unit
operations to design the membrane system.
Using ingenious transformations, an analytical solution to the
II. METHODOLODY three equations (eq. (i) - eq. (iii)) have been obtained [10].

A. Governing equations E
U
D R U α F S U F T
The study is based on the cross flow model derived by E (4)
U U α F U F
D
Weller and Steiner [22] as shown in the detailed flow
diagram (Fig. 1). The nomenclature of the flow sheet is as Where
follows:
dV= dL=Total flow rate permeating through the area 1 L/Lf (L as flow rate permeated in the differential
xf = Feed mole fraction element)
x0 = Retentate mole fraction
yn = Permeate mole fraction i
Lf = Feed flow rate
Lr = Retentate flow rate .
u Di i 2Ei F
Vn = Permeate flow rate
ph = Pressure on the high pressure side
1 α
pl = Pressure on the low pressure side D 0.5 α

The model assumes no mixing in the permeate side as well

E = α/2)-DF
as on the high pressure side. Thus the composition of
permeate can be determined at any point along the
1 α
membrane by the relative permeation rates of feed F 0.5 1
component at that point [23].
The assumptions that follow the suggested model are:
R = 1/ (2D 1)
1. It holds for the binary gas mixture
2. Permeability is independent of pressure and
α D 1 F
temperature of the gas stream. S α
2D 1 F
2

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 World Academy of Science, Engineering and Technology
International Journal of Chemical and Molecular Engineering
Vol:4, No:12, 2010 III. RESULTS AND DISCUSSIONS
1
T A. Model Validation
E A mathematical model is validated with the published
1 D
F
experimental data for membrane separation process. The data
The term uf is the value of u at i = if = xf / (1-xf). The value by Pan et al. [27] is based on the experiments done on sour
of is the fraction permeated up to the value of x. At the natural gas. The feed gas contains 48.5 % CO2 that is
outlet where x=x0, the value of becomes equal to i.e., removed in the permeate stream, with the purpose to increase
the total fraction permeated. The composition of the the recovery of methane in the retentate stream. The
permeate stream is yp and thus can be calculated from the temperature and pressure of the gas are 10oC and 35.28 bar
overall material balance. respectively whereas, on the other hand, the permeate
pressure is 9.28 bar. The selectivity is assumed to be 25.
Table 1 shows that the suggested model gives good
(5)
approximation to the experimental data with maximum
percentage error < 17.8%.
The total membrane area is then calculated using additional The proposed model is further validated with the data from
transformations of eqs. (i)-(v) in order to obtain Liu et al [28] based on the study conducted on propylene
enrichment using cross flow membrane. Table 2 show that
L
the simulated data are in close agreement with the
experimental data with maximum percentage error < 5 % . It
International Science Index, Chemical and Molecular Engineering Vol:4, No:12, 2010 waset.org/Publication/9428

can also be observed that the simulated model gives better

approximation with experimental data from Liu et al. as
Where
compared to experimental data from Pan et al. [28]. The
fi = (Di – F) + (D2i2 + 2Ei + F2)0.5 small error in the comparison can be attributed to the
sensitivity of membrane permeability towards high pressure,
The term if is the value of i at the feed and i0 is the value of i which is assumed negligible in the suggested mathematical
at the outlet. The integral is solved numerically to calculate model.
the value of total membrane area required for the separation.
TABLE I
B. Design Configurations VALIDATION OF MATHEMATICAL MODEL WITH EXPERIMENTAL
The design of a membrane separation process involves (i) DATA BY PAN et al
the configuration of permeators (ii) the operating parameters Stage Cut Permeate mole fraction, CO2
of the individual permeators [18]. Different configurations ( ) Simulated Experimental % Error
have been proposed for the membrane separation as shown
in Fig. 2. For moderate purity and recovery requirement, 0.40 0.91 0.96 5.49
single stage system (with and without recycle) is appropriate 0.42 0.88 0.95 7.95
[24]. For more demanding separations, multiple stage system 0.45 0.83 0.94 13.25
is required [25, 26]. It is a conventional approach to select
different configurations and then optimize the operating 0.47 0.81 0.93 14.8
permeation [19]. 0.50 0.78 0.91 16.6
0.52 0.75 0.89 18.6
0.55 0.73 0.86 17.8

TABLE I I
VALIDATION OF MATHEMATICAL MODEL WITH EXPERIMENTAL
DATA BY LIU et al.
Stage Cut Mole fraction of Species in permeate
( ) Simulated Experimental % Error

0.01 0.80 0.76  5.00

0.02 0.78 0.76  2.56
0.03 0.77 0.76  1.29
0.04 0.78 0.75  3.8

Fig. 2 Design configurations for CH4/CO2 separations: (a) single

stage (b) Single stage with recycle (c) two stage (d) Two stage with B. Parametric analysis:
permeate recycle (e) Two stage with retentate recycle. The methane recovery and total membrane area are
considered as the main parameters for membrane system
design. The effects of feed composition, feed pressure and

