Journal of Natural Gas Science and Engineering 67 (2019) 172–195

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Journal of Natural Gas Science and Engineering

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

Review Article

Membrane-based carbon capture technologies: Membrane gas separation vs. T

membrane contactor
Utjok W.R. Siagiana, Anggit Raksajatib, Nurul F. Himmac, K. Khoiruddinb, I.G. Wentenb,d,∗
a
Department of Petroleum Engineering, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, 40132, Indonesia
b
Department of Chemical Engineering, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, 40132, Indonesia
c
Department of Chemical Engineering, Universitas Brawijaya, Jl. Mayjen Haryono 167, Malang, 65145, Indonesia
d
Research Center for Nanosciences and Nanotechnology, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, 40132, Indonesia

A R T I C LE I N FO A B S T R A C T

Keywords: In this paper, the recent development of membrane-based carbon capture technologies is reviewed, including
Energy membrane gas separation (MGS) and membrane contactor (MC). The state of the art of both technologies and
Flue gas recent development of membrane materials are discussed. The main challenges such as plasticization and
Gas absorption physical aging in MGS, and wetting phenomena in MC are then discussed, followed by attractive attempts to
Gas separation
suppress them. In addition, both technologies are compared in terms of their characteristics, carbon capture
Natural gas
performances, and techno-economic assessment. Finally, prospects and challenges of membrane-based carbon
capture technology, especially at very high CO2 concentration are pointed out.

1. Introduction patents) on absorption, 21.9% (350 patents) on adsorption, 7.8% (2749

The capture of carbon dioxide (CO2) from gaseous streams has
gained a great interest and becomes an important process in many in-
dustrial areas. Concerning global warming and climate change, carbon
capture is considered as an attractive and efficient solution to mitigate
the CO2 emission from combustion of fossil fuels (Ratnakar et al., 2018;
Venkatraman et al., 2017). In this regard, CO2 can be captured using
the following technological pathways: post- or pre-combustion capture
and oxy-combustion (Figueroa et al., 2008; Gibbins et al., 2008; Johns
and Dindoruk, 2013; Pires et al., 2011; Ratnakar et al., 2018; Yuan
et al., 2005). Meanwhile, in natural gas processing, CO2 (and other acid
gases) needs to be separated to meet the specifications required by the
buyers (for example pipeline transmission and distribution companies).
By separating CO2 from natural gas, the calorific value of natural gas
increases, the volume of the transported gas decreases, and its corrosive
tendency decreases. Another emerging application of CO2 removal is
biogas purification to produce biomethane. These needs have en-
couraged the continuous development of carbon capture methods.
Common technologies for CO2 capture are solvent absorption, solid
adsorption, and membrane-based separation (Darabkhani et al., 2018;
Hemmati et al., 2019a, 2019b; Lee et al., 2019; Pellegrini et al., 2019;
Wenten et al., 2017). It has been reported that up to 2017 there were
35,434 patents on CO2 capture technologies consisting of approxi-
mately 32.4% (11,463 patents) on chemical separation, 29.8% (10,550
patents) on membrane system, 6.3% (2242 patents) on rectification-
condensation, and 1.9% (687 patents) on biological separation (Luis
Míguez et al., 2018). The fewer patents on membrane systems were
likely due to the relatively fewer materials that have been investigated
and developed for CO2 capture. Solvent-based CO2 capture is currently
the well-established technology and the most promising methods in the
near future due to the high selectivity, -high capacity, and simplicity in
the regeneration of solvents (Aaron and Tsouris, 2005; Wang et al.,
2011a). However, the solvent absorption has also major drawbacks,
including high energy required for solvent regeneration and operational
problems such as flooding which limits the capacity of the absorption
column (Ahmad et al., 2010; Mansourizadeh and Ismail, 2009). This
opens opportunities for emerging alternatives technologies, such as
membrane, to be applied in CO2 capture and natural gas processing
fields in the longer term because of the potential to overcome the
limitations of current technology (Roussanaly et al., 2016).
Membrane technologies have been applied in various processes and
industrial sectors replacing conventional technologies due to their in-
teresting features (Bernardo and Drioli, 2010; Drioli et al., 2011, 2003;
Himma et al., 2018, 2019; Makertiharta et al., 2017; Purwasasmita
et al., 2015a; Van der Bruggen et al., 2004; Wardani et al., 2017;
Wenten et al., 2018). In the case of CO2 separation from natural gas and
flue gas, the main advantages of membrane-based technologies are low
cost, low energy requirement, flexible operation, and modularity.

∗
Corresponding author. Department of Chemical Engineering, Institut Teknologi Bandung, Jl. Ganesha 10, Bandung, 40132, Indonesia.
E-mail address: igw@che.itb.ac.id (I.G. Wenten).

https://doi.org/10.1016/j.jngse.2019.04.008
Received 30 January 2019; Received in revised form 16 March 2019; Accepted 9 April 2019
Available online 13 April 2019
1875-5100/ © 2019 Elsevier B.V. All rights reserved.
U.W.R. Siagian, et al.
Fig. 1. Number of annual publications related to membrane gas separation and
membrane contactor for CO2 capture and separation the past 20 years. Source:
Scopus (TITLE-ABS-KEY (terms); terms: membrane gas separation CO2, mem-
brane contactor CO2 + membrane gas absorption CO2; January 10th, 2019).
Selective membranes for CO2 capture have been widely developed and
applied since the 1970s. The application of gas separation using
membranes has been rapidly growing. This is indicated by the nu-
merous works on membrane gas separation (MGS) for CO2 which have
been published during the last two decades (Fig. 1). MGS has been
widely investigated for CO2/CH4 separation from natural gas (Adewole
et al., 2013; Scholes et al., 2012; Yeo et al., 2012). MGS could also be
applied for post-combustion capture (CO2/N2 or CO2/N2/O2 separation
from flue gases (Aaron and Tsouris, 2005; Powell and Qiao, 2006)) and
pre-combustion capture (CO2/H2 separation after or in water-gas shift-
membrane reactor unit (Scholes et al., 2010b)).
Although gas transport through membranes has been systematically
studied in more than a century, membrane fabrication technology was
significantly advanced along with the development of asymmetric
membrane in the 1970s (Baker, 2004). Afterward, notable milestones in
the industrial application of MGS, particularly for CO2 capture appli-
cation are reported (Bernardo and Clarizia, 2013). Even so, many im-
provements are still required to achieve high performance of gas se-
paration using membrane, i.e. producing a high CO2 rate, as well as
improving selectivity and durability of the membrane. There have been
efforts in the field of membrane development in order to achieve such
membrane improvements. One of the options of novel membrane-based
technologies is gas–liquid membrane contactor (MC) which combines
membrane with conventional phase contacting operation such as ab-
sorption, and hence the benefits of both technologies can be fully uti-
lized. In MC, a porous membrane is used to provide an extra area for
Fig. 2. Schematic of (a) membrane gas separation (MGS) and (b) membrane contactor (MC) for CO2 removal.
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Journal of Natural Gas Science and Engineering 67 (2019) 172–195
contact between the gas and liquid phases and to avoid the dispersion
between them (non-dispersive contact). Hollow fiber membrane mod-
ules are preferentially used since they give high specific surface area
(Gabelman and Hwang, 1999; Li and Chen, 2005; Mansourizadeh and
Ismail, 2009; Pabby and Sastre, 2013), i.e. up to 30 times higher than
the conventional contactor (Mansourizadeh and Ismail, 2009). In ad-
dition to the high surface area, the hybrid process offers other ad-
vantages, such as independent gas/liquid flow rates control without
causing flooding, modularity, and low cost (Drioli et al., 2005; Klaassen
et al., 2005). The interesting features of MC have attracted the in-
creasing attention from researchers for applying this process in CO2
removal (Fig. 1).
This article aims to present a summary and a comparative review of
membrane-based CO2 separation technologies. An overview of mem-
brane-based technologies for CO2 separation is first presented, followed
by a specific discussion on MGS and MC. With regard to MGS, the state-
of-the-art and challenges in MGS for CO2 removal are presented. To
date, all membranes used in commercial applications are polymeric
membranes mainly because of their ease of manufacture. Even though
in recent year various type of materials (including inorganic and
polymer-inorganic composite) have been developed as alternatives
demonstrating promising features under research conditions, such as
ceramic, glass, metals, zeolite, and carbon molecular sieve, but they
cannot compete commercially with the current polymeric membranes
because of the high module fabrication cost. Therefore, the review
presented in this paper also discusses the prospect and challenges of
various materials for CO2 removal. In addition, the current status and
development of MC for CO2 removal are discussed, in particular, the
development of superhydrophobic membrane as an attractive strategy
to prevent membrane wetting. Finally, the performances of MGS and
MC for carbon capture are compared and analyzed, and some per-
spectives are given.
2. Membrane gas separation (MGS)
Schematic illustrations of MGS and MC process for CO2 capture and
separation are shown in Fig. 2. The membrane for MGS can be classified
into three groups according to the mechanism of separation, namely:
simple sorption diffusion (i.e. selective surface diffusion, molecular
sieving, and solution-diffusion), complex sorption-diffusion (i.e. fa-
cilitated transport and palladium-based membrane for hydrogen), and
ion-conducting membranes (Koros and Mahajan, 2000). Among those
types, polymeric membranes with solution-diffusion mechanism have
been the most widely used (Koros and Fleming, 1993; Moradihamedani
et al., 2013; Robeson, 1999; Wang et al., 2013). In this mechanism, gas
molecules from the feed side are firstly absorbed by the membrane,
then they diffuse across the membrane matrix, and subsequently desorb
on the permeate side. Schematic of MGS process is illustrated in Fig. 2 a.
U.W.R. Siagian, et al.
A dense membrane is employed as a selective barrier between the feed
gas and the permeate gas stream. The selectivity of the membrane de-
pends on the solubility and diffusivity of the gas molecule in the
membrane matrix. The performance of MGS is generally measured as its
permeability and selectivity. To achieve the desired performance (high
permeability and selectivity), the type of membrane material should be
appropriately selected. Therefore, various types of membranes for MGS,
especially for CO2 removal, have been developed. More details on the
types of membranes are discussed in the following sub-section.
2.1. Membranes used in MGS
The performance and characteristics of gas separation using mem-
brane depend on several factors, such as the membrane material,
structure, thickness, and configuration (e.g. hollow fiber, flat sheet) as
well as the module/system design (Bernardo et al., 2009). Several
materials have been developed for CO2-capture membrane, including
organics, inorganics, and organic – inorganic composites, with their
own typical advantages and limitations.
Most commercial membranes for gas separation are currently
dominated by organic or polymeric membranes since they have some
attractive features, e.g. lower fabrication cost compared to inorganic
material, and easy to fabricate either into flat and hollow fiber module.
The polymeric membranes can be divided into rubbery state (kept
above its glass transition temperature and presents substantial free-
volume) and glassy state (kept below its glass transition temperature
and has low fractional free-volume) (Bernardo et al., 2009). Several
types of polymeric materials such as cellulose acetate, polyimide,
polysulfones, and perfluoropolymer, have been used for MGS. Among
these polymeric membranes, it has been reported that polyimide and
cellulose acetate are the most widely used in commercial scale. Fig. 3 a
and b shows some of the most important studies regarding the se-
lectivity and permeability performance of the polymeric membranes
used for gas separation (see Fig. 4).
Cellulose acetate was initially developed for reverse osmosis mem-
brane which is commercially applied in desalination. Cellulose acetate
is now the most widely used membrane material for CO2 removal from
natural gas. Commercial cellulose acetate membrane for gas sweetening
is manufactured by, for example, UOP (Separex), Natco (Cynara), and
Kvaerner (GMS) (Baker, 2002). This material is a glassy polymer that
has been widely known to have remarkable CO2/CH4 selectivity and
thus has been used as a standard in the existing industry (Baker and
Low, 2014). Cellulose acetate membranes normally have selectivity of
CO2/CH4 between 10 and 15 under normal operating conditions
(Baker, 2002). In addition, cellulose acetate is considered to be rela-
tively inexpensive as it uses cellulose as the raw material, which is an
abundant and renewable resource. One of the major drawbacks of
cellulose acetate is plasticization, which would decrease the membrane
permeability. This drawback is due to the high solubility of CO2 and
H2S in cellulose acetate (Bernardo and Drioli, 2010). This problem is
further discussed in Section 2.3 of this paper. Furthermore, cellulose
acetate membrane is also prone to acetylation, which is a hydroxyl
group substitution on glucoside repeating unit by acetyl group that
increases gas permeability with a decrease in selectivity (Scholes et al.,
2012). In order to address the limitations of this commercial type of
membrane, new various type of materials have been developed as the
alternative material for MGS.
The performance of several polymeric membranes has been pre-
viously summarized by Zhang et al. (2013a,b). The authors noted that
polyimide membranes are ideal for CO2/CH4 separation due to their
good selectivity of CO2/CH4 and also good chemical and thermal sta-
bility. Polyimide belongs to glassy state polymer with a free volume in
the range of 10–20% (Baker and Low, 2014). Cho and Park synthesized
2,6-diaminotriptycene-based polyimide membrane that has high in-
ternal free volume elements. In the case of CO2/CH4 and CO2/N2 se-
paration, the membrane showed both high permeability and selectivity,
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Journal of Natural Gas Science and Engineering 67 (2019) 172–195
surpassing the Robeson's upper bound (Cho and Park, 2011). Polyimide
membranes have been extensively studied and developed for gas se-
paration application (Zhang et al., 2013a,b). Polyimides with tri-
fluoromethyl (CF3) groups have drawn interest due to the good pure gas
selectivity and permeability and also the good solubility in many or-
ganic solvents (Baker and Low, 2014). The drawback of polyimide
membrane is the decrease of permeability and selectivity in practical
applications using mixed gas feed (compared to lab conditions) with
higher loss of performance than cellulose acetate, the most commonly
used polymeric membrane for gas separation (White, 2010). Further-
more, polyimide is also more susceptible to plasticization compared
with cellulose acetate.
Polysulfones have been discussed as the other commercial mem-
branes that have excellent mechanical properties, good thermal and
chemical stabilities, and are easy to process into a membrane (Sanders
et al., 2013). Compared with cellulose acetate, polysulfones have lower
CO2 permeability and CO2/CH4 selectivity, but higher plasticization
pressure (Julian and Wenten, 2012). An optimum polysulfone mem-
brane formulation reported in (Pesek and Koros, 1993) has been ex-
amined for CO2/CH4 and showed selectivity between 33 and 65
(Gordeyev et al., 2001; Gordeyev and Shilton, 2004; Ismail et al., 2003,
1999; Ismail and Lorna, 2003; Sharpe et al., 1999).
Another target of works devoted to MGS is to develop polymeric
membranes that could withstand a challenging environment (for ex-
ample high temperature operation). Perfluoropolymer membrane is one
of the polymeric membranes that suitable for such challenging condi-
tion, for example, raw natural gas treatment (Okamoto et al., 2016).
Perfluoropolymer membranes have strong C-F bonds, which result in
excellent chemical and thermo-oxidative stability. Poly(tetra-
fluoroethylene)/PTFE, which is considered to be the early generation of
perfluoropolymer, has been reported to have low permeability and low
processability due to the high crystallinity. However, during further
development of this membrane, amorphous glassy perfluoropolymer
membranes were introduced, such as Cytop©, Teflon AF©, and Hyflon
AD©, which have high gas permeability, and high solubility in per-
fluorinated solvents (thus good processability) (Arcella et al., 2003,
1999; Cui et al., 2014; Pinnau and Toy, 1996). Despite those ad-
vantages, perfluoropolymer has the relatively expensive raw material
and thus considered to have high fabrication cost (Scholes et al., 2012).
Recently, new classes of polymeric membranes have been developed
and tested for CO2 removal, i.e. thermally rearranged (TR) polymer and
polymers of intrinsic micro-porosity (PIM) membranes. As can be seen
in Fig. 3, these new types of membrane offer promising features for CO2
removal. TR membranes are glassy polymers, which are prepared by the
thermal treatment of polyimides at 350–450 °C (Rizzuto et al., 2017).
The improvement of the thermally treated polymeric membrane was
reported to be the results of chemical and structural change of the
polymer due to rearrangement and molecular transformation during the
thermal treatment (George et al., 2016). This transformation increases
the free volume of the polymer matrix (Han et al., 2012; Kim et al.,
2013). During the thermal treatment, an evolution of interconnected
micro-cavities occurs and micro-cavities with a narrow size distribution
are formed (Rizzuto et al., 2017), hence the permeability of TR mem-
brane increases with a slight change in their selectivity. In addition, the
TR membranes have improved resistance to CO2 plasticization
(AlQahtani and Mezghani, 2018; Smith et al., 2015). However, the
thermal rearrangement can also result in decreased mechanical strength
of the membrane (Liu et al., 2016; Scholes, 2016). Mechanical prop-
erties improvement of TR membranes has been conducted through
various strategies, such as copolymerization (TR copolymers) and
crosslinking (Calle et al., 2013; Li et al., 2013a,b; Scholes et al., 2014b,
2017). Even though the challenge of strengthening the mechanical
properties has been addressed, industrial trials are still needed to prove
the performance of TR membrane as the promising gas separation
membrane (Scholes, 2016).
PIM is another new class of polymeric membrane that is expected to
U.W.R. Siagian, et al. Journal of Natural Gas Science and Engineering 67 (2019) 172–195

