1 s2.0 S1875510019301039 Main PDF

Journal of Natural Gas Science and Engineering 67 (2019) 172–195
Contents lists available at ScienceDirect
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

patents) on membrane system, 6.3% (2242 patents) on rectification-
The capture of carbon dioxide (CO2) from gaseous streams has condensation, and 1.9% (687 patents) on biological separation (Luis
gained a great interest and becomes an important process in many in- Míguez et al., 2018). The fewer patents on membrane systems were
dustrial areas. Concerning global warming and climate change, carbon likely due to the relatively fewer materials that have been investigated
capture is considered as an attractive and efficient solution to mitigate and developed for CO2 capture. Solvent-based CO2 capture is currently
the CO2 emission from combustion of fossil fuels (Ratnakar et al., 2018; the well-established technology and the most promising methods in the
Venkatraman et al., 2017). In this regard, CO2 can be captured using near future due to the high selectivity, -high capacity, and simplicity in
the following technological pathways: post- or pre-combustion capture the regeneration of solvents (Aaron and Tsouris, 2005; Wang et al.,
and oxy-combustion (Figueroa et al., 2008; Gibbins et al., 2008; Johns 2011a). However, the solvent absorption has also major drawbacks,
and Dindoruk, 2013; Pires et al., 2011; Ratnakar et al., 2018; Yuan including high energy required for solvent regeneration and operational
et al., 2005). Meanwhile, in natural gas processing, CO2 (and other acid problems such as flooding which limits the capacity of the absorption
gases) needs to be separated to meet the specifications required by the column (Ahmad et al., 2010; Mansourizadeh and Ismail, 2009). This
buyers (for example pipeline transmission and distribution companies). opens opportunities for emerging alternatives technologies, such as
By separating CO2 from natural gas, the calorific value of natural gas membrane, to be applied in CO2 capture and natural gas processing
increases, the volume of the transported gas decreases, and its corrosive fields in the longer term because of the potential to overcome the
tendency decreases. Another emerging application of CO2 removal is limitations of current technology (Roussanaly et al., 2016).
biogas purification to produce biomethane. These needs have en- Membrane technologies have been applied in various processes and
couraged the continuous development of carbon capture methods. industrial sectors replacing conventional technologies due to their in-
Common technologies for CO2 capture are solvent absorption, solid teresting features (Bernardo and Drioli, 2010; Drioli et al., 2011, 2003;
adsorption, and membrane-based separation (Darabkhani et al., 2018; Himma et al., 2018, 2019; Makertiharta et al., 2017; Purwasasmita
Hemmati et al., 2019a, 2019b; Lee et al., 2019; Pellegrini et al., 2019; et al., 2015a; Van der Bruggen et al., 2004; Wardani et al., 2017;
Wenten et al., 2017). It has been reported that up to 2017 there were Wenten et al., 2018). In the case of CO2 separation from natural gas and
35,434 patents on CO2 capture technologies consisting of approxi- flue gas, the main advantages of membrane-based technologies are low
mately 32.4% (11,463 patents) on chemical separation, 29.8% (10,550 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. 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-
Fig. 1. Number of annual publications related to membrane gas separation and of-the-art and challenges in MGS for CO2 removal are presented. To
membrane contactor for CO2 capture and separation the past 20 years. Source: date, all membranes used in commercial applications are polymeric
Scopus (TITLE-ABS-KEY (terms); terms: membrane gas separation CO2, mem- membranes mainly because of their ease of manufacture. Even though
brane contactor CO2 + membrane gas absorption CO2; January 10th, 2019). in recent year various type of materials (including inorganic and
polymer-inorganic composite) have been developed as alternatives
Selective membranes for CO2 capture have been widely developed and demonstrating promising features under research conditions, such as
applied since the 1970s. The application of gas separation using ceramic, glass, metals, zeolite, and carbon molecular sieve, but they
membranes has been rapidly growing. This is indicated by the nu- cannot compete commercially with the current polymeric membranes
merous works on membrane gas separation (MGS) for CO2 which have because of the high module fabrication cost. Therefore, the review
been published during the last two decades (Fig. 1). MGS has been presented in this paper also discusses the prospect and challenges of
widely investigated for CO2/CH4 separation from natural gas (Adewole various materials for CO2 removal. In addition, the current status and
et al., 2013; Scholes et al., 2012; Yeo et al., 2012). MGS could also be development of MC for CO2 removal are discussed, in particular, the
applied for post-combustion capture (CO2/N2 or CO2/N2/O2 separation development of superhydrophobic membrane as an attractive strategy
from flue gases (Aaron and Tsouris, 2005; Powell and Qiao, 2006)) and to prevent membrane wetting. Finally, the performances of MGS and
pre-combustion capture (CO2/H2 separation after or in water-gas shift- MC for carbon capture are compared and analyzed, and some per-
membrane reactor unit (Scholes et al., 2010b)). spectives are given.
Although gas transport through membranes has been systematically
studied in more than a century, membrane fabrication technology was 2. Membrane gas separation (MGS)
significantly advanced along with the development of asymmetric
membrane in the 1970s (Baker, 2004). Afterward, notable milestones in Schematic illustrations of MGS and MC process for CO2 capture and
the industrial application of MGS, particularly for CO2 capture appli- separation are shown in Fig. 2. The membrane for MGS can be classified
cation are reported (Bernardo and Clarizia, 2013). Even so, many im- into three groups according to the mechanism of separation, namely:
provements are still required to achieve high performance of gas se- simple sorption diffusion (i.e. selective surface diffusion, molecular
paration using membrane, i.e. producing a high CO2 rate, as well as sieving, and solution-diffusion), complex sorption-diffusion (i.e. fa-
improving selectivity and durability of the membrane. There have been cilitated transport and palladium-based membrane for hydrogen), and
efforts in the field of membrane development in order to achieve such ion-conducting membranes (Koros and Mahajan, 2000). Among those
membrane improvements. One of the options of novel membrane-based types, polymeric membranes with solution-diffusion mechanism have
technologies is gas–liquid membrane contactor (MC) which combines been the most widely used (Koros and Fleming, 1993; Moradihamedani
membrane with conventional phase contacting operation such as ab- et al., 2013; Robeson, 1999; Wang et al., 2013). In this mechanism, gas
sorption, and hence the benefits of both technologies can be fully uti- molecules from the feed side are firstly absorbed by the membrane,
lized. In MC, a porous membrane is used to provide an extra area for then they diffuse across the membrane matrix, and subsequently desorb
on the permeate side. Schematic of MGS process is illustrated in Fig. 2 a.
Fig. 2. Schematic of (a) membrane gas separation (MGS) and (b) membrane contactor (MC) for CO2 removal.