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 World Academy of Science, Engineering and Technology
International Journal of Chemical and Molecular Engineering
thee selectivity of
o the membraane were studied on the meethane reten
Vol:4, No:12, ntate stream in
2010 i double
stagge configurattion can leadd to
reccovery for different
d conffigurations ussing the sugggested largee requirementss of area, whhile in single stage,
s recycling
crooss-flow moddel. has not
n much effeect. These ressults are consiistent with thoose
obtaiined by Qi et al
a [18].
ffect of feed coomposition:
Eff
Methane recovery decreaases with thee increase in CO2 Effecct of feed presssure:
coontents of thhe feed [18]. At the sam me time, meethane Thhe increase in feed pressuree improves methane
m recovery
reccovery can be b improved by recyclingg the permeaate or [11, 18]. It is duee to the fact thhat the increm
ment of pressuure
reccycle stream as well as ussing double sttage configuraations creattes a greater driving forcee across the membrane.
m As a
[24, 29, 30]. resullt, a net increease in permeeation through h the membraane
The effect of
o feed compoosition on meethane recoverry for increeases methanee recovery undder present sellectivity.
alll proposed coonfigurations,, for the stagge cut of 0.55 and Figg. 4(a) showss the effect oof feed pressure on methaane
selectivity of 25, is shown in i Fig. 3 (a). The feed preessure recov very for diffferent configuurations. Thee stage cut and a
annd permeate pressure are maintained at a 100 and 4 bar selecctivity is samee as in previouus case, wherreas the feed gas
g
resspectively. The
T permeability of CH4 is considereed as contaains 20% CO O2 and 80% CH4. The increasei in feeed
1.44×10-3 mol/M MPa-m2-s. presssure increases the methane recovery, esp pecially when the
It can be obsserved that thhe methane reecovery is redducing presssure is less thhan 70 bar. Baased on the figure, the douuble
wiith the increaase of CO2 in the feed gas. The syystems stagee configuratioons with reccycles stream m give the hiigh
wiithout recycle, as expectted, provide the lowest CH4 recov very followedd by double staage without reecycle. Similaarly
International Science Index, Chemical and Molecular Engineering Vol:4, No:12, 2010 waset.org/Publication/9428

reccovery. It is obvious
o as thee portion of first
f stage perm
meate singlle stage withh recycle strream is obseerved with high
thaat is lost is taaken from thee first membraane module, where
w meth hane recoveryy, though leess than thee double staage
feeed CO2, hencce permeate CO2 C is highestt and hydrocaarbons confi
figurations, in comparison to single stagee without recyycle
aree lowest. Bessides, the simuulated results also show thhat the streaam.
ussage of two sttage system couldc minimizze the reductiion of
CHH4 recovery under
u high COO2 feed compoosition.

Fig. 4(a) Effect

E of feed presssure on methane recovery

Fig. 3 (a) Effect

E of feed com
mposition on meethane recovery

Fig.. 4 (b) Efffect of feed presssure on total mem

mbrane area

Fig. 3(b) Effeect of feed compposition on totaal membrane arrea Onn the other hand,
h an increase in feed pressure wouuld
decreease the total membrane aarea required for the effecttive
Thhe total membbrane area requuired for the effective
e separration separration as showwn in the figg. 4(b). It is obvious as hiigh
inccreases with the
t increase in i CO2 compposition of thee feed presssure leads to high rate oof permeation n which direcctly
unntil its maximu
mum point reacches. After thhat, further inccrease reducce the membrane area requiired for the seeparation.
caan lead to deccrease in the membrane arrea requiremeent as
shhown in fig. 3((b). It can also be observedd that recyclinng the

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 World Academy of Science, Engineering and Technology
International Journal of Chemical and Molecular Engineering
Eff
ffect of membrrane selectivity
ty: conte
Vol:4, No:12, ents in the feed
2010 f has
highh influence ono the methaane
Membrane properties
p havve high influuence on meethane recovvery as well as membranne area. The increased feeed
reccovery. Methhane recoveryy increases with the increaase in presssure and use of highly selective memb branes cans also
a
selectivity of thhe membrane [18]. It is duee to the reasonn that lead to the imprroved methanne recovery. Moreover, the
inccreased selecctivity leads tot higher perrmeation andd thus memmbrane area reequired for thhe effective seeparation can be
im
mproved methaane recovery. decreeased by increeasing the feedd pressure or selectivity of the
Fig. 5(a) shows the effect of membranee selectivity on o the memmbrane, especiially for low ccomposition of o CO2 in natuural
meethane recovvery for fivee proposed configurations
c s. As gas. The ASPEN N HYSYS uuser defined membrane unit u
exxpected, the inncrease in seleectivity increaases CH4 recoovery, operaation proposeed under preesent study potentially to be
esppecially for the double stage
s configuurations and single
s appliied for com mplex membbrane system m design and a
staage with recyycle stream. It can also be noted thaat the optim
mization.
inccrement in seelectivity for the
t single stagge configuration is
ACKNOWLEEDGMENT
lesss significant on the methanne recovery.
Thhis work wass done with the financiaal support from
Univ
versiti Teknoloogi PETRONA
AS.

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International Journal of Chemical and Molecular Engineering
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