Fig. 3. Permeability versus selectivity for selected membranes. (a) permeability vs. CO2/CH4 selectivity and (b) permeability vs. CO2/N2 selectivity. Note: FCM –
fixed carrier membrane; MMM – mixed matrix membranes; PIM – polymers of intrinsic micro-porosity; TR – thermally rearranged membrane; data (a) from refs.
(Adams et al., 2011; Al-Masri et al., 2000, 1999; Asghari and Afsari, 2018; Bae et al., 2010; Baker and Low, 2014; Belhaj Messaoud et al., 2015; Budd et al., 2008,
2005; Cao et al., 2003; Car et al., 2006; Centeno and Fuertes, 1999; Chen et al., 2012; Cho and Park, 2011; Choi et al., 2010; Chung et al., 2004; Cui et al., 2004; De
Vos and Verweij, 1998; Dorosti et al., 2014; Du et al., 2012a; Fritsch et al., 2011; Ghanem et al., 2009, 2008; Han et al., 2010; Himeno et al., 2007; Ismail et al., 2016;
Jazebizadeh and Khazraei, 2017; Jeazet et al., 2013; José et al., 2004; Jung et al., 2010; Khoshkharam et al., 2017; Kim et al., 2000, 2003; 2012; Koros et al., 1988;
Li, 1984; Lin and Chung, 2001; Liu et al., 2009, 2018; 2014, 2003b; 2003a; Mizumoto et al., 1993; Nagel et al., 2002; Nakagawa et al., 2002; Nik et al., 2012, 2011;
Overman et al., 1991; Park et al., 2007a; Perez et al., 2009; Peydayesh et al., 2013; Puleo et al., 1989; Raman and Brinker, 1995; Ren et al., 2003, 2019; Saedi et al.,
2014b, 2014a; Scholes, 2018; Scholes et al., 2012; Shao et al., 2005b, 2005a; 2004; Sodeifian et al., 2019; Suzuki and Yamada, 2005; Syrtsova et al., 2004; Tanaka
et al., 1992; Tena et al., 2010; Thür et al., 2019; Tin et al., 2003; Tomita et al., 2004; Vu et al., 2003b, 2003a; Wang et al., 2007, 2002; Wiheeb et al., 2015; Xiao et al.,
2004; Yang et al., 2001; Yong et al., 2001; Zhang et al., 2013a,b, 2008; Zhao et al., 2008; Zhu et al., 2006; Zornoza et al., 2011); data (b) from refs. (Al-Masri et al.,
1999; Althumayri et al., 2016; Askari et al., 2012; Bezzu et al., 2012; Budd et al., 2005, 2008; Calle et al., 2013; Calle and Lee, 2011; Carta et al., 2013; Chen et al.,
2018a; Cho and Park, 2011; Choi et al., 2010; Chua et al., 2012; Comesaña-Gándara et al., 2014; de Abajo et al., 2003; Du et al., 2009a, 2009b; 2010; Du et al.,
2011a, b; Du et al., 2012b; Fritsch et al., 2011; Ghanem et al., 2009; Han et al., 2010; Hirayama et al., 1996; Japip et al., 2014; Jawad et al., 2016; Jung et al., 2010;
Kasahara et al., 2012; Khan et al., 2013; Lau et al., 2015; Li et al., 2013a,b; Lin and Freeman, 2005; Liu and Xie, 2013; Ma et al., 2014, 2015; Ma and Pinnau, 2016;
Mondal and Mandal, 2014; Nafisi and Hägg, 2014; Okamoto et al., 1992; Park et al., 2007a, 2010; Rogan et al., 2014; Rose et al., 2015; Sakaguchi et al., 2017;
Sanders et al., 2012, 2014; Scholes et al., 2014b; Sekizkardes et al., 2016; Shao et al., 2009b, 2009a; Shishatskiy et al., 2010; Sodeifian et al., 2019; Song et al., 2013;
Swaidan et al., 2014; Tanaka et al., 1992; Wang et al., 2014a; Wang et al., 2014b; Wijenayake et al., 2013; Xiao and Chung, 2011; Xin et al., 2015; Yeong et al., 2012;
Yun et al., 2018; Zhang et al., 2018a; Zhao and Ho, 2013; Zhao and Winston Ho, 2012).

Fig. 4. Materials of MGS used for CO2 removal (based on publications indexed
by Scopus (TITLE (terms); January 9th, 2019). CA – cellulose acetate; MMM –
mixed-matrix membrane; MOF – metal-organic framework; PI – polyimide; PSF
– polysulfone; PIM – polymers of intrinsic micro-porosity.
surpass Robeson's upper bond for CO2 removal (Fig. 3). By definition,
intrinsic micro-porosity is a continuous network of interconnected
inter-molecular microcavities resulted from the contorted shape and
chain rigidity of the polymer structure (Wang et al., 2016). The inter-
connected pores are less than 2 nm (Wang et al., 2016). PIMs are easy to
be fabricated due to their high processability and solubility in the sol-
vent (Du et al., 2009a). PIM membrane exhibited high CO2 perme-
ability as well as selectivity which make them as a potential candidate
for gas separation membrane, especially in the case of CO2 removal or
capture. The high permeability and moderate selectivity are the results
of considerable open structure or high free volume due to the rigidity of
the chain polymer structure (Wang et al., 2016). The other considerable
features of PIMs for gas separation membrane are: they have low ac-
tivation energies for permeation, the transport properties are sig-
nificantly influenced by the preparation procedure of the membrane,
and the separation performance are affected by competitive sorption
(Gemeda et al., 2017). The first ladder-type PIMs, which are composed
of structurally contorted ladder-like backbones of spiro-centers and
fused dioxane rings, were introduced in 2004 for gas separation (Budd
et al., 2004b, 2004a). Since then, numerous works on modification of
this type of PIM, such as the addition of functional groups, have been
reported (Alaslai et al., 2016; Song et al., 2014). Among all types of
PIMs (PIM-1 to PIM-10), PIM-1 receives the most attention because of
its feasible fabrication, dense film formation, and ease of modifications
(Yong et al., 2016).
Inorganic membranes have been used for CO2 separation, particu-
larly at high temperature and pressure or other harsh conditions where
organic membranes cannot withstand (Makertihartha et al., 2017;
Zhang et al., 2013a,b). Some of zeolite-based inorganic membranes,
such as DDR zeolite, SAPO-34 zeolite, and Zeolite-T, exhibited high
selectivity and permeability for CO2/CH4 (Cui et al., 2004; Li et al.,
2006; Tomita et al., 2004) (Fig. 3). However, this type of membranes
has limited applicability due to the high cost and low processability,
membrane poisoning that reduce the performance, and low perme-
ability especially for dense inorganic membrane (Zhang et al., 2013a,b).
The fabrication cost of the module is around 3000 US$/m2, which is
much higher than the hollow fiber polymeric membrane (around 20 US