173
A dense membrane is employed as a selective barrier between the feed surpassing the Robeson's upper bound (Cho and Park, 2011). Polyimide
gas and the permeate gas stream. The selectivity of the membrane de- membranes have been extensively studied and developed for gas se-
pends on the solubility and diffusivity of the gas molecule in the paration application (Zhang et al., 2013a,b). Polyimides with tri-
membrane matrix. The performance of MGS is generally measured as its fluoromethyl (CF3) groups have drawn interest due to the good pure gas
permeability and selectivity. To achieve the desired performance (high selectivity and permeability and also the good solubility in many or-
permeability and selectivity), the type of membrane material should be ganic solvents (Baker and Low, 2014). The drawback of polyimide
appropriately selected. Therefore, various types of membranes for MGS, membrane is the decrease of permeability and selectivity in practical
especially for CO2 removal, have been developed. More details on the applications using mixed gas feed (compared to lab conditions) with
types of membranes are discussed in the following sub-section. higher loss of performance than cellulose acetate, the most commonly
used polymeric membrane for gas separation (White, 2010). Further-
2.1. Membranes used in MGS more, polyimide is also more susceptible to plasticization compared
with cellulose acetate.
The performance and characteristics of gas separation using mem- Polysulfones have been discussed as the other commercial mem-
brane depend on several factors, such as the membrane material, branes that have excellent mechanical properties, good thermal and
structure, thickness, and configuration (e.g. hollow fiber, flat sheet) as chemical stabilities, and are easy to process into a membrane (Sanders
well as the module/system design (Bernardo et al., 2009). Several et al., 2013). Compared with cellulose acetate, polysulfones have lower
materials have been developed for CO2-capture membrane, including CO2 permeability and CO2/CH4 selectivity, but higher plasticization
organics, inorganics, and organic – inorganic composites, with their pressure (Julian and Wenten, 2012). An optimum polysulfone mem-
own typical advantages and limitations. brane formulation reported in (Pesek and Koros, 1993) has been ex-
Most commercial membranes for gas separation are currently amined for CO2/CH4 and showed selectivity between 33 and 65
dominated by organic or polymeric membranes since they have some (Gordeyev et al., 2001; Gordeyev and Shilton, 2004; Ismail et al., 2003,
attractive features, e.g. lower fabrication cost compared to inorganic 1999; Ismail and Lorna, 2003; Sharpe et al., 1999).
material, and easy to fabricate either into flat and hollow fiber module. Another target of works devoted to MGS is to develop polymeric
The polymeric membranes can be divided into rubbery state (kept membranes that could withstand a challenging environment (for ex-
above its glass transition temperature and presents substantial free- ample high temperature operation). Perfluoropolymer membrane is one
volume) and glassy state (kept below its glass transition temperature of the polymeric membranes that suitable for such challenging condi-
and has low fractional free-volume) (Bernardo et al., 2009). Several tion, for example, raw natural gas treatment (Okamoto et al., 2016).
types of polymeric materials such as cellulose acetate, polyimide, Perfluoropolymer membranes have strong C-F bonds, which result in
polysulfones, and perfluoropolymer, have been used for MGS. Among excellent chemical and thermo-oxidative stability. Poly(tetra-
these polymeric membranes, it has been reported that polyimide and fluoroethylene)/PTFE, which is considered to be the early generation of
cellulose acetate are the most widely used in commercial scale. Fig. 3 a perfluoropolymer, has been reported to have low permeability and low
and b shows some of the most important studies regarding the se- processability due to the high crystallinity. However, during further
lectivity and permeability performance of the polymeric membranes development of this membrane, amorphous glassy perfluoropolymer
used for gas separation (see Fig. 4). membranes were introduced, such as Cytop©, Teflon AF©, and Hyflon
Cellulose acetate was initially developed for reverse osmosis mem- AD©, which have high gas permeability, and high solubility in per-
brane which is commercially applied in desalination. Cellulose acetate fluorinated solvents (thus good processability) (Arcella et al., 2003,
is now the most widely used membrane material for CO2 removal from 1999; Cui et al., 2014; Pinnau and Toy, 1996). Despite those ad-
natural gas. Commercial cellulose acetate membrane for gas sweetening vantages, perfluoropolymer has the relatively expensive raw material
is manufactured by, for example, UOP (Separex), Natco (Cynara), and and thus considered to have high fabrication cost (Scholes et al., 2012).
Kvaerner (GMS) (Baker, 2002). This material is a glassy polymer that Recently, new classes of polymeric membranes have been developed
has been widely known to have remarkable CO2/CH4 selectivity and and tested for CO2 removal, i.e. thermally rearranged (TR) polymer and
thus has been used as a standard in the existing industry (Baker and polymers of intrinsic micro-porosity (PIM) membranes. As can be seen
Low, 2014). Cellulose acetate membranes normally have selectivity of in Fig. 3, these new types of membrane offer promising features for CO2
CO2/CH4 between 10 and 15 under normal operating conditions removal. TR membranes are glassy polymers, which are prepared by the
(Baker, 2002). In addition, cellulose acetate is considered to be rela- thermal treatment of polyimides at 350–450 °C (Rizzuto et al., 2017).
tively inexpensive as it uses cellulose as the raw material, which is an The improvement of the thermally treated polymeric membrane was
abundant and renewable resource. One of the major drawbacks of reported to be the results of chemical and structural change of the
cellulose acetate is plasticization, which would decrease the membrane polymer due to rearrangement and molecular transformation during the
permeability. This drawback is due to the high solubility of CO2 and thermal treatment (George et al., 2016). This transformation increases
H2S in cellulose acetate (Bernardo and Drioli, 2010). This problem is the free volume of the polymer matrix (Han et al., 2012; Kim et al.,
further discussed in Section 2.3 of this paper. Furthermore, cellulose 2013). During the thermal treatment, an evolution of interconnected
acetate membrane is also prone to acetylation, which is a hydroxyl micro-cavities occurs and micro-cavities with a narrow size distribution
group substitution on glucoside repeating unit by acetyl group that are formed (Rizzuto et al., 2017), hence the permeability of TR mem-
increases gas permeability with a decrease in selectivity (Scholes et al., brane increases with a slight change in their selectivity. In addition, the
2012). In order to address the limitations of this commercial type of TR membranes have improved resistance to CO2 plasticization
membrane, new various type of materials have been developed as the (AlQahtani and Mezghani, 2018; Smith et al., 2015). However, the
alternative material for MGS. thermal rearrangement can also result in decreased mechanical strength
The performance of several polymeric membranes has been pre- of the membrane (Liu et al., 2016; Scholes, 2016). Mechanical prop-
viously summarized by Zhang et al. (2013a,b). The authors noted that erties improvement of TR membranes has been conducted through
polyimide membranes are ideal for CO2/CH4 separation due to their various strategies, such as copolymerization (TR copolymers) and
good selectivity of CO2/CH4 and also good chemical and thermal sta- crosslinking (Calle et al., 2013; Li et al., 2013a,b; Scholes et al., 2014b,
bility. Polyimide belongs to glassy state polymer with a free volume in 2017). Even though the challenge of strengthening the mechanical
the range of 10–20% (Baker and Low, 2014). Cho and Park synthesized properties has been addressed, industrial trials are still needed to prove
2,6-diaminotriptycene-based polyimide membrane that has high in- the performance of TR membrane as the promising gas separation
ternal free volume elements. In the case of CO2/CH4 and CO2/N2 se- membrane (Scholes, 2016).
paration, the membrane showed both high permeability and selectivity, PIM is another new class of polymeric membrane that is expected to
174
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).