175
U.W.R. Siagian, et al.
$/m2) (Jusoh et al., 2016). In addition, zeolite membrane is also sig-
nificantly affected by impurities (e.g. water and H2S), which deterio-
rates the membrane performance (Li et al., 2005). In addition to zeolite,
the other inorganic materials that have been widely investigated for
CO2 separation are silica, metal organic frameworks (MOFs), carbon,
and amorphous metal oxide (Li et al., 2015a).
Carbon membrane is a porous inorganic membrane that offers
higher permeability and selectivity in comparison with the available
polymeric membrane (Ismail and David, 2001). The superior separation
performance is attributed to molecular sieving capability and ad-
sorptivity owned by carbon membrane. In addition, carbon membranes
have also been proven to be able to withstand high pressure (up to
70–200 bar) (Haider et al., 2018; Kruse et al., 2016; Vu et al., 2002),
thus promising to be applied for carbon capture from natural gas.
MOF is an emerging hybrid material, composing of metal ions as
coordination center, which are covalently bonded with organic linkers
(Férey, 2008; Furukawa et al., 2013). This material possesses high
porosity, high surface area, and high CO2 uptakes, making it as a pro-
mising candidate for CO2 separation (Venna and Carreon, 2015). A
number of studies have reported the development of MOF membrane
for CO2 separation, including the use of solvothermal growth method
for MOF-5 membrane preparation (Zhao et al., 2013a,b), continuous
flow process for ZIF-8 membrane preparation (Marti et al., 2017), and
annealing post treatment of MOF membrane (Rui et al., 2018). It was
shown that the annealed membrane exhibited a remarkable improve-
ment in both CO2 permeance and CO2 selectivity over H2 (Rui et al.,
2018). However, it is quite challenging to develop continuous MOF
membrane due to its poor intergrowth, low stability at high moisture
content, low reproducibility, and limited molecular sieving by the or-
ganic linker (Venna and Carreon, 2014).
Mixed matrix membranes (MMMs) are constructed from inorganic
materials in the form of micro or nanoparticles dispersed in the con-
tinuous polymeric matrix. The key advantage of the MMMs is the mo-
lecular sieving ability of the inorganic filler. In addition, the introduc-
tion of filler into an organic membrane solution may induce the
formation of the asymmetric structure allowing a membrane with a thin
skin layer supported by porous sub-layer. The asymmetric layer would
provide a better separation performance. The performance of notable
MMMs for CO2 removal is shown in Fig. 3. The major drawback of the
MMMs is the poor dispersibility of the inorganic particles within the
polymer matrix. The low distribution of the particles will lead to par-
ticle aggregation, resulting in membrane defects. This will deteriorate
the overall performance of a MMM (Zhang et al., 2013a,b). Therefore,
to produce an ideal MMM for gas separation, several parameters should
be considered/improved, such as polymer-inorganic filler pairs, adhe-
sion and interfacial contact between polymer and inorganic material,
the dispersion of inorganic filler in the polymer phase, particle size and
shape, and the loading of particles in the polymer (Jusoh et al., 2016).
Zeolite, alumina, silica nanoparticles, carbon nanotubes, graphene
oxide, and ZIFs have been widely used in MMM preparation for CO2
separation (Dilshad et al., 2019; Julian et al., 2019; Sarfraz and Ba-
Shammakh, 2018; Vinoba et al., 2017). Dilshad et al. (2019) reported
that a high CO2/N2 separation performance surpassing Robeson upper
bound 2008 could be obtained when 6 wt% loading of alumina particles
was used. Higher loading resulted in a decrease of gas permeation be-
cause of particles aggregation blocking the path of the gas molecule.
Hence, the number of inorganic particles incorporated need to be
controlled to achieve optimum permeation properties. Some recent
studies have shown that incorporating MOF significantly improved the
performance of MMM in CO2/CH4 separation (Ahmad et al., 2018; Guo
et al., 2018), but a major challenge still exists in the preparation of
MOF-based MMM for gas separation. Similar to other MMM synthesis,
the major challenge is defect formation in the membrane matrix due to
poor compatibility of MOF particle-polymer matrix which may result in
a low selectivity (Zhang et al., 2016).
Facilitated transport membranes (FTMs) have been developed for
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Journal of Natural Gas Science and Engineering 67 (2019) 172–195
CO2 separation from various gas mixtures (Deng et al., 2009; Huang
et al., 2008; Hussain, 2012; Quinn et al., 1997; Quinn and Laciak, 1997;
Tong et al., 2015; Zhao et al., 2014). In FTMs, CO2 could selectively
permeate through the membrane by means of a reversible reaction
between CO2 and a complexing agent-carrier incorporated in the
membrane, whereas the other non-reacting gases such as H2, N2, and
CH4 permeate exclusively by the solution–diffusion mechanism (Huang
et al., 2008). Thus, both high CO2 selectivity and permeability could be
achieved. The carriers could be designed as a mobile carrier (e.g. sup-
ported liquid membrane and ion-exchange membrane) or fixed carrier.
Deng et al. (2009) developed a PVAm/PVA blend FTM, where the
amino groups in the PVAm matrix facilitate the transport of CO2 and
result in high CO2 permeance up to 0.58 m3(STP)/(m2 h bar) as well as
a high CO2/N2 separation factor up to 174. Numerous studies have
reported FTMs with different carriers for CO2 separation from CH4 and
N2, however, more studies in the future need to address the perfor-
mance of FTM at high pressure CO2/CH4 separation application and
other harsh conditions of CO2 separation from flue gas (Rafiq et al.,
2016). It has been realized that FTMs are favorable to be used at low
CO2 partial pressures due to the carrier saturation phenomenon.
Moreover, membrane compression becomes another problem in high-
pressure application. Combining FTMs in mixed matrix configuration
then could be used to improve the stability at high pressures (Ansaloni
et al., 2015; Tong and Ho, 2017; Zhao et al., 2014).
2.2. State-of-the-art MGS for CO2 removal
The use of MGS for CO2 removal from natural gas has been applied
commercially from the 1980s and continually growing. It is estimated
that the market in this area to be $220 million/year in 2020 (Baker,
2002). Commercial MGSs in this area are currently supplied by several
companies including Medal (Air Liquid), W.R. Grace, Separex (now part
of UOP), Cynara (now part of Schlumberger), and ABB/MTR (Baker and
Lokhandwala, 2008). Essentially, all membranes currently used in
commercial applications are polymeric membranes mainly because of
their ease of manufacture. The use of cellulose acetate still dominates
the commercial membranes (such as UOP Separex™ and Schlumberger
Cynara) nowadays, while the use of alternative materials has been
continually increasing, such as polyimide (Air Liquide) and polysulfone
(Air Products). These commercial membranes are typically fabricated
into hollow fiber and spiral wound module.
Some of industrial-scale MGSs for CO2 removal are as follow (Baker
and Lokhandwala, 2008; Chen et al., 2018b; Sanders et al., 2013):
(1) A gas separation membrane plant was installed in Texas in 1983
for CO2 removal by Cynara (now part of Schlumberger). The
membrane was originally designed to treat 48 MMscfd of natural
gas and to reduce CO2 concentration from 45% to 28%. The plant
has been modified to double the capacity and to reduce CO2
concentration from 80% to below 10%.
(2) In 1994, a CO2 removal plant was installed in Michigan, USA to
handle 40 MMscfd gas with 11% of CO2 concentration. The plant
uses spiral-wound cellulose acetate membrane from UOP. The
treated gas contains less than 2% of CO2 after passing through a
two-stage configuration that is designed to minimize methane
losses.
(3) In 1995, a gas separation membrane plant was installed in
Kadanwari (Pakistan) with 210 MMscfd of capacity. At the time, it
was the largest plant of membrane-based natural gas processing.
The plant uses UOP Separex ™ membrane (cellulose acetate). The
plant reduces CO2 content from 11% to below 3%. The second
plant was installed with 234 MMscfd of capacity in Qadirpur. This
second plant is used to reduce CO2 content from 6.5% to below
2%. The capacity of Qadirpur Plant was upgraded to 500 MMscfd
in 2003 and then upgraded to 600 MMscfd in 2007.
(4) In 1997, a membrane gas separation plant was installed in Mexico
U.W.R. Siagian, et al.
using UOP's membrane for Enhanced Oil Recovery (EOR) appli-
cation. The plant processes 120 MMscfd gas containing 70% of
CO2. The purified CO2 gas stream with a concentration of 93%
CO2 is reinjected. The hydrocarbon product contains 5% of CO2.
(5) In 1999, UOP Separex™ membrane (cellulose acetate) was in-
stalled in two plants in Egypt, namely Salam (two units) and Tarek
(one unit). Each unit is a two-stage membrane unit to treat 100
MMscfd of natural gas from 6% CO2 to 3% CO2. The Salam Plant
was then expanded with 2 additional trains, which brings the total
capacity if Salam and Tarek Plants to 564 MMscfd.
(6) In 2004, natural gas sweetening using a hollow fiber cellulose
triacetate membrane from Cynara (now part of Schlumberger) was
installed in an offshore platform in the Thailand gulf (Cakerwala
gas field). The plant capacity is 668 MMscfd. to reduce CO2 con-
centration from 36% to 16%. The capacity has been doubled up to
1.28 Bscfd and it is currently the world's largest CO2 membrane
plant for natural gas processing.
(7) A natural gas processing plant using commercial polysulfone
membrane from PRISM (Air Products) was installed in July 2004.
The plant has a capacity of 8 MMscfd. CO2 in the natural gas
stream is reduced from 4.5% to 2%.
(8) In 2006, a hybrid system was installed in Indonesia processing 245
MMscfd of 40% CO2 gas down 20% in a UOP's membrane and then
down to 8% in a conventional amine solvent system.
(9) In 2007, a membrane gas separation plant was installed by UOP in
offshore Malaysia to process 680 MMscfd of gas from 45% CO2 to
6% CO2.
(10) In 2008, a membrane gas separation plant was installed by UOP in
offshore Thailand to process 530 MMscfd of gas from 34% CO2 to
12% CO2.
(11) In 2013, built a biogas upgrading plant in Switzerland with a ca-
pacity of 210 standard m3/year. The membrane is polyamide
hollow fiber.
There are several considerations in designing a membrane-based
CO2/CH4 separation system, which have been explained in detail by
Baker and Lokhandwala (2008). Pretreatment is typically required to
avoid fouling, plasticization, and condensation of hydrocarbons on the
membrane. The exact pretreatment required depends on the membrane
material and the feed gas characteristics (impurities, heavy compo-
nents, operating conditions). The design configuration of membrane
system could be designed in various ways, which depends on membrane
selectivity and permeance, CO2 contents in the feed gas, pretreatment
facilities required, the value of the gas, and the location of the plant
(onshore or offshore). For example, one-stage membrane configuration
is typically preferred for a plant dealing with a small gas flow because
of its simplicity, not involving rotating equipment, and minimal
maintenance required. In some cases, a two-stage membrane system is
used to reduce methane loss during processing. In this design, permeate
from the first stage is recompressed and passed through the second
stage. By doing so, the methane loss could be reduced to a few percent.
A combination of one-stage and two-stage membrane systems is useful
for treating a high concentration gas.
Koch et al. (2005) from UOP reported two types of pretreatment
systems for gas separation membrane in the CO2 removal process. The
first pretreatment system is called traditional pretreatment, which
consists of: (i) coalescing filter for the removal of liquid and mist from
the feed stream, (ii) non-regenerable adsorbent bed for removing trace
contaminants, (iii) particle filter for dust or particulates removal, and
(iv) heater for heating the gas to superheated condition. This traditional
pretreatment is sufficient for treating gasses with light and stable
compositions. However, adsorbent bed is the only item removing heavy
hydrocarbon compounds in this configuration and hence it may only be
limited for some applications. The second pretreatment is called as a
regenerative pretreatment. In this pretreatment, liquid or entrained
particles are removed in a filter-coalescer. Then, other harmful
177
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
components (water, heavy hydrocarbon, and others) are removed in a
thermal swing regenerable adsorbent-based system. To recover any
adsorbent fines in the gas, a particle filter is used. Preheater is used to
adjust the temperature of the gas. The regenerative system has some
advantages, including (i) water and other contaminants (e.g. mercury):
are removed along with heavy hydrocarbon, thus additional dehydra-
tion unit is unnecessary, (ii) mercury and mercaptans can be removed
in the same bed, and (iii) it can be used in wide variation of the feed gas
content.
For CO2 removal from flue gas, the use of MGS is still not available
commercially and only applied in the research and development stage.
This is due to the challenges such as low partial pressure of CO2 in flue
gas and a high temperature of the flue gas stream (Norahim et al.,
2018). However, MGS may be ranked as the most promising technology
for CO2 removal from flue gas for certain applications/emission sources
and the great promise of metallic and ceramic membranes that are
capable of withstanding high temperature (Aaron and Tsouris, 2005).
Hasan et al. (2012a,b) study the viability of three processes (absorption,
membrane, and adsorption) to capture CO2 from various emission
sources (with the range of CO2 concentration in feed stream between 2
and 70%-mole. It was reported that membrane is still less economically
attractive than absorption for heat and energy generation sector where
the feed gas contains less than 15–20% CO2 because the operating cost
of the membrane-based process is higher than absorption-based pro-
cess. This is because the membrane-based process (at this feed con-
centration) requires a large feed compressor to provide sufficient
driving force of separation. However, the membrane was reported to be
the most economically attractive process to capture CO2 from industrial
sources with a higher CO2 concentration in the flue gas (above 20
%-mole), such as cement, oil refinery, and steel plants. At this com-
position, the membrane-based process requires a smaller feed gas
compressor (and hence lower cost), while the absorption-based process
requires a higher operating cost because of the higher energy required
to regenerate the solvent. A study by Chung et al. further confirms this
approach, where it was reported that the most economically attractive
option to capture CO2 from a blast furnace in the steelmaking industry