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
Fig. 4. Materials of MGS used for CO2 removal (based on publications indexed
by Scopus (TITLE (terms); January 9th, 2019). CA – cellulose acetate; MMM – (Yong et al., 2016).
mixed-matrix membrane; MOF – metal-organic framework; PI – polyimide; PSF Inorganic membranes have been used for CO2 separation, particu-
– polysulfone; PIM – polymers of intrinsic micro-porosity. 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,
surpass Robeson's upper bond for CO2 removal (Fig. 3). By definition,
such as DDR zeolite, SAPO-34 zeolite, and Zeolite-T, exhibited high
intrinsic micro-porosity is a continuous network of interconnected
selectivity and permeability for CO2/CH4 (Cui et al., 2004; Li et al.,
inter-molecular microcavities resulted from the contorted shape and
2006; Tomita et al., 2004) (Fig. 3). However, this type of membranes
chain rigidity of the polymer structure (Wang et al., 2016). The inter-
has limited applicability due to the high cost and low processability,
connected pores are less than 2 nm (Wang et al., 2016). PIMs are easy to
membrane poisoning that reduce the performance, and low perme-
be fabricated due to their high processability and solubility in the sol-
ability especially for dense inorganic membrane (Zhang et al., 2013a,b).
vent (Du et al., 2009a). PIM membrane exhibited high CO2 perme-
The fabrication cost of the module is around 3000 US$/m2, which is
ability as well as selectivity which make them as a potential candidate
much higher than the hollow fiber polymeric membrane (around 20 US
for gas separation membrane, especially in the case of CO2 removal or
175
$/m2) (Jusoh et al., 2016). In addition, zeolite membrane is also sig- CO2 separation from various gas mixtures (Deng et al., 2009; Huang
nificantly affected by impurities (e.g. water and H2S), which deterio- et al., 2008; Hussain, 2012; Quinn et al., 1997; Quinn and Laciak, 1997;
rates the membrane performance (Li et al., 2005). In addition to zeolite, Tong et al., 2015; Zhao et al., 2014). In FTMs, CO2 could selectively
the other inorganic materials that have been widely investigated for permeate through the membrane by means of a reversible reaction
CO2 separation are silica, metal organic frameworks (MOFs), carbon, between CO2 and a complexing agent-carrier incorporated in the
and amorphous metal oxide (Li et al., 2015a). membrane, whereas the other non-reacting gases such as H2, N2, and
Carbon membrane is a porous inorganic membrane that offers CH4 permeate exclusively by the solution–diffusion mechanism (Huang
higher permeability and selectivity in comparison with the available et al., 2008). Thus, both high CO2 selectivity and permeability could be
polymeric membrane (Ismail and David, 2001). The superior separation achieved. The carriers could be designed as a mobile carrier (e.g. sup-
performance is attributed to molecular sieving capability and ad- ported liquid membrane and ion-exchange membrane) or fixed carrier.
sorptivity owned by carbon membrane. In addition, carbon membranes Deng et al. (2009) developed a PVAm/PVA blend FTM, where the
have also been proven to be able to withstand high pressure (up to amino groups in the PVAm matrix facilitate the transport of CO2 and
70–200 bar) (Haider et al., 2018; Kruse et al., 2016; Vu et al., 2002), result in high CO2 permeance up to 0.58 m3(STP)/(m2 h bar) as well as
thus promising to be applied for carbon capture from natural gas. a high CO2/N2 separation factor up to 174. Numerous studies have
MOF is an emerging hybrid material, composing of metal ions as reported FTMs with different carriers for CO2 separation from CH4 and
coordination center, which are covalently bonded with organic linkers N2, however, more studies in the future need to address the perfor-
(Férey, 2008; Furukawa et al., 2013). This material possesses high mance of FTM at high pressure CO2/CH4 separation application and
porosity, high surface area, and high CO2 uptakes, making it as a pro- other harsh conditions of CO2 separation from flue gas (Rafiq et al.,
mising candidate for CO2 separation (Venna and Carreon, 2015). A 2016). It has been realized that FTMs are favorable to be used at low
number of studies have reported the development of MOF membrane CO2 partial pressures due to the carrier saturation phenomenon.
for CO2 separation, including the use of solvothermal growth method Moreover, membrane compression becomes another problem in high-
for MOF-5 membrane preparation (Zhao et al., 2013a,b), continuous pressure application. Combining FTMs in mixed matrix configuration
flow process for ZIF-8 membrane preparation (Marti et al., 2017), and then could be used to improve the stability at high pressures (Ansaloni
annealing post treatment of MOF membrane (Rui et al., 2018). It was et al., 2015; Tong and Ho, 2017; Zhao et al., 2014).
shown that the annealed membrane exhibited a remarkable improve-
ment in both CO2 permeance and CO2 selectivity over H2 (Rui et al., 2.2. State-of-the-art MGS for CO2 removal
2018). However, it is quite challenging to develop continuous MOF
membrane due to its poor intergrowth, low stability at high moisture The use of MGS for CO2 removal from natural gas has been applied
content, low reproducibility, and limited molecular sieving by the or- commercially from the 1980s and continually growing. It is estimated
ganic linker (Venna and Carreon, 2014). that the market in this area to be $220 million/year in 2020 (Baker,
Mixed matrix membranes (MMMs) are constructed from inorganic 2002). Commercial MGSs in this area are currently supplied by several
materials in the form of micro or nanoparticles dispersed in the con- companies including Medal (Air Liquid), W.R. Grace, Separex (now part
tinuous polymeric matrix. The key advantage of the MMMs is the mo- of UOP), Cynara (now part of Schlumberger), and ABB/MTR (Baker and
lecular sieving ability of the inorganic filler. In addition, the introduc- Lokhandwala, 2008). Essentially, all membranes currently used in
tion of filler into an organic membrane solution may induce the commercial applications are polymeric membranes mainly because of
formation of the asymmetric structure allowing a membrane with a thin their ease of manufacture. The use of cellulose acetate still dominates
skin layer supported by porous sub-layer. The asymmetric layer would the commercial membranes (such as UOP Separex™ and Schlumberger
provide a better separation performance. The performance of notable Cynara) nowadays, while the use of alternative materials has been
MMMs for CO2 removal is shown in Fig. 3. The major drawback of the continually increasing, such as polyimide (Air Liquide) and polysulfone
MMMs is the poor dispersibility of the inorganic particles within the (Air Products). These commercial membranes are typically fabricated
polymer matrix. The low distribution of the particles will lead to par- into hollow fiber and spiral wound module.
ticle aggregation, resulting in membrane defects. This will deteriorate Some of industrial-scale MGSs for CO2 removal are as follow (Baker
the overall performance of a MMM (Zhang et al., 2013a,b). Therefore, and Lokhandwala, 2008; Chen et al., 2018b; Sanders et al., 2013):
to produce an ideal MMM for gas separation, several parameters should
be considered/improved, such as polymer-inorganic filler pairs, adhe- (1) A gas separation membrane plant was installed in Texas in 1983
sion and interfacial contact between polymer and inorganic material, for CO2 removal by Cynara (now part of Schlumberger). The
the dispersion of inorganic filler in the polymer phase, particle size and membrane was originally designed to treat 48 MMscfd of natural
shape, and the loading of particles in the polymer (Jusoh et al., 2016). gas and to reduce CO2 concentration from 45% to 28%. The plant
Zeolite, alumina, silica nanoparticles, carbon nanotubes, graphene has been modified to double the capacity and to reduce CO2
oxide, and ZIFs have been widely used in MMM preparation for CO2 concentration from 80% to below 10%.
separation (Dilshad et al., 2019; Julian et al., 2019; Sarfraz and Ba- (2) In 1994, a CO2 removal plant was installed in Michigan, USA to
Shammakh, 2018; Vinoba et al., 2017). Dilshad et al. (2019) reported handle 40 MMscfd gas with 11% of CO2 concentration. The plant
that a high CO2/N2 separation performance surpassing Robeson upper uses spiral-wound cellulose acetate membrane from UOP. The
bound 2008 could be obtained when 6 wt% loading of alumina particles treated gas contains less than 2% of CO2 after passing through a
was used. Higher loading resulted in a decrease of gas permeation be- two-stage configuration that is designed to minimize methane
cause of particles aggregation blocking the path of the gas molecule. losses.
Hence, the number of inorganic particles incorporated need to be (3) In 1995, a gas separation membrane plant was installed in
controlled to achieve optimum permeation properties. Some recent Kadanwari (Pakistan) with 210 MMscfd of capacity. At the time, it
studies have shown that incorporating MOF significantly improved the was the largest plant of membrane-based natural gas processing.
performance of MMM in CO2/CH4 separation (Ahmad et al., 2018; Guo The plant uses UOP Separex ™ membrane (cellulose acetate). The
et al., 2018), but a major challenge still exists in the preparation of plant reduces CO2 content from 11% to below 3%. The second
MOF-based MMM for gas separation. Similar to other MMM synthesis, plant was installed with 234 MMscfd of capacity in Qadirpur. This
the major challenge is defect formation in the membrane matrix due to second plant is used to reduce CO2 content from 6.5% to below
poor compatibility of MOF particle-polymer matrix which may result in 2%. The capacity of Qadirpur Plant was upgraded to 500 MMscfd
a low selectivity (Zhang et al., 2016). in 2003 and then upgraded to 600 MMscfd in 2007.
Facilitated transport membranes (FTMs) have been developed for (4) In 1997, a membrane gas separation plant was installed in Mexico
176
using UOP's membrane for Enhanced Oil Recovery (EOR) appli- components (water, heavy hydrocarbon, and others) are removed in a
cation. The plant processes 120 MMscfd gas containing 70% of thermal swing regenerable adsorbent-based system. To recover any
CO2. The purified CO2 gas stream with a concentration of 93% adsorbent fines in the gas, a particle filter is used. Preheater is used to
CO2 is reinjected. The hydrocarbon product contains 5% of CO2. adjust the temperature of the gas. The regenerative system has some
(5) In 1999, UOP Separex™ membrane (cellulose acetate) was in- advantages, including (i) water and other contaminants (e.g. mercury):
stalled in two plants in Egypt, namely Salam (two units) and Tarek are removed along with heavy hydrocarbon, thus additional dehydra-
(one unit). Each unit is a two-stage membrane unit to treat 100 tion unit is unnecessary, (ii) mercury and mercaptans can be removed
MMscfd of natural gas from 6% CO2 to 3% CO2. The Salam Plant in the same bed, and (iii) it can be used in wide variation of the feed gas
was then expanded with 2 additional trains, which brings the total content.
capacity if Salam and Tarek Plants to 564 MMscfd. For CO2 removal from flue gas, the use of MGS is still not available
(6) In 2004, natural gas sweetening using a hollow fiber cellulose commercially and only applied in the research and development stage.
triacetate membrane from Cynara (now part of Schlumberger) was This is due to the challenges such as low partial pressure of CO2 in flue
installed in an offshore platform in the Thailand gulf (Cakerwala gas and a high temperature of the flue gas stream (Norahim et al.,
gas field). The plant capacity is 668 MMscfd. to reduce CO2 con- 2018). However, MGS may be ranked as the most promising technology
centration from 36% to 16%. The capacity has been doubled up to for CO2 removal from flue gas for certain applications/emission sources
1.28 Bscfd and it is currently the world's largest CO2 membrane and the great promise of metallic and ceramic membranes that are
plant for natural gas processing. capable of withstanding high temperature (Aaron and Tsouris, 2005).
(7) A natural gas processing plant using commercial polysulfone Hasan et al. (2012a,b) study the viability of three processes (absorption,
membrane from PRISM (Air Products) was installed in July 2004. membrane, and adsorption) to capture CO2 from various emission
The plant has a capacity of 8 MMscfd. CO2 in the natural gas sources (with the range of CO2 concentration in feed stream between 2
stream is reduced from 4.5% to 2%. and 70%-mole. It was reported that membrane is still less economically
(8) In 2006, a hybrid system was installed in Indonesia processing 245 attractive than absorption for heat and energy generation sector where
MMscfd of 40% CO2 gas down 20% in a UOP's membrane and then the feed gas contains less than 15–20% CO2 because the operating cost
down to 8% in a conventional amine solvent system. of the membrane-based process is higher than absorption-based pro-
(9) In 2007, a membrane gas separation plant was installed by UOP in cess. This is because the membrane-based process (at this feed con-
offshore Malaysia to process 680 MMscfd of gas from 45% CO2 to centration) requires a large feed compressor to provide sufficient
6% CO2. driving force of separation. However, the membrane was reported to be
(10) In 2008, a membrane gas separation plant was installed by UOP in the most economically attractive process to capture CO2 from industrial
offshore Thailand to process 530 MMscfd of gas from 34% CO2 to sources with a higher CO2 concentration in the flue gas (above 20
12% CO2. %-mole), such as cement, oil refinery, and steel plants. At this com-
(11) In 2013, built a biogas upgrading plant in Switzerland with a ca- position, the membrane-based process requires a smaller feed gas
pacity of 210 standard m3/year. The membrane is polyamide compressor (and hence lower cost), while the absorption-based process
hollow fiber. requires a higher operating cost because of the higher energy required
to regenerate the solvent. A study by Chung et al. further confirms this
There are several considerations in designing a membrane-based approach, where it was reported that the most economically attractive
CO2/CH4 separation system, which have been explained in detail by option to capture CO2 from a blast furnace in the steelmaking industry
Baker and Lokhandwala (2008). Pretreatment is typically required to is a hybrid of amine scrubbing and membrane with a heat recovery
avoid fouling, plasticization, and condensation of hydrocarbons on the system (Chung et al., 2018).