is a hybrid of amine scrubbing and membrane with a heat recovery
system (Chung et al., 2018).
Several membrane design configurations have been proposed as
cost-effective options for this CO2 capture purpose. Merkel et al. (2010,
2013) reported that they developed new membrane called Polaris™,
which possesses modest selectivity but much higher CO2 permeance
(10–50 times the commercial cellulose acetate membranes). This
membrane was applied in a novel design process that possess a higher
driving force of separation than the conventional membrane design by
utilizing the combustion air as a sweep gas. They also found that ap-
plying vacuum in the permeate side will require less energy consump-
tion than compressing in the feed side. Moreover, the former approach
will be the referred and cost-effective membrane design approach
especially if high permeance membranes (> 4000 gpu) or cheap
membrane cost (< $50/m2) are developed (Merkel et al., 2010). A
study by Scholes et al. proposed an alternate design to further improve
the performance, where an additional air separation unit is installed to
enrich the O2 in the sweep gas for combustion. This leads to a higher
CO2 concentration in the feed gas, which results in low parasitic load
(30%) (Scholes et al., 2013).
Han and Ho. (2018) reported that PEO-based membranes and
amine-based facilitated transport membrane are currently the only
feasible materials for CO2 removal for both post-combustion and pre-
combustion schemes. This material provides a minimal CO2/N2 se-
lectivity of 50 and high permeance (up to 3000 gpu). These membrane
materials are also suitable for pre-combustion CO2 capture because of
high CO2/H2 selectivity and good stability at high pressure (> 100 °C)
in the presence of H2S.
U.W.R. Siagian, et al.
2.3. Main challenges in MGS for CO2 removal
In designing MGS for CO2 separation system, it is desired to get high
permeability and selectivity. High CO2 permeability is desired to reduce
the required membrane area and the operating pressure thus reducing
the total processing cost. Meanwhile, a high selectivity membrane re-
duces the membrane area (or stage) and it increases the product re-
covery. In the case of CO2/CH4 separation, a high selectivity membrane
is also important to reduce the loss of CH4 during the process. CH4 loss
is one of the important parameters determining the overall processing
cost. For example, a membrane with a selectivity (CO2/CH4) of 35 has
been investigated by Peters et al. for natural gas upgrading (Peters
et al., 2011). Results of the simulation showed that about 9.5% of CH4
loss (feed gas: 9.5 mol-% of CO2; 72.4 mol-% of CH4; and other gases i.e.
ethane, propane, butane, pentane, and hexane) was observed in a single
stage membrane processing while only 0.47% of CH4 loss was observed
in a 2-stage process. Even though the 2-stage process exhibited a lower
total processing cost, this cost could be further reduced if the selectivity
of the membrane is improved.
The main drawbacks of the polymeric membrane used for gas se-
paration are a trade-off between permeability and selectivity, and the
phenomena of plasticization and aging. Another challenge in the de-
velopment of the MGS is the limited report on the selectivity of the
membrane material in the CO2-methane mixture measurements (Baker
and Low, 2014). Most reported performances of the developed mem-
branes were based on the pure-gas measurements. Some novel materials
have been found to show pure-gas selectivity of 50 or more, yet cellu-
lose acetate (with mixed gas selectivity of 10–15) remains as the in-
stalled material in natural gas processing plants. It has been reported
that most materials may lose their selectivity performance when tested
with mixed gas at the high natural gas processing pressures.
The permeability of the membrane has an inverse relationship with
the selectivity, wherein the increase of permeability results in the de-
crease of selectivity and vice versa. This characteristic has been studied
by Robeson, which is known as Robeson's upper bond (Robeson, 2008,
1991). Only a few of membrane materials can across this upper bond.
Therefore, in order to achieve a significant process performance im-
provement, it is essential to characterize and develop membranes that
could across this upper bound (high permeability and selectivity). In
terms of CO2/CH4 upper bound relationship, Robeson classified the
thermally rearranged polymers, which contain benzoxazole-phenylene
or benzothiazole-phenylene structures (Park et al., 2007b), as materials
with remarkable separation performance. This Robeson's upper bound
has now been widely used as a standard for the membrane development
as it shows the superiority of the transport and separation character-
istics of fabricated membranes (Adewole et al., 2013).
Plasticization is another main concern in the application of poly-
meric membrane for CO2 removal, as membrane typically becomes
swollen when it is exposed to CO2 and hydrocarbon compounds, par-
ticularly at high pressures. Bos et al. reported a study on CO2-induced
plasticization-in various glassy polymers and defined this phenomenon
as the increase in CO2 permeability as a function of feed pressure (Bos
et al., 1999). This plasticization results in an increase of permeability of
CO2 with the increasing pressure while the selectivity is reduced. In
addition, membranes may be irreparably damaged due to plasticization.
Plasticization pressure is usually used as an indicator to evaluate
polymeric material for CO2 removal. Plasticization pressure is the
minimum pressure that is required to induce the increase in perme-
ability (Dai et al., 2016a) (Fig. 5). At plasticization pressure, the per-
formance of a membrane starts to decrease, which leads to an increase
in methane loss and thus negatively impact the economics (Wind et al.,
2004). Sanders et al. (2013) described two common indicators of
plasticization, which are: 1) increase in gas permeability as the function
of upstream gas partial pressure and 2) a loss in membrane selectivity
when the upstream total pressure (or partial pressure of one or more
components) increases. It has been found that plasticization depends on
178
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
the thickness of the materials, CO2 pressure, exposure time, aging time,
and the prior preparation/storage/thermal treatment history (Dai et al.,
2016a). In the case of membrane material, the plasticization pressures
of several membranes have been identified. The plasticization pressures
of other materials are shown in Fig. 6.
Many efforts have been devoted to overcoming this problem by
modifying the polymeric membrane, such as by thermal rearrangement,
polymer cross-linking, and polymer blending (Zhang et al., 2013a,b).
By using those modification methods, plasticization could be reduced
while the membrane performance could be improved. The improve-
ment of thermally modified membrane was reported as the result of the
arrangement of the fractional free volume of the membrane (Han et al.,
2010). Thermal annealing of the Matrimide membrane, for example,
has been developed to suppress plasticization of this type of polyimide
membrane (Dai et al., 2016a). Cross-linking may result in the change in
the chemical structure of the polymers, and so consequently changing
the mobility of the chains. When a membrane is modified via cross-
linking, the molecular free volume between the polymer chain increases
after modification (Zhang et al., 2013a,b). An example of the cross-
linking process in order to obtain higher rigidity and improved anti-
plasticization is the cross-linked polyimide. The cross-linking process
can be done by thermal, UV, and chemical treatments. Diol cross-
linking polyimides, which contain carboxylic acid groups, have been
widely studied for this purpose (Baker and Low, 2014).
Physical aging is another significant hurdle for the application of
glassy polymeric membrane in gas separation. Physical aging is asso-
ciated with the change of free volume or macro void inside the mem-
brane matrix (Adewole et al., 2013; Sanders et al., 2013). This is the
result of the segmental motion of the polymer, which gradually in-
creases the density of the polymer. The permeability of the membrane
declines along with the increase of membrane selectivity because the
free volume decreases (Fig. 5). This phenomenon could be observed by
the declining membrane flux over time. The mechanism of the rapid
physical aging that occurs in the thin film membranes has not been fully
understood yet. However, previous studies have reported several key
variables that affect the physical aging behavior of the thin film
membranes, which are membrane thickness (thinner membranes may
have high physical aging rate), membrane preparation/storage history,
and membrane operation temperature/pressure and storage atmo-
sphere (Dai et al., 2016a). Strategies to solve the physical aging can be
classified as two different approaches, (i) by freezing the initial free
volume state in place (e.g. hybrid material, polymer blending) and (ii)
by using a cross-linking agent to increase the structure rigidity
(Amooghin et al., 2016). For example, an effort to suppress physical
aging of super glassy polymer for gas separation has been reported by
Lau et al. (Amooghin et al., 2016). Three types of polymeric membrane,
i.e. poly(trime-thylsilylpropyne) (PTMSP), poly(4-methyl-2-pentyne)
(PMP), and PIM-1 were modified with the addition of ultraporous ad-
ditive, porous aromatic framework (PAF). Long-term performance test
(1 year) indicated that the modification could successfully inhibit the
physical aging of those membranes whilst retaining the improved CO2
permeability and high CO2/N2 selectivity. A new approach for produ-
cing an anti-aging of MMM for CO2 removal has been reported by
Kitchin et al. (HonáLau, 2015). The so-called anti-aging intercalating
membrane (AIM) was prepared by introducing soluble metal-organic
polyhedral (MOP) with various organic chain lengths. The use of MOP
was reported as an effective way to reduce the aging rate (up to three
times). The introduction of MOP allowed a better mixing with poly-
meric membrane eliminating non-selective void which usually found in
a traditional MMM.
Generally, there are a number of impurities present in a natural gas
stream that could reduce the performance of the membrane or even
induce membrane damage. A moisture content could cause mechanical
damage of the membrane, while heavy hydrocarbons could form a film
on the membrane surface which reduces the permeability (George et al.,
2016). In addition, liquid or condensation should be avoided because it
U.W.R. Siagian, et al.
Fig. 5. Schematic representation of (a) CO2 permeability vs feed pressure and plasticization pressure (Ppl) and (b) physical aging.
Fig. 6. Plasticization pressure (Ppl) and (a) permeability and (b) productivity loss at Ppl of various material. Data from refs. (Akbar Samadi et al., 2016; Bos
et al., 2001, 1999; 1998; Chern et al., 1987; Mohr et al., 1991; Reimers and Barbari, 1994; Scholes et al., 2010a; Wessling et al., 1995).
can decrease the membrane integrity. The effect of various impurities
on PVAm/PVA blend composite membrane performance has been re-
ported (Uddin and Hägg, 2012). They reported that the performance of
membrane and the effect of impurities such as hydrogen sulfide, n-
hexane, and propane, are significantly affected by water (humidity).
The maximum loss of CO2 permeance and CO2/CH4 were about 18%
and 16%, respectively, at high humidity. Therefore, the feed gas stream
should undergo a stringent pretreatment to avoid a significant loss of
membrane performance. The detail on design and pre-treatment of
MGS, especially for natural gas processing, has been reported in pre-
vious works (Baker, 2002; Baker and Lokhandwala, 2008).
3. Membrane contactor (MC)
Schematic of MC process is illustrated in Fig. 2 b. In MC, the porous
membrane acts as a support to provide extra area for contact between
two phases, and hence it promotes the mass transfer (Purwasasmita
et al., 2015b). The membrane is expected to provide non-dispersive and
better contacting process between the gas and the solvent, while the
CO2 selectivity is dominated by the solvent. Ideally, MC is operated in
non-wetted mode, of which the membrane pores are filled only with the
gas phase. The penetration of the absorbent liquid into membrane pores
should be prevented so that a low mass transfer resistance can be
achieved as the gas–liquid interface in the pore mouth is maintained.
For this purpose, microporous membranes from polymers with a high
hydrophobicity such as polytetrafluoroethylene (PTFE), poly-
vinylidenefluoride (PVDF), and polypropylene (PP) are commonly
used. Among these materials, microporous PTFE membranes are the
most hydrophobic and they offer good and stable performance, but the
materials are very expensive (DeMontigny et al., 2006; Khaisri et al.,
179
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
2009; Nishikawa et al., 1995). Microporous PP membranes are in-
expensive, but they are less hydrophobic than membranes from
fluorine-containing polymer (such as PTFE and PVDF). Microporous
PVDF membranes could be a good candidate for the development of MC
as they are cheaper and easier to fabricate than PTFE.
In addition to the high hydrophobicity, membranes used in MC
should also have good thermal stability, excellent chemical stability,
and high porosity. It was reported that the use of polymers with high
melting temperature (Tm), such as PTFE and polyether ether ketone
(PEEK), with Tm of 327 °C and 335 °C, respectively, can be a good
choice as the membrane material in order to achieve durable and
thermally-stable MC (Wang et al., 2011a). It is desirable that the
membrane has a high porosity to minimize the mass transfer resistance.
However, it can also give impact on membrane wetting, as reported by
Rajabzadeh et al. (2013), where a highly porous membrane with large
pore diameter was completely wetted and the CO2 absorption flux de-
creased drastically after 100 h.
Apart from the membrane selection, absorbent type and operating
parameters are also important factors determining the MC performance.
In this regard, a number of experiments, modeling, and simulations
have been carried out (Mansourizadeh et al., 2010; Zhang et al., 2019;
Zhang, 2016). A recent study reported that the absorbent concentration
had the greatest effect on the efficiency of CO2 absorption, followed by
gas velocity and liquid (absorbent) velocity (Zhang et al., 2019). This
was associated with the increase in chemical reaction rate between the
CO2 and the absorbent. A high chemical reaction rate can also be ob-
tained by selecting a suitable chemical absorbent. Having CO2 reaction
rate constant, piperazine (PZ) has gained great attention to be used as
the single absorbent or to be blended with the other alkanolamine ab-
sorbent (Zhang et al., 2018b; Zhang, 2016).
U.W.R. Siagian, et al. Journal of Natural Gas Science and Engineering 67 (2019) 172–195