membrane. The exact pretreatment required depends on the membrane Several membrane design configurations have been proposed as
material and the feed gas characteristics (impurities, heavy compo- cost-effective options for this CO2 capture purpose. Merkel et al. (2010,
nents, operating conditions). The design configuration of membrane 2013) reported that they developed new membrane called Polaris™,
system could be designed in various ways, which depends on membrane which possesses modest selectivity but much higher CO2 permeance
selectivity and permeance, CO2 contents in the feed gas, pretreatment (10–50 times the commercial cellulose acetate membranes). This
facilities required, the value of the gas, and the location of the plant membrane was applied in a novel design process that possess a higher
(onshore or offshore). For example, one-stage membrane configuration driving force of separation than the conventional membrane design by
is typically preferred for a plant dealing with a small gas flow because utilizing the combustion air as a sweep gas. They also found that ap-
of its simplicity, not involving rotating equipment, and minimal plying vacuum in the permeate side will require less energy consump-
maintenance required. In some cases, a two-stage membrane system is tion than compressing in the feed side. Moreover, the former approach
used to reduce methane loss during processing. In this design, permeate will be the referred and cost-effective membrane design approach
from the first stage is recompressed and passed through the second especially if high permeance membranes (> 4000 gpu) or cheap
stage. By doing so, the methane loss could be reduced to a few percent. membrane cost (< $50/m2) are developed (Merkel et al., 2010). A
A combination of one-stage and two-stage membrane systems is useful study by Scholes et al. proposed an alternate design to further improve
for treating a high concentration gas. the performance, where an additional air separation unit is installed to
Koch et al. (2005) from UOP reported two types of pretreatment enrich the O2 in the sweep gas for combustion. This leads to a higher
systems for gas separation membrane in the CO2 removal process. The CO2 concentration in the feed gas, which results in low parasitic load
first pretreatment system is called traditional pretreatment, which (30%) (Scholes et al., 2013).
consists of: (i) coalescing filter for the removal of liquid and mist from Han and Ho. (2018) reported that PEO-based membranes and
the feed stream, (ii) non-regenerable adsorbent bed for removing trace amine-based facilitated transport membrane are currently the only
contaminants, (iii) particle filter for dust or particulates removal, and feasible materials for CO2 removal for both post-combustion and pre-
(iv) heater for heating the gas to superheated condition. This traditional combustion schemes. This material provides a minimal CO2/N2 se-
pretreatment is sufficient for treating gasses with light and stable lectivity of 50 and high permeance (up to 3000 gpu). These membrane
compositions. However, adsorbent bed is the only item removing heavy materials are also suitable for pre-combustion CO2 capture because of
hydrocarbon compounds in this configuration and hence it may only be high CO2/H2 selectivity and good stability at high pressure (> 100 °C)
limited for some applications. The second pretreatment is called as a in the presence of H2S.
regenerative pretreatment. In this pretreatment, liquid or entrained
particles are removed in a filter-coalescer. Then, other harmful
177
2.3. Main challenges in MGS for CO2 removal the thickness of the materials, CO2 pressure, exposure time, aging time,
and the prior preparation/storage/thermal treatment history (Dai et al.,
In designing MGS for CO2 separation system, it is desired to get high 2016a). In the case of membrane material, the plasticization pressures
permeability and selectivity. High CO2 permeability is desired to reduce of several membranes have been identified. The plasticization pressures
the required membrane area and the operating pressure thus reducing of other materials are shown in Fig. 6.
the total processing cost. Meanwhile, a high selectivity membrane re- Many efforts have been devoted to overcoming this problem by
duces the membrane area (or stage) and it increases the product re- modifying the polymeric membrane, such as by thermal rearrangement,
covery. In the case of CO2/CH4 separation, a high selectivity membrane polymer cross-linking, and polymer blending (Zhang et al., 2013a,b).
is also important to reduce the loss of CH4 during the process. CH4 loss By using those modification methods, plasticization could be reduced
is one of the important parameters determining the overall processing while the membrane performance could be improved. The improve-
cost. For example, a membrane with a selectivity (CO2/CH4) of 35 has ment of thermally modified membrane was reported as the result of the
been investigated by Peters et al. for natural gas upgrading (Peters arrangement of the fractional free volume of the membrane (Han et al.,
et al., 2011). Results of the simulation showed that about 9.5% of CH4 2010). Thermal annealing of the Matrimide membrane, for example,
loss (feed gas: 9.5 mol-% of CO2; 72.4 mol-% of CH4; and other gases i.e. has been developed to suppress plasticization of this type of polyimide
ethane, propane, butane, pentane, and hexane) was observed in a single membrane (Dai et al., 2016a). Cross-linking may result in the change in
stage membrane processing while only 0.47% of CH4 loss was observed the chemical structure of the polymers, and so consequently changing
in a 2-stage process. Even though the 2-stage process exhibited a lower the mobility of the chains. When a membrane is modified via cross-
total processing cost, this cost could be further reduced if the selectivity linking, the molecular free volume between the polymer chain increases
of the membrane is improved. after modification (Zhang et al., 2013a,b). An example of the cross-
The main drawbacks of the polymeric membrane used for gas se- linking process in order to obtain higher rigidity and improved anti-
paration are a trade-off between permeability and selectivity, and the plasticization is the cross-linked polyimide. The cross-linking process
phenomena of plasticization and aging. Another challenge in the de- can be done by thermal, UV, and chemical treatments. Diol cross-
velopment of the MGS is the limited report on the selectivity of the linking polyimides, which contain carboxylic acid groups, have been
membrane material in the CO2-methane mixture measurements (Baker widely studied for this purpose (Baker and Low, 2014).
and Low, 2014). Most reported performances of the developed mem- Physical aging is another significant hurdle for the application of
branes were based on the pure-gas measurements. Some novel materials glassy polymeric membrane in gas separation. Physical aging is asso-
have been found to show pure-gas selectivity of 50 or more, yet cellu- ciated with the change of free volume or macro void inside the mem-
lose acetate (with mixed gas selectivity of 10–15) remains as the in- brane matrix (Adewole et al., 2013; Sanders et al., 2013). This is the
stalled material in natural gas processing plants. It has been reported result of the segmental motion of the polymer, which gradually in-
that most materials may lose their selectivity performance when tested creases the density of the polymer. The permeability of the membrane
with mixed gas at the high natural gas processing pressures. declines along with the increase of membrane selectivity because the
The permeability of the membrane has an inverse relationship with free volume decreases (Fig. 5). This phenomenon could be observed by
the selectivity, wherein the increase of permeability results in the de- the declining membrane flux over time. The mechanism of the rapid
crease of selectivity and vice versa. This characteristic has been studied physical aging that occurs in the thin film membranes has not been fully
by Robeson, which is known as Robeson's upper bond (Robeson, 2008, understood yet. However, previous studies have reported several key
1991). Only a few of membrane materials can across this upper bond. variables that affect the physical aging behavior of the thin film
Therefore, in order to achieve a significant process performance im- membranes, which are membrane thickness (thinner membranes may
provement, it is essential to characterize and develop membranes that have high physical aging rate), membrane preparation/storage history,
could across this upper bound (high permeability and selectivity). In and membrane operation temperature/pressure and storage atmo-
terms of CO2/CH4 upper bound relationship, Robeson classified the sphere (Dai et al., 2016a). Strategies to solve the physical aging can be
thermally rearranged polymers, which contain benzoxazole-phenylene classified as two different approaches, (i) by freezing the initial free
or benzothiazole-phenylene structures (Park et al., 2007b), as materials volume state in place (e.g. hybrid material, polymer blending) and (ii)
with remarkable separation performance. This Robeson's upper bound by using a cross-linking agent to increase the structure rigidity
has now been widely used as a standard for the membrane development (Amooghin et al., 2016). For example, an effort to suppress physical
as it shows the superiority of the transport and separation character- aging of super glassy polymer for gas separation has been reported by
istics of fabricated membranes (Adewole et al., 2013). Lau et al. (Amooghin et al., 2016). Three types of polymeric membrane,
Plasticization is another main concern in the application of poly- i.e. poly(trime-thylsilylpropyne) (PTMSP), poly(4-methyl-2-pentyne)
meric membrane for CO2 removal, as membrane typically becomes (PMP), and PIM-1 were modified with the addition of ultraporous ad-
swollen when it is exposed to CO2 and hydrocarbon compounds, par- ditive, porous aromatic framework (PAF). Long-term performance test
ticularly at high pressures. Bos et al. reported a study on CO2-induced (1 year) indicated that the modification could successfully inhibit the
plasticization-in various glassy polymers and defined this phenomenon physical aging of those membranes whilst retaining the improved CO2
as the increase in CO2 permeability as a function of feed pressure (Bos permeability and high CO2/N2 selectivity. A new approach for produ-
et al., 1999). This plasticization results in an increase of permeability of cing an anti-aging of MMM for CO2 removal has been reported by
CO2 with the increasing pressure while the selectivity is reduced. In Kitchin et al. (HonáLau, 2015). The so-called anti-aging intercalating
addition, membranes may be irreparably damaged due to plasticization. membrane (AIM) was prepared by introducing soluble metal-organic
Plasticization pressure is usually used as an indicator to evaluate polyhedral (MOP) with various organic chain lengths. The use of MOP
polymeric material for CO2 removal. Plasticization pressure is the was reported as an effective way to reduce the aging rate (up to three
minimum pressure that is required to induce the increase in perme- times). The introduction of MOP allowed a better mixing with poly-
ability (Dai et al., 2016a) (Fig. 5). At plasticization pressure, the per- meric membrane eliminating non-selective void which usually found in
formance of a membrane starts to decrease, which leads to an increase a traditional MMM.
in methane loss and thus negatively impact the economics (Wind et al., Generally, there are a number of impurities present in a natural gas
2004). Sanders et al. (2013) described two common indicators of stream that could reduce the performance of the membrane or even
plasticization, which are: 1) increase in gas permeability as the function induce membrane damage. A moisture content could cause mechanical
of upstream gas partial pressure and 2) a loss in membrane selectivity damage of the membrane, while heavy hydrocarbons could form a film
when the upstream total pressure (or partial pressure of one or more on the membrane surface which reduces the permeability (George et al.,
components) increases. It has been found that plasticization depends on 2016). In addition, liquid or condensation should be avoided because it
178
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 2009; Nishikawa et al., 1995). Microporous PP membranes are in-
on PVAm/PVA blend composite membrane performance has been re- expensive, but they are less hydrophobic than membranes from
ported (Uddin and Hägg, 2012). They reported that the performance of fluorine-containing polymer (such as PTFE and PVDF). Microporous
membrane and the effect of impurities such as hydrogen sulfide, n- PVDF membranes could be a good candidate for the development of MC
hexane, and propane, are significantly affected by water (humidity). as they are cheaper and easier to fabricate than PTFE.
The maximum loss of CO2 permeance and CO2/CH4 were about 18% In addition to the high hydrophobicity, membranes used in MC
and 16%, respectively, at high humidity. Therefore, the feed gas stream should also have good thermal stability, excellent chemical stability,
should undergo a stringent pretreatment to avoid a significant loss of and high porosity. It was reported that the use of polymers with high
membrane performance. The detail on design and pre-treatment of melting temperature (Tm), such as PTFE and polyether ether ketone
MGS, especially for natural gas processing, has been reported in pre- (PEEK), with Tm of 327 °C and 335 °C, respectively, can be a good
vious works (Baker, 2002; Baker and Lokhandwala, 2008). 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.
3. Membrane contactor (MC) However, it can also give impact on membrane wetting, as reported by
Rajabzadeh et al. (2013), where a highly porous membrane with large
Schematic of MC process is illustrated in Fig. 2 b. In MC, the porous pore diameter was completely wetted and the CO2 absorption flux de-
membrane acts as a support to provide extra area for contact between creased drastically after 100 h.
two phases, and hence it promotes the mass transfer (Purwasasmita Apart from the membrane selection, absorbent type and operating
et al., 2015b). The membrane is expected to provide non-dispersive and parameters are also important factors determining the MC performance.
better contacting process between the gas and the solvent, while the In this regard, a number of experiments, modeling, and simulations
CO2 selectivity is dominated by the solvent. Ideally, MC is operated in have been carried out (Mansourizadeh et al., 2010; Zhang et al., 2019;
non-wetted mode, of which the membrane pores are filled only with the Zhang, 2016). A recent study reported that the absorbent concentration
gas phase. The penetration of the absorbent liquid into membrane pores had the greatest effect on the efficiency of CO2 absorption, followed by
should be prevented so that a low mass transfer resistance can be gas velocity and liquid (absorbent) velocity (Zhang et al., 2019). This
achieved as the gas–liquid interface in the pore mouth is maintained. was associated with the increase in chemical reaction rate between the
For this purpose, microporous membranes from polymers with a high CO2 and the absorbent. A high chemical reaction rate can also be ob-
hydrophobicity such as polytetrafluoroethylene (PTFE), poly- tained by selecting a suitable chemical absorbent. Having CO2 reaction
vinylidenefluoride (PVDF), and polypropylene (PP) are commonly rate constant, piperazine (PZ) has gained great attention to be used as
used. Among these materials, microporous PTFE membranes are the the single absorbent or to be blended with the other alkanolamine ab-
most hydrophobic and they offer good and stable performance, but the sorbent (Zhang et al., 2018b; Zhang, 2016).
materials are very expensive (DeMontigny et al., 2006; Khaisri et al.,
179
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
membrane surface roughening using nanoparticles such as TiO2 dense skin layer should also have high hydrophobicity in addition to the
(Razmjou et al., 2012), silver (Liao et al., 2013a), and silica (Fang et al., high CO2 permeability so that it would be more effective for CO2 re-
2012; Park et al., 2016) followed by hydrophobization using fluor- moval application (Scholes et al., 2015). Aside from wetting preven-
osilane compounds are the most reported. tion, another advantage by placing the dense skin layer on the porous
Most inorganic membranes which are hydrophilic in nature require support is the ability for selective mass transfer. Belaissaou et al. (2016)
surface modification to alter its surface nature from hydrophilic to su- used dense skin MC for biogas purification. In addition to giving mass
perhydrophobic. Some studies have modified ceramic membranes sur- transfer performance that is comparable to microporous MC, the poly
face by grafting method using fluoroalkyl silane (FAS) compounds (phenylene oxide)-based dense skin MC could reduce the loss of me-
(Abdulhameed et al., 2017; An et al., 2015; Lu et al., 2009; Yu et al., thane.