FAS – fluoroalkyl silane; LDPE – low-density polyethylene; PDMS – polydimethylsiloxane; PP – polypropylene; PTFE – Polytetrafluoroethylene: PVDF – polyvinylidene fluoride; SMM – surface modifying macromolecule.
3.1. Recent development of membranes for MC

Abdulhameed et al. (2017)

(Ahmad et al., 2013a)

Pengrui et al. (2017)

Recently, there are numerous studies devoted to developing mem-

Franco et al. (2011)

Lv et al. (2012a)
brane displaying good separation properties for MC application. The

Lin et al. (2016)

Lin et al. (2009)

Yu et al. (2015)

Lu et al. (2009)
Li et al. (2018)
main purpose is for preventing membrane wetting. There are two types
of membrane developed for this purpose, i.e. superhydrophobic mi-
croporous and non-porous composite membranes. Both types of mem-

Ref.
brane are discussed in the following sub-sections.

CO2 absorption using DEA, MDEA, activated MDEA, and activated K2CO3 (Feed gas: CO2
3.1.1. Superhydrophobic (microporous) membrane

CO2 absorption using MEA (Feed gas: CO2 and N2 with a volume ratio of12.5:87.5)
As stated above, a microporous membrane having a surface that is

CO2 absorption using MEA (Feed gas: CO2 and N2 with the volume ratio of 20:80)
highly resistant to wetting is required in gas–liquid MC. For this reason,

CO2 absorption using PZ, MDEA, and AMP (Feed gas: (CO2/CH4 20/80 vol.%)
superhydrophobic membranes having high water-repellency is then
proposed for use in MC. It has been well-known that superhydrophobic

CO2 absorption using AMP/PZ (Feed gas: 9 vol% CO2/N2 gas mixture)
surface with high water contact angle (WCA) of above 150° and low
sliding angle (SA) of below 10° is the result of a combination of low

CO2 absorption using K2CO3 (Feed gas: CO2/CH4 40/60 vol%)

surface energy material and the surface roughness (Celia et al., 2013;

CO2 absorption using MEA (Feed gas: CO2/CH4 40/60 vol%)

CO2 absorption using MEA (Feed gas: 20% (v/v) CO2 in N2)
CO2 absorption using MEA (Feed gas: 14 vol % CO2 in N2)
Roach et al., 2008; Xue et al., 2010). Based on this insight, numerous
efforts have been devoted to synthesize superhydrophobic membranes
from various materials and through different methods. The past studies

CO2 absorption using water (Feed gas: pure CO2)

reporting the superhydrophobic preparation and investigating its use in
MC for CO2 absorption are tabulated in Table 1.
Superhydrophobic polymeric membranes can be fabricated by di-

and N2 with the molar ratio of 13:87)

rect processing - Electrospinning is one of the direct processing methods
which is reported to have succeeded in fabricating superhydrophobic
nanofibrous membranes from various neat polymer solutions (Kang
et al., 2008; Lee et al., 2013; Liao et al., 2013b; Patel and Chase, 2014)
and polymer blends (Dong et al., 2014). In addition, nanoparticles-in-
corporated polymer solutions have also been used as the feed of elec-
trospinning resulting in superhydrophobic composite membrane (Li
et al., 2015b; Liao et al., 2014b, 2014a; Tijing et al., 2016; Wang et al.,
Process

2011b). However, only a few of these studies tested the resulting

membrane performance for carbon capture. Another method is the

–
improvement of phase separation by controlling solution and process
LEPw (bar)

parameters such as polymer concentration, coagulant type, vapor ex-

6.5/5.5b
posure time, and air temperature (Kuo et al., 2008; Peng et al., 2012).
0.7a

2.5
In both electrospinning and improvement of phase separation processs,
–

–
–
–

–
–

–
surface roughness can be introduced during membrane preparation,
WCA/SA (°)

158.4/1.3

thus when it is combined with the hydrophobicity of polymer used,

155/ < 3

superhydrophobicity can be achieved. Blending polymer solution with

164.5
150

143
151
152
158

153
142

low surface energy material such as surface modifying macromolecule

–

(SMM) can also increase the membrane hydrophobicity (Bakeri et al.,

2012; Efome et al., 2015; Essalhi and Khayet, 2012; Mansourizadeh
et al., 2014; Rahbari-Sisakht et al., 2012a, 2012b; Suk et al., 2010).
Grafting with perfluoro oligomer
Electrospinning followed by FAS

Spray deposition of silica/PDMS

Spray deposition of silica/PDMS

However, the superhydrophobicity seems difficult to be achieved by

Coating with rough LDPE layer
Plasma treatment using PTFE

Coating with rough PP layer

using such a method which might be due to insufficient surface

roughness created.
The liquid entry pressure of 5 wt% MEA aqueous solution.
CF4 plasma treatment

Superhydrophobic polymeric membrane can also be fabricated by

Modification Method

Grafting with FAS

Grafting with FAS
Grafting with FAS

surface modification of the existing polymeric membrane, in which the

modification can be performed in one-step or two-steps processes. Low
modification

surface energy materials can be used for simultaneous surface rough-

Superhydrophobic membrane for CO2 absorption.

ening and hydrophobization via several different ways, one of which is

plasma treatment. Hydrocarbon precursors, either containing fluorine
The liquid entry pressure of 2-propanol.

(Bae et al., 2001; Franco et al., 2011, 2012; Lin et al., 2009; Yang et al.,
2014, 2015) or fluorine-free (Lee et al., 2011), have been successfully
used to fabricate superhydrophobic membranes. Coating membrane
γ-alumina membranes on α-alumina

with rough hydrophobic polymer film is a simpler way, in which the

alumina tube with ZrO2 layer

rough surface can be induced by using non-solvent(s) (Ahmad et al.,

kaolin-alumina hollow fiber

2013a; Franco et al., 2008; Himma et al., 2017a, 2017b; Lv et al.,

Membrane Base Material

2012a) or by introducing nanoparticles (Zhang et al., 2013a; Zhou

et al., 2014). It has also been reported that the preparation of super-
hydrophobic polymer membrane through one-step modification can be
PDMS/PVDF

support

done by using a chemical vapor deposition method (Zheng et al., 2009).