2015). During the grafting process, the hydroxyl (–OH) groups on the
surface of pristine ceramic membrane react with Si–O–alkyl groups of 3.2. State-of-the-art of MC for CO2 removal
the silane (Picard et al., 2001). The grafting efficiency is strongly in-
fluenced by the length of FAS chains, grafting time, and multiplicity of Considerable studies on the MC application for CO2 removal from
grafting (Kujawa et al., 2014; Lu et al., 2009). Using appropriate various gas streams have been conducted, even though only a few of
parameters, superhydrophobic ceramic membranes have been suc- them have been tested in pilot or larger scale. In this regard, two major
cessfully prepared (Lu et al., 2009; Yu et al., 2015). The super- applications of MC for CO2 removal are post-combustion carbon cap-
hydrophobic ceramic membranes are highly potential to be applied in ture and CO2 removal from natural gas (Sreedhar et al., 2017; Zhao
membrane contactor for carbon capture at high temperature. et al., 2016). The following section discusses the development of MC
A number of studies on the use of superhydrophobic membranes for technology.
CO2 absorption have shown that superhydrophobic membranes out- MC technology was early developed by Kvaerner Process Systems
performed membranes without superhydrophobicity (Abdulhameed (KPS) together with W.L. Gore & Associates GmbH (GORE), SGL Carbon
et al., 2017; Ahmad et al., 2013a; Franco et al., 2012; Lin et al., 2016; Group (SGL) and Ottestad Breathing Systems (OBS) for CO2 removal
Lv et al., 2012a). The superhydrophobic membranes showed higher from gas turbines on off-shore oil and gas platforms in Norway in 1992
CO2 absorption flux and more stable flux over long periods. For in- (Zhao et al., 2016). Between 1998 and 2001, the trials were performed
stance, superhydrophobic nanofibrous membrane prepared by electro- in a large pilot scale. The MC showed a CO2 capture efficiency of 85%
spinning and FAS modification showed a stable CO2 absorption flux of with the exhaust gas flow rate was 2610 kg/h. From 1998 to 1999, pilot
approximately 1.5 mmol/m2.s for four days of operation, which was in tests of MC were also performed for natural gas treatment (Herzog and
contrast with the unmodified nanofibrous membrane showing a dra- Falk-Pedersen, 2000). Pilot tests with the longest operation of 5000 h
matic decrease in CO2 absorption flux even in the first 100 min (Lin were held at a gas terminal in Scotland, in which activated MDEA was
et al., 2016). The high performance is attributed to anti-wetting beha- used as the absorbent. In addition, a physical solvent was also used in
vior of the superhydrophobic membranes, preventing penetration of pilot tests held at the Shell Fandango field in Texas. TNO, the Nether-
liquid absorbent into membrane pores (Franco et al., 2011; Himma lands Organization for Applied Scientific Research, has long been de-
et al., 2018, 2019; Himma and Wenten, 2017; Lu et al., 2008). veloping CO2 membrane gas absorption. Its application for CO2 removal
from flue gas and reuse in the horticultural industry has been reported,
3.1.2. Non-porous composite membrane in which a significant reduction in the CO2 production cost could be
Apart from porous MCs with a superhydrophobicity, recent re- achieved by using the MC (Feron and Jansen, 1995). In 1997, the
searches focus more on the development of non-porous MCs. It is ex- project was developed in a pilot plant, at which the carbon dioxide and
pected that the non-porous MCs provides a much more stable perfor- heat supply were combined to greenhouses (Feron and Jansen, 1997).
mance compared to porous MCs, especially in terms of wetting. The Gas Technology Institute (GTI) in the United States (US) have de-
membrane used in non-porous MC can be an integrally dense mem- veloped MC technology (called Carbo-Lock™) for CO2 capture with
brane, skinned asymmetric membrane, or composite membrane con- PEEK membrane since 2010 (Zhao et al., 2016). The super-
sisting of a thin dense layer coated on a porous support. The integrally hydrophobized PEEK membrane maintained its high performance in the
dense membrane logically imposes higher resistance to mass transfer presence of flue gas contaminants (such as O2, NO2, and SO2) and stable
than skinned asymmetric membrane or composite membrane. The use performance with CO2 capture efficiency of above 90% was achieved in
of non-porous composite membrane was then most widely reported. an absorption test for ∼120 h (Shiguang Li et al., 2013a,b).
In a non-porous composite membrane, the dense skin layer imposes Researchers in Cooperative Research Center for Greenhouse Gas
an additional mass transfer resistance, thus polymers with high CO2 Technologies (CO2CRC), Australia, reported pilot plant trials of porous
permeability such as PTMSP (Dibrov et al., 2014; Nguyen et al., 2011; MC (PP and PTFE) and nonporous MC (polydimethylsiloxane, PDMS)
Scholes et al., 2015) and PIM-1 (Scholes et al., 2015) is preferentially for post-combustion CO2 separation (Scholes et al., 2014a). The PP
used as its material. In addition, polymers with less permeability but membrane experienced significant wetting in both laboratory and pilot
has very high hydrophobicity such Teflon AF 1600 (Scholes et al., plant tests, whereas the PTFE membrane experienced wetting when
2015) and Teflon AF 2400 (Dai et al., 2016c; Nguyen et al., 2011) have tested in pilot plant. The PDMS MC did not experience wetting, but it
also been investigated for its use as the dense skin layer material. had the lowest overall mass transfer coefficient among other materials
Nguyen et al. (2011) have prepared composite hollow fiber membranes testes, which was lower than PP MC in two orders of magnitude both in
based on a thin dense skin, based on Teflon-AF and PTMSP, coated on laboratory and pilot scale performance tests.