In two-steps modification, the process sequence can be roughening
Table 1

PVDF

PVDF
PEEK

PTFE

membrane surface followed by hydrophobization using low-surface-

PP
PP

PP

b
a

energy material or vice versa. Sequential modifications through

180
U.W.R. Siagian, et al.
membrane surface roughening using nanoparticles such as TiO2
(Razmjou et al., 2012), silver (Liao et al., 2013a), and silica (Fang et al.,
2012; Park et al., 2016) followed by hydrophobization using fluor-
osilane compounds are the most reported.
Most inorganic membranes which are hydrophilic in nature require
surface modification to alter its surface nature from hydrophilic to su-
perhydrophobic. Some studies have modified ceramic membranes sur-
face by grafting method using fluoroalkyl silane (FAS) compounds
(Abdulhameed et al., 2017; An et al., 2015; Lu et al., 2009; Yu et al.,
2015). During the grafting process, the hydroxyl (–OH) groups on the
surface of pristine ceramic membrane react with Si–O–alkyl groups of
the silane (Picard et al., 2001). The grafting efficiency is strongly in-
fluenced by the length of FAS chains, grafting time, and multiplicity of
grafting (Kujawa et al., 2014; Lu et al., 2009). Using appropriate
parameters, superhydrophobic ceramic membranes have been suc-
cessfully prepared (Lu et al., 2009; Yu et al., 2015). The super-
hydrophobic ceramic membranes are highly potential to be applied in
membrane contactor for carbon capture at high temperature.
A number of studies on the use of superhydrophobic membranes for
CO2 absorption have shown that superhydrophobic membranes out-
performed membranes without superhydrophobicity (Abdulhameed
et al., 2017; Ahmad et al., 2013a; Franco et al., 2012; Lin et al., 2016;
Lv et al., 2012a). The superhydrophobic membranes showed higher
CO2 absorption flux and more stable flux over long periods. For in-
stance, superhydrophobic nanofibrous membrane prepared by electro-
spinning and FAS modification showed a stable CO2 absorption flux of
approximately 1.5 mmol/m2.s for four days of operation, which was in
contrast with the unmodified nanofibrous membrane showing a dra-
matic decrease in CO2 absorption flux even in the first 100 min (Lin
et al., 2016). The high performance is attributed to anti-wetting beha-
vior of the superhydrophobic membranes, preventing penetration of
liquid absorbent into membrane pores (Franco et al., 2011; Himma
et al., 2018, 2019; Himma and Wenten, 2017; Lu et al., 2008).
3.1.2. Non-porous composite membrane
Apart from porous MCs with a superhydrophobicity, recent re-
searches focus more on the development of non-porous MCs. It is ex-
pected that the non-porous MCs provides a much more stable perfor-
mance compared to porous MCs, especially in terms of wetting. The
membrane used in non-porous MC can be an integrally dense mem-
brane, skinned asymmetric membrane, or composite membrane con-
sisting of a thin dense layer coated on a porous support. The integrally
dense membrane logically imposes higher resistance to mass transfer
than skinned asymmetric membrane or composite membrane. The use
of non-porous composite membrane was then most widely reported.
In a non-porous composite membrane, the dense skin layer imposes
an additional mass transfer resistance, thus polymers with high CO2
permeability such as PTMSP (Dibrov et al., 2014; Nguyen et al., 2011;
Scholes et al., 2015) and PIM-1 (Scholes et al., 2015) is preferentially
used as its material. In addition, polymers with less permeability but
has very high hydrophobicity such Teflon AF 1600 (Scholes et al.,
2015) and Teflon AF 2400 (Dai et al., 2016c; Nguyen et al., 2011) have
also been investigated for its use as the dense skin layer material.
Nguyen et al. (2011) have prepared composite hollow fiber membranes
based on a thin dense skin, based on Teflon-AF and PTMSP, coated on
microporous support (PP). It was demonstrated that the Teflon-AF
composite membrane showed CO2 capture ratio (as a function of gas
velocity) similar to the microporous PP membrane. With the addition of
dense skin thickness of 1.1 μm, the Teflon-AF composite membrane
exhibited the lowest reduction in the mass transfer coefficient of about
15%. Moreover, an investigation over long time scales, i.e. over 1000 h
showed that dense skin composite membranes based on PMP/PP and
Teflon-AF/PP exhibited CO2 flux density comparable to PTFE and sig-
nificantly higher than PP after 500 h (Chabanon et al., 2011). These
studies proved that a dense skin composite MC could provide both
wetting prevention characteristics and high mass transfer of CO2. The
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Journal of Natural Gas Science and Engineering 67 (2019) 172–195
dense skin layer should also have high hydrophobicity in addition to the
high CO2 permeability so that it would be more effective for CO2 re-
moval application (Scholes et al., 2015). Aside from wetting preven-
tion, another advantage by placing the dense skin layer on the porous
support is the ability for selective mass transfer. Belaissaou et al. (2016)
used dense skin MC for biogas purification. In addition to giving mass
transfer performance that is comparable to microporous MC, the poly
(phenylene oxide)-based dense skin MC could reduce the loss of me-
thane.
3.2. State-of-the-art of MC for CO2 removal
Considerable studies on the MC application for CO2 removal from
various gas streams have been conducted, even though only a few of
them have been tested in pilot or larger scale. In this regard, two major
applications of MC for CO2 removal are post-combustion carbon cap-
ture and CO2 removal from natural gas (Sreedhar et al., 2017; Zhao
et al., 2016). The following section discusses the development of MC
technology.
MC technology was early developed by Kvaerner Process Systems
(KPS) together with W.L. Gore & Associates GmbH (GORE), SGL Carbon
Group (SGL) and Ottestad Breathing Systems (OBS) for CO2 removal
from gas turbines on off-shore oil and gas platforms in Norway in 1992
(Zhao et al., 2016). Between 1998 and 2001, the trials were performed
in a large pilot scale. The MC showed a CO2 capture efficiency of 85%
with the exhaust gas flow rate was 2610 kg/h. From 1998 to 1999, pilot
tests of MC were also performed for natural gas treatment (Herzog and
Falk-Pedersen, 2000). Pilot tests with the longest operation of 5000 h
were held at a gas terminal in Scotland, in which activated MDEA was
used as the absorbent. In addition, a physical solvent was also used in
pilot tests held at the Shell Fandango field in Texas. TNO, the Nether-
lands Organization for Applied Scientific Research, has long been de-
veloping CO2 membrane gas absorption. Its application for CO2 removal
from flue gas and reuse in the horticultural industry has been reported,
in which a significant reduction in the CO2 production cost could be
achieved by using the MC (Feron and Jansen, 1995). In 1997, the
project was developed in a pilot plant, at which the carbon dioxide and
heat supply were combined to greenhouses (Feron and Jansen, 1997).
Gas Technology Institute (GTI) in the United States (US) have de-
veloped MC technology (called Carbo-Lock™) for CO2 capture with
PEEK membrane since 2010 (Zhao et al., 2016). The super-
hydrophobized PEEK membrane maintained its high performance in the
presence of flue gas contaminants (such as O2, NO2, and SO2) and stable
performance with CO2 capture efficiency of above 90% was achieved in
an absorption test for ∼120 h (Shiguang Li et al., 2013a,b).
Researchers in Cooperative Research Center for Greenhouse Gas
Technologies (CO2CRC), Australia, reported pilot plant trials of porous
MC (PP and PTFE) and nonporous MC (polydimethylsiloxane, PDMS)
for post-combustion CO2 separation (Scholes et al., 2014a). The PP
membrane experienced significant wetting in both laboratory and pilot
plant tests, whereas the PTFE membrane experienced wetting when
tested in pilot plant. The PDMS MC did not experience wetting, but it
had the lowest overall mass transfer coefficient among other materials
testes, which was lower than PP MC in two orders of magnitude both in
laboratory and pilot scale performance tests.
A study by Vericella et al. (2015) proposed a novel approach called
encapsulated solvent to combine the use of membrane and solvent
absorption to capture CO2 from flue gas. The solvent is encapsulated in
a thin membrane capsule with a diameter of 100–600 μm and thickness
of 10 μm. This concept combines the benefit of both technologies,
where the solvent selectively reacts with CO2 (not with N2) in a high
surface area contactor provided by the silicone-based membrane cap-
sule (Vericella et al., 2015). This results in smaller contactor dimensions
required compared to conventional absorber This is beneficial the
permeability and selectivity of the system can be independently mod-
ified, which is different to conventional MGS where permeability and
U.W.R. Siagian, et al.
selectivity are usually competing parameters. This novel design has
been tested at lab-scale and pilot scale (1 MWe coal testing facility at
the DOE National Carbon Capture Center) (Hornbostel et al., 2019).
Using their expected capsule properties and N2CO3 30%-wt. as working
solvent, the absorber height required and the energy penalty are ap-
proximately 10% and 18% lower, respectively, than the conventional
MEA-absorber system. In order to be economically competitive (com-
pared to conventional absorber), it was reported that the capsule
thickness needs to be reduced by up to an order of magnitude without
adversely affecting the capsule stability and integrity (Raksajati et al.,
2018, 2017).
A number of studies on MC that were close to real conditions of CO2
separation from natural gas have also been carried out. Al-Marzouqi
et al. (2017) have reported the long-term operational stability of PFA
hollow fibers MC in simultaneous CO2 and H2S removal from a gas
stream whose composition was similar to natural gas at a high pressure
of 50 bar using hot absorbent at a temperature of 100 °C. High pressure
MCs were also reported in other works (Kang et al., 2017; Marzouk
et al., 2012, 2010). Modeling and simulation of MC for natural gas
sweetening have also been conducted (Quek et al., 2018; Rezakazemi
et al., 2011), providing important insights for the design and operation
aspects.
MC has also been widely developed for CO2 separation from re-
newable resources such as biogas. A pilot-scale MC based on nonporous
PVTMS membrane for biogas conditioning has been constructed and
tested by researchers from Topchiev Institute of Petrochemical
Synthesis, Russian Academy of Sciences in collaboration with NPK
BIOTEST (Shalygin et al., 2011). The test results suggested that con-
trolling absorbent flow is very important for dealing with varying
biogas compositions and flow. Considerable efforts in developing MCs
for biogas upgrading were also reported by Park et al. (2017) proposing
MC with pressure-cascaded stripping configuration and Schiavon Maia
et al. (2017) conducting bench-scale and pilot test of MC for H2S and
CO2 removal from biogas using a regenerable Fe-EDTA solution.
3.3. Challenges in MC
For MC, the solvent must be selected carefully in order to achieve a
high separation performance. Generally, the solvent should have a high
absorption capacity for CO2 and should also be compatible with the
type of membrane used in MC. It is important to consider solvent-
membrane compatibility since the solvent may react with the polymeric
membrane, which could result in membrane degradation (Luis et al.,
2012). The solvent-membrane pair should be carefully selected to avoid
the damage of the membrane, both physically and chemically. The
change of membrane properties, when exposed to sorbent, has been
investigated by several studies. Barbe and co-workers studied the
change of surface morphology of PP membrane during initial contact
with water (Barbe et al., 2000). After 72 h of contact, they observed
that the membrane surface morphology, such as porosity, pore (area,
length, breadth, and diameter) and pore spread factor, changed as the
result of the non-wetting intrusion of the water into some pores which
enlarge the pore entrance. Two types of hydrophobic hollow fiber
membranes, PP and PTFE, were used in carbon capture from flue gas
using MC in a work conducted by DeMontigny et al. (2006), where
aqueous solutions of 2-amino-2-methyl-1-propanol (AMP) and mono-
ethanolamine (MEA) were used as solvents. It was reported that the
PTFE membrane could maintain the initial performance, while the PP
membrane underwent performance deterioration over time. The effect
of various solvent on microporous polyethylene membrane properties
was investigated by Komo et al. (Kamo et al., 1992). The solvents used
in their study were n-hexane, ethyl alcohol, p-Xylene, Mono-
chlorobenzene, DMF, and DMSO. When treated with those various
solvents, the permeability of the membrane was increased, the pore size
was enlarged, and the membrane was shrinking. They concluded that it
was due to the deformation of microfibrils of the hollow fiber
182
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
membrane, which may be caused by the surface tension of the solvents.
This deformation of microfibrils was followed by adhesion of adjacent
microfibrils. Membrane-solvent compatibility for CO2 removal appli-
cations using MC was also investigated by Dindore et al. (2004). Five
types membrane material i.e. PTFE, PP, PVDF, PES, and PS, and eight
types of solvent i.e. water, propylene carbonate, selexol, N-methyl
pyrrolidone, dimethyl formamide, tributyl phosphate, glycerol triace-
tate, and n-formyl morpholine were used in their study. It was reported
that only PTFE and PP were compatible with the organic solvents while
the others were incompatible in terms of morphological damage,
shrinkage, dissolution, swelling, and color changes. The authors found
that PTFE and PP in combination with propylene carbonate were the
most promising membrane-solvent pairs for CO2 absorption. Further-
more, with regard to the membrane fabrication cost, PP-propylene
carbonate was considered as the most promising candidate.
The membrane wetting becomes a major concern in MC since it
highly determines the long-term performance of the membrane. Partial
wetting can still occur although the membrane used is intensive hy-
drophobic (Chabanon et al., 2011; Lu et al., 2008; Zhang et al.,
2008a,b), which then increasing the membrane resistance (Rangwala,
1996; Zhang et al., 2008a,b) (Fig. 7). This situation may result in a
significant drop CO2 (Lv et al., 2012b). Wetting phenomena in MC and
its prevention have been widely investigated -(Goyal et al., 2015; Lv
et al., 2010; Malek et al., 1997; Mosadegh-Sedghi et al., 2014; Zhang
et al., 2008a,b). Various approaches have been made to prevent the
membrane wetting, including optimization of operating condition
(Simons et al., 2009; Yan et al., 2007), solvent and membrane selection
(Albrecht et al., 2005; DeMontigny et al., 2006; Dindore et al., 2004;
Yan et al., 2007), and membrane development by controlling the
membrane pore structure (Nguyen et al., 2011; Rajabzadeh et al., 2013)
and the membrane surface properties, in particular, towards super-
hydrophobicity (Bakeri et al., 2012; Franco et al., 2012; Lin et al., 2016;
Rahbari-Sisakht et al., 2012b; Yu et al., 2015). Among these, the two
latter strategies have gained great attention recently due to the pro-
mising high performances as discussed in the previous section. How-
ever, for further development of CO2 absorption membrane, the chal-
lenges are how their durability in operation at high pressures and
temperatures and in the presence of contaminants such as SO2. This is
necessary to be investigated in the development of superhydrophobic
MCs as well as non-porous MCs.
One of the major drawbacks which is usually faced in membrane
operation is fouling (Ariono et al., 2017; Kang and Cao, 2012;
Khoiruddin et al., 2017; Rana and Matsuura, 2010; Wenten and
Khoiruddin, 2016). Fouling phenomena generally reduce the mem-
brane flux (either temporarily or permanently) which seriously ham-
pering the applications of membrane processes (Aryanti et al., 2017;
Fig. 7. Schematic illustration of membrane hydrophobicity and CO2 flux in MC
as a function of operation time.
U.W.R. Siagian, et al.
Khoiruddin et al., 2014; Rana and Matsuura, 2010; Sianipar et al.,
2017). Membrane fouling is another challenge in MC, even though the
adverse impact on the performance of MC is less significant compared
to the impact of membrane wetting. Fouling in MC is reported to be not
as severe as that of membrane filtration. However, in industrial appli-
cations where the flue gas stream contains contaminants such as dust or
suspended particles, the membrane fouling becomes a bigger concern.
Zhang et al. (2015) reported that the existence of fine particles in flue
gas from coal-fired desulphurized power plant decreased the efficiency
of CO2 removal due to the deposition and adsorption of fine particles on
the surface and pores of the microporous membrane. In order to avoid
membrane fouling, the contaminants should be removed in the flue gas
pre-treatment facilities. Alternatively, the use of membrane with anti-
fouling properties or self-cleaning ability can be used to prevent such
problem without requiring pre-treatment facilities. It has been reported
that superhydrophobic surface also has the self-cleaning ability
(Bhushan et al., 2009; Xue et al., 2010). In membrane application, the
self-cleaning property of superhydrophobic membrane makes foulants
are easy to be released from the membrane surface (Himma et al., 2016;
Himma et al., 2018, 2019; Zhao et al., 2013a,b). Therefore, the use of
superhydrophobic membrane could mitigate the membrane fouling in
MC. A study by Yu et al. (2015) showed that superhydrophobic ceramic
membrane displayed a better anti-fouling property compared to the PP
membrane without superhydrophobicity. The ceramic membrane sur-
face is not covered by dust even after being operated for treating flue
gas for one-month operation.
4. Comparison of MGS and MC for carbon capture
In CO2 removal applications, MGS and MC have their own ad-
vantages and disadvantages. The comparison of both membrane-based
processes is listed in Table 2. With regard to the status of commercia-
lization, MGS has been commercialized and applied on a large scale
particularly for natural gas sweetening (see Section 2.2) competing with
amine-based absorption system.
The effect of gas flow rate and CO2 concentration in feed gas stream
on the choice of CO2 removal methods from natural gas were illustrated
schematically by Baker and Lokhandwala (2008). According to the plot,
MGS is favorable when the gas stream contains relatively high CO2
concentration (up to 40 mol%) and a low gas flow rate (< 10 MMscfd).
On the other hand, an amine-based absorption system is preferable for
feed gas stream with a low concentration of CO2 (∼2–25 mol%) and
high gas flow rate (up to 500 MMscfd). Meanwhile, for feed gas stream
with high CO2 concentration and flow rate, a combination of MGS and
amine is preferable. One of the important features of MGS is that it does
not require solvent, therefore it does not require chemical regeneration,
solvent make up, and another associated handling. Since the separation
is not dependent on the chemical sorbent, the use of MGS for separation
of high concentration is more economical than amine-based absorption
(in certain feed gas characteristics). Furthermore, when the
Table 2
Comparison of membrane gas separation vs. membrane contactor for CO2 removal from natural gas.
Parameter MGS
Typical membrane used Dense
Solvent None
Selectivity Determined by the membrane (20–50)
Pre-treatment for impurities removal Highly required (Baker and Lokhandwala,
2008)
Energy consumption Normal to high
Cost Normal to high
Drawbacks ➢ Plasticization (polymeric-based membrane);
➢ The trade-off between permeability and
selectivity;
➢ Physical aging;
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Journal of Natural Gas Science and Engineering 67 (2019) 172–195
concentration of the CO2 is higher, the driving force for the separation
will be increased, which is beneficial for MGS. However, it should be
noted that, as the CO2 concentration increases, the membrane will be
more susceptible to plasticization (Bos et al., 1999). If MGS is used for
treating a feed gas with a low CO2 concentration, the driving force will
reduce and a significant amount of valuable gas (product or CH4 loss in
case of CO2/CH4) is lost. As a consequence, the performance of MGS can
decline and the processing cost may increase. In term of energy con-
sumption, MGS required a relatively high energy consumption than MC,
which associated with the use of a dense membrane and the high op-
erating pressure.
MC could provide very high selectivity and it can be used to treat
feed gas stream with a low concentration of CO2 effectively (Klaassen
et al., 2008). Unlike MGS, MC has a very high selectivity so that it could
be applied in a wide range of gas flow rate and concentration without
any loss of product gas. The high selectivity is provided by the chemical
or physical interaction between the gas and the absorbent. MC is
usually operated under low operating pressure so the operating cost
will be lower than MGS. Despite the advantages, MC also has several
disadvantages, such as wetting phenomenon, fouling, and membrane
degradation, as have been discussed in the previous sections. Other
disadvantages, which should also be considered, are as follow
(Mansourizadeh and Ismail, 2009):
- The membrane used in MC becomes another transport resistance
because it could reduce the overall mass transfer and reduce the
selectivity. This resistance will be more pronounced if the mem-
brane becomes wetted.
- Non-uniform hollow fiber distribution in the membrane module can
lead to channeling and bypassing which can reduce mass transfer
efficiency. Therefore, the flow configuration and module geometry
should be considered.
- Operating conditions can significantly affect the performance of MC.
Temperature, pressure, and flow rates, both gas and solvent or li-
quid streams, should be carefully controlled to (i) avoid gas bubble
formation which could result in gas loss, (ii) avoid wetting by the
solvent, and (iii) simultaneously increase residence time and gas
absorption.
Generally, MC uses organic solvent such as amine solution for CO2
removal applications. Despite the high selectivity provided by the sol-
vent, the use of this type of organic solvent also has several drawbacks.
Amine solution has high vapor pressure, is corrosive, and needs high-
energy for regeneration (Babamohammadi et al., 2015). Recently, a
new type of absorbent, ionic liquid (IL), has attracted researchers to
apply it in MC for carbon capture. An IL is a salt which has a melting
point below 100 °C and is composed of an organic cation and an organic
or inorganic anion (Dai et al., 2016b). The interesting features of IL are
high CO2 solubility, high selectivity, low vapor pressure, and high
thermal stability (Dai et al., 2016b; Karadas et al., 2010). With those
MC Ref.
Porous (Bernardo et al., 2009; Li and Chen, 2005;
Zhang et al., 2013a,b)
Needed
Determined by the solvent (> 1000) (Li et al., 2013a,b)
Required
Low Zhang et al. (2013a,b)
Low Zhang et al. (2013a,b)
➢ Wetting phenomenon; (Luis et al., 2012, 2011; Wang et al., 2016)
➢ Fouling;
➢ Membrane degradation;
 U.W.R. Siagian, et al.

Table 3
Economic of MGS for CO2/CH4 separation.
Flow (k N m3/ Membrane Type α (CO2/CH4) AT (103 m2) Membrane Cost ($/m2) CO2 in feed (mole- Fraction of CO2 removed (A) or in Total capital investment Total cost ($/k N Ref.
h) %) product (B) (106 $) m3)

43.2 CA 21 ∼10 (2S) ∼54a 25 A: 0.944 2.8 8.2/Vf Bhide et al. (1998)
35 CA 20 NA (2S) 54b 20 vol.-% NA – 16/Vp Datta and Sen
(2006)
43.2 6FDA-HAB 60 ∼14 (1S) ∼100 (including 20 A: 0.9 – 7.7/Vp Hao et al. (2002)
module)
26.5 NA (model) 20 ∼0.35 (2S) ∼90 20 A: 0.9 – 10.7/Vp Qi and Henson
(1998)
b
416.7 PVAm/PVA 35 11 (2S) 50 2.9 B: < 0.02 14 4.05/Vf Peters et al. (2011)
416.7 PVAm/PVA 35 79 (2S) 50b 9.5d B: < 0.02 14.1 4.05/Vf Peters et al. (2011)
29.2 PVAm/PVA 35 56 (2S) 50b 9.5d B: < 0.02 1.7 4.73/Vf Peters et al. (2011)

184
500 CNTs reinforced PVAm/ 17.9 (Pf: 40 bar) 262 35c 10 B: 0.039 – 5.73/Vp He et al. (2014)
PVA
50 CNTs reinforced PVAm/ 24.6 (Pf: 20 bar) 10.3 35c 50 B: 0.039 – 0.572/Vp He et al. (2014)
PVA
c
50 Carbon 49.74 (Pf: 119 100 10 B: < 0.02 – 0.128/Vp
50 bar)
c
50 Carbon 49.74 (Pf: 495 100 50 B: < 0.02 – 0.433/Vp
50 bar)

Notes:1S – single stage; 2S – two stages; 6FDA-HAB: the fluorine-containing polyimide membrane; AT – total membrane area; CA – cellulose acetate; PVAm/PVA – polyvinyl amine and polyvinyl alcohol) membrane; Vf –
volume of feed; Vp – volume of product.
a
Membrane life: 3 years; Plant life: 10 years.
b
Membrane life: 4 years.
c
Membrane life: 5 years.
d
CH4: 72.4; Total of other compounds (ethane, propane, butane, pentane, hexane): 18.1; all in mole-%.
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
U.W.R. Siagian, et al. Journal of Natural Gas Science and Engineering 67 (2019) 172–195

interesting features, the performance of MC for CO2 removal could be

Merkel et al. (2010)

Yan et al. (2008)

Yan et al. (2011)
further improved especially when operated at high temperatures, such

Ho et al. (2006)

Ho et al. (2008)

He et al. (2015)
Zhai and Rubin

Ho and Wiley
as for flue gas treatment. However, for future applications, IL still need

Scholes et al.

Tuinier et al.
much efforts to make it favorable for commercial scale (Dai et al.,

(2013)

(2011)

(2013)

(2004)
2016b).
Ref.

Techno-economic assessment of membrane-based carbon capture

for both natural gas sweetening and flue gas cleaning have been con-

α(CO2/N4): 50; PCO2: 1000 GPU; AT = 2521b;

α(CO2/N4): 20; PCO2: 100 barrer; two stages;

α(CO2/N4): 135; PCO2: 740 GPU; two stages;

ducted by several studies (Table 3 and Table 4). Analysis of techno-
economic aspects of MGS for natural gas sweetening (CO2 and H2S
removal) has been conducted by Bhide and Stern (Bhide and Stern,
α(CO2/N4): 500; PCO2: 1000 GPU;

α(CO2/N4): 500; PCO2: 1000 GPU;

α(CO2/N4): 50; PCO2: 1000 GPU;
α(CO2/N4): 20; PCO2: 72 Barrer;

α(CO2/N4): 20; PCO2: 72 Barrer;

1993a, 1993b). The effects of process configuration, operating condi-

Absorbent: MEA (20%; 40 °C)

tions, and membrane properties were also analyzed. In the first study,
AT = 3 × 106; two stages

they found that the three-stage membrane configuration offers the

Absorbent: MEA (30%)

lowest processing cost. This configuration consisted of a single mem-
brane stage in series with two-stage membrane cascade with recycling.
AT = 2 × 105;

In the second study, the authors compared the MGS with conventional
two stages;

amine gas absorption system. They concluded that the MGS showed
Remarks

lower gas processing cost than the amine plant over the entire CO2
concentration considered (5-40 mol-% of CO2 in feed). They also com-
pared the performance of MGS and hybrid process (MGS + amine
plant) in natural gas sweetening application (Bhide et al., 1998). In the
31.3 (2S); 30.7 (3S)

hybrid system, the MGS was used as the first stage of treatment to re-
CO2 Capture cost

move the portion of CO2 while the amine system was used as polisher
step to obtain a product gas that meet the pipeline specification. The
($/tonne)a

2.9–4.4

study indicated that MGS was more economic than the hybrid process
∼39.3
120.9

47.87
∼55

∼50
46.8

for gas stream containing only CO2. The gas processing cost of the
82

39

hybrid process was lower than a solely MGS system when the feed gas
Hollow fiber Polyphenyleneoxide membrane;

contained 1 mol-% of H2S. Meanwhile, the independent gas absorption

was not competitive under most of the conditions.
Simulation of MGS for CO2/CH4 separation was conducted by Datta
and Sen to find an optimum gas processing cost (Datta and Sen, 2006).
The system was simulated using up to three-stage membrane config-
uration for CO2 concentration of 5–90 vol.%). They found that there
Polyphenyleneoxide; 50;
Membrane; Cost ($/m2)

Polypropylene; ∼4.8;

was no single process configuration that is optimum for all CO2 con-
Polypropylene; 7.4;

centration and natural gas price ranges evaluated, instead the optimum
configuration was found only in a specific range of CO2 concentration.
Polaris™; 50;

In addition, the gas processing cost of two- and three-stage configura-

PPO; 80;

FSC; 35

tion was similar in almost all cases, especially for 5–40 vol.% CO2
-; 50;

-; 50;
150;

Per tonne of CO2 avoided (= CO2 capture - CO2 emitted from supplementary power).
50;

concentration.
Process design and economic analysis of MGS for CH4/CO2/H2S
Operating condition (P;

separation were investigated by Hao et al. using two different types of

membrane (Hao et al., 2002). The first type of membrane was H2S-
116.3 kPa; 30 °C;

5–10 kPa; 25 °C;

0.25 MPa; 35 °C

11.3 kPa; 40 °C;

1.5 MPa; 30 °C;

0.2 MPa; 30 °C;

0.4 MPa; 30 °C;

AT – membrane area (m2); PPO – Polyphenyleneoxide; FSC: fixed-site-carrier.

selective polymeric membrane (PEUU), while the second type was CO2-
2 MPa; 30 °C;

2 MPa; 30 °C;

selective membrane (6FDA-HAB). The concentration of CO2 was up to

0.2 MPa

40 mol-%. The results indicated that the cost of methane loss was
dominant for gas processing cost of process configuration without re-
T)

cycle stream. A single stage system utilizing only H2S-selective mem-

Inlet feed gas (P; T)

Atmospheric; 95 °C

brane was favorable for treating a feed gas with ≤10 mol-% of H2S and
0.1 MPa; 21.5 °C
0.1 MPa; 150 °C;

0.1 MPa; 93 °C;

Economic of MGS and MC for CO2 capture from flue gas.

lower concentration of CO2. Meanwhile, for feed gas containing

95 kPa; 110 °C

2 kPa; 150 °C;

≤40 mol-% of CO2 and a small amount of H2S (≤8 ppm), a single stage
0.1 MPa

system utilizing the CO2-selective membrane was favorable. For feed

gas stream containing a substantial amount of CO2 (≤40 mol-%) and
–

H2S (10 mol-%), two stage membrane system wherein the first stage
CCO2 in feed

utilizing H2S-selective membrane and the second stage using CO2-se-

13.31%-vol
13.5%-vol

12%-mole

14%-mole

∼15%-wt

lective membrane was the most economical process configuration.

11.6%

12.9%
14%

13%

13%

Ahmad et al. studied the techno-economic aspect of MGS for CO2/

CH4 where the effect of temperature and pressure on membrane per-
1652.4 (k N m /hr)

formance were investigated (Ahmad et al., 2013b). They reported that

3238 (tonne/hr)
578.7 (tonne/h)

those parameters influenced the separation performance in terms of

3

m2/tonne/h of CO2.
18,260 kmol/h
40,000 m3/h

product composition, methane loss, and separation stage which affected

500 (m3/s)

535 S m /s

500 m3/s
Flowrate

3
635 kg/s

894 kg/s

the gas processing cost. Engineering evaluation of MGS for CO2 se-
paration from flue gas and biogas has been conducted by Brunetti et al.
(2014). Several selection criteria have been analyzed. According to the
study, the separation of MGS depended on various interrelated factors
Process
Table 4

MGS

MGS

MGS

MGS

MGS

MGS

MGS

MGS

such as membrane selectivity and permeability which is typically de-

MC
MC

b
a

pend on membrane material, operating conditions, and the product gas

185
U.W.R. Siagian, et al.
requirement.
Compared to MGS, economic analysis of MC for carbon capture can
hardly be found in the literature. Comparison of MC and conventional
amines system for CO2 capture from flue gas has been conducted by Yan
et al. (2008), where the performance and economic of the processes
were investigated. According to their result, the performance and gas
processing cost of MC were significantly affected by the wetting phe-
nomenon. MC exhibited a larger overall mass transfer coefficient, about
2.9 times, than the conventional amine system when a fresh membrane
was utilized. As a result, the gas processing cost of MC was lower than
MGS (Table 4). However, the superiority of MC could not be maintained
when half of the membrane pores was wetted. When the membrane was
wetted, a considerable reduction of the overall mass transfer was ob-
served. Therefore, to keep the superiority of MC, this wetting phe-
nomenon should be addressed. From the economic analysis, it was
found that the capital investment and CO2 capture cost of MC were
significantly influenced by membrane price and lifetime, and the SO2
concentration in the feed gas stream. If the lifetime of the membrane
was less than the critical value, the cost of CO2 capture of the MC would
be higher than the amine plant system.
The study of Yan et al. (2008) indicated that the carbon capture
from flue gas stream using MC had lower CO2 capture cost than MGS
reported by several studies. This may be associated with the high se-
lectivity, high mass transfer of porous membrane, the low operating
pressure of MC, and lower membrane cost. Nevertheless, MC also has
several disadvantages (see section 4.2) that should be addressed for its
industrial applications. In the case of MGS, the major challenge for flue
gas treatment is the scale of the process, which is associated with the
large volume of the gas stream and the low CO2 concentration (Luis
et al., 2012). It will particularly affect the separation performance of
MGS (mass transfer rate and selectivity) and the required membrane
area. Even though the driving force of MGS can be improved using
several strategies, such as by increasing feed pressure, recirculating an
enriched CO2 stream, decreasing the permeate pressure, and reducing
CO2 concentration in the permeate pressure via a sweep gas, those will
require an additional energy consumption and extra cost (Luis et al.,
2012). Favre has pointed out several aspects that should be taken into
consideration if it would be applied in carbon capture from a flue gas
stream (Favre, 2007). The points are as follows: (i) MGS will require a
higher energy consumption than absorption for feed gas stream con-
taining 10% of CO2 even when the membrane has selectivity above 120;
(ii) energy consumption of MGS will be competitive for treating feed
gas stream with more than 20% of CO2; (iii) to be competitive in the
latter case, the selectivity of the membrane should be around 60 or
higher; (iv) the energy consumption can be significantly reduced when
a vacuum condition is applied in permeate side; (v) since the mass
transfer of MGS is much lower than MC (4–6 times), permeability im-
provement is needed; and (vi) the best type of operation should be
identified to fit with the target of residual water concentration because
it is rarely be analyzed. Improving membrane performance to obtain
CO2 permeance of 3 m3(STP)/m2 h bar) and CO2/N2 selectivity more
than 40 is required in the development of membrane materials (He,
2018). In addition, further improvement to reduce the cost of CO2
capture to $20/tonne CO2 is also necessary to make the MGS eco-
nomically feasible for industrial applications.
Another interesting case for the selection of membrane-based
carbon capture is when it should be applied for sweetening natural gas
with very high CO2 concentration, for example, a natural gas reserved
in Natuna field, Indonesia. As the biggest natural gas field in Asia
Pacific, the utilization of natural gas in Natuna field is challenged by the
high concentration of CO2 (up to 71%) (Batubara et al., 2014; Muslim
et al., 2015). It leads to a very expensive processing cost and only a
small portion of CH4 remains in the sales gas. As this natural gas field is
projected to fulfill the long-term national gas demand, the development
of the reliable process is strongly needed. The high concentration will
be beneficial for MGS since it will result in a high driving force and high
186
Journal of Natural Gas Science and Engineering 67 (2019) 172–195
transfer rate. However, the membrane will be more susceptible to
plasticization. In addition, the loss of CH4 during the process is in-
evitable. Therefore, in this case, MC would be an interesting alternative
process. Generally, the feed gas from the field has high pressure that
allows the use of physical absorption for CO2 removal (see section 4.3).
The absorption of CO2 can be performed in MC using water such as
from seawater as the solvent or absorbent. The use of water from sea-
water could potentially reduce the cost of CO2 capture due to its large
resource (and inexpensive), even when a high flow rate of gas should be
handled and a large volume of absorbent is required (due to the high
concentration of CO2). In addition, the use of water instead of alka-
nolamine solutions can reduce the tendency of membrane wetting (for
hydrophobic and superhydrophobic membranes) because it has high
surface tension. Since the absorbent has high CO2 concentration and
still has high pressure, it could be directly injected into a nearby oil well
for pressure maintenance that it is beneficial for enhancing oil pro-
duction. Another benefit from this scheme is carbon credit obtained
from the carbon storage. As the overall result, a cost involved in gen-
erating high-pressure water in the absorption process would be ac-
commodated by the benefits of the carbon storage. By using the pro-
posed scheme, the processing of a gas stream with a very high CO2
concentration may make sense economically.
5. Conclusion and perspectives
In recent years, there have been increasing efforts in reducing CO2
emissions, including energy efficiency improvement, implementation of
low/no fossil carbon, and carbon capture & storage (CCS) as well as
geo-engineering. Among these, CCS is likely to become an attractive
and efficient way of mitigating CO2 emissions since it requires
minimum fundamental changes in the existing design, production, and
products schemes. For CO2 capture, solvent absorption is currently the
well-established technology and the most promising methods in the
near future due to the high selectivity and capacity, as well as simplicity
in the regeneration of solvents. However, absorption has some dis-
advantages related to regeneration energy, limited mass transfer area
and flow rates, and operational problems including flooding, loading,
channeling, and foaming. This opens opportunities for emerging alter-
natives technologies, such as membrane-based processes, to be applied
in CO2 capture and natural gas processing fields in the longer term
because of the potential to overcome the limitations of current tech-
nology. The main advantages of CO2 separation from natural gas and
CO2 capture using membrane-based technologies are low cost, low
energy requirement, flexible operation, and modularity.
Despite the potential application of membrane-based carbon cap-
ture, i.e. MGS and MC, they also have some limitations for the industrial
application that should be addressed. For MGS, the effort for industrial
application should be focused on developing a new generation of
membrane that has high mechanical stability against high temperature
and pressure, has anti-plasticization property to ensure its durability
(Zhang et al., 2013a,b), as well as high permeability and selectivity.
Meanwhile, for MC future research should aim to find new membrane
materials that are compatible with the absorbent (Zhang et al.,
2013a,b). In addition, future studies of MC should also assess the
techno-economic evaluation in large scale application, development of
novel module configuration to achieve a better mass transfer, and
performance test under a real gas condition and high operating pressure
and temperature (Mansourizadeh and Ismail, 2009). The use of super-
hydrophobic that has high wetting resistance against aqueous solvent in
MC is one of the interesting ways to avoid wetting and to ensure a long-
term stability. The interesting features of new developed ionic liquids
could be one of the promising candidates of solvent for improving the
performance of MC. However, confirmation of the performance of ionic
liquids is needed before it can be used for commercial applications.
Another interesting case for the selection of membrane-based carbon
capture is when it should be applied for sweetening natural gas with
U.W.R. Siagian, et al.
very high CO2 concentration.
Acknowledgement
Financial assistance for this work was provided by “Program
Penelitian, Pengabdian kepada Masyarakat, dan Inovasi (P3MI)”,
Institut Teknologi Bandung.
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