microporous support (PP). It was demonstrated that the Teflon-AF A study by Vericella et al. (2015) proposed a novel approach called
composite membrane showed CO2 capture ratio (as a function of gas encapsulated solvent to combine the use of membrane and solvent
velocity) similar to the microporous PP membrane. With the addition of absorption to capture CO2 from flue gas. The solvent is encapsulated in
dense skin thickness of 1.1 μm, the Teflon-AF composite membrane a thin membrane capsule with a diameter of 100–600 μm and thickness
exhibited the lowest reduction in the mass transfer coefficient of about of 10 μm. This concept combines the benefit of both technologies,
15%. Moreover, an investigation over long time scales, i.e. over 1000 h where the solvent selectively reacts with CO2 (not with N2) in a high
showed that dense skin composite membranes based on PMP/PP and surface area contactor provided by the silicone-based membrane cap-
Teflon-AF/PP exhibited CO2 flux density comparable to PTFE and sig- sule (Vericella et al., 2015). This results in smaller contactor dimensions
nificantly higher than PP after 500 h (Chabanon et al., 2011). These required compared to conventional absorber This is beneficial the
studies proved that a dense skin composite MC could provide both permeability and selectivity of the system can be independently mod-
wetting prevention characteristics and high mass transfer of CO2. The ified, which is different to conventional MGS where permeability and
181
selectivity are usually competing parameters. This novel design has membrane, which may be caused by the surface tension of the solvents.
been tested at lab-scale and pilot scale (1 MWe coal testing facility at This deformation of microfibrils was followed by adhesion of adjacent
the DOE National Carbon Capture Center) (Hornbostel et al., 2019). microfibrils. Membrane-solvent compatibility for CO2 removal appli-
Using their expected capsule properties and N2CO3 30%-wt. as working cations using MC was also investigated by Dindore et al. (2004). Five
solvent, the absorber height required and the energy penalty are ap- types membrane material i.e. PTFE, PP, PVDF, PES, and PS, and eight
proximately 10% and 18% lower, respectively, than the conventional types of solvent i.e. water, propylene carbonate, selexol, N-methyl
MEA-absorber system. In order to be economically competitive (com- pyrrolidone, dimethyl formamide, tributyl phosphate, glycerol triace-
pared to conventional absorber), it was reported that the capsule tate, and n-formyl morpholine were used in their study. It was reported
thickness needs to be reduced by up to an order of magnitude without that only PTFE and PP were compatible with the organic solvents while
adversely affecting the capsule stability and integrity (Raksajati et al., the others were incompatible in terms of morphological damage,
2018, 2017). shrinkage, dissolution, swelling, and color changes. The authors found
A number of studies on MC that were close to real conditions of CO2 that PTFE and PP in combination with propylene carbonate were the
separation from natural gas have also been carried out. Al-Marzouqi most promising membrane-solvent pairs for CO2 absorption. Further-
et al. (2017) have reported the long-term operational stability of PFA more, with regard to the membrane fabrication cost, PP-propylene
hollow fibers MC in simultaneous CO2 and H2S removal from a gas carbonate was considered as the most promising candidate.
stream whose composition was similar to natural gas at a high pressure The membrane wetting becomes a major concern in MC since it
of 50 bar using hot absorbent at a temperature of 100 °C. High pressure highly determines the long-term performance of the membrane. Partial
MCs were also reported in other works (Kang et al., 2017; Marzouk wetting can still occur although the membrane used is intensive hy-
et al., 2012, 2010). Modeling and simulation of MC for natural gas drophobic (Chabanon et al., 2011; Lu et al., 2008; Zhang et al.,
sweetening have also been conducted (Quek et al., 2018; Rezakazemi 2008a,b), which then increasing the membrane resistance (Rangwala,
et al., 2011), providing important insights for the design and operation 1996; Zhang et al., 2008a,b) (Fig. 7). This situation may result in a
aspects. significant drop CO2 (Lv et al., 2012b). Wetting phenomena in MC and
MC has also been widely developed for CO2 separation from re- its prevention have been widely investigated -(Goyal et al., 2015; Lv
newable resources such as biogas. A pilot-scale MC based on nonporous et al., 2010; Malek et al., 1997; Mosadegh-Sedghi et al., 2014; Zhang
PVTMS membrane for biogas conditioning has been constructed and et al., 2008a,b). Various approaches have been made to prevent the
tested by researchers from Topchiev Institute of Petrochemical membrane wetting, including optimization of operating condition
Synthesis, Russian Academy of Sciences in collaboration with NPK (Simons et al., 2009; Yan et al., 2007), solvent and membrane selection
BIOTEST (Shalygin et al., 2011). The test results suggested that con- (Albrecht et al., 2005; DeMontigny et al., 2006; Dindore et al., 2004;
trolling absorbent flow is very important for dealing with varying Yan et al., 2007), and membrane development by controlling the
biogas compositions and flow. Considerable efforts in developing MCs membrane pore structure (Nguyen et al., 2011; Rajabzadeh et al., 2013)
for biogas upgrading were also reported by Park et al. (2017) proposing and the membrane surface properties, in particular, towards super-
MC with pressure-cascaded stripping configuration and Schiavon Maia hydrophobicity (Bakeri et al., 2012; Franco et al., 2012; Lin et al., 2016;
et al. (2017) conducting bench-scale and pilot test of MC for H2S and Rahbari-Sisakht et al., 2012b; Yu et al., 2015). Among these, the two
CO2 removal from biogas using a regenerable Fe-EDTA solution. latter strategies have gained great attention recently due to the pro-
mising high performances as discussed in the previous section. How-
3.3. Challenges in MC ever, for further development of CO2 absorption membrane, the chal-
lenges are how their durability in operation at high pressures and
For MC, the solvent must be selected carefully in order to achieve a temperatures and in the presence of contaminants such as SO2. This is
high separation performance. Generally, the solvent should have a high necessary to be investigated in the development of superhydrophobic
absorption capacity for CO2 and should also be compatible with the MCs as well as non-porous MCs.
type of membrane used in MC. It is important to consider solvent- One of the major drawbacks which is usually faced in membrane
membrane compatibility since the solvent may react with the polymeric operation is fouling (Ariono et al., 2017; Kang and Cao, 2012;
membrane, which could result in membrane degradation (Luis et al., Khoiruddin et al., 2017; Rana and Matsuura, 2010; Wenten and
2012). The solvent-membrane pair should be carefully selected to avoid Khoiruddin, 2016). Fouling phenomena generally reduce the mem-
the damage of the membrane, both physically and chemically. The brane flux (either temporarily or permanently) which seriously ham-
change of membrane properties, when exposed to sorbent, has been pering the applications of membrane processes (Aryanti et al., 2017;
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 Fig. 7. Schematic illustration of membrane hydrophobicity and CO2 flux in MC
was due to the deformation of microfibrils of the hollow fiber as a function of operation time.
182
Khoiruddin et al., 2014; Rana and Matsuura, 2010; Sianipar et al., concentration of the CO2 is higher, the driving force for the separation
2017). Membrane fouling is another challenge in MC, even though the will be increased, which is beneficial for MGS. However, it should be
adverse impact on the performance of MC is less significant compared noted that, as the CO2 concentration increases, the membrane will be
to the impact of membrane wetting. Fouling in MC is reported to be not more susceptible to plasticization (Bos et al., 1999). If MGS is used for
as severe as that of membrane filtration. However, in industrial appli- treating a feed gas with a low CO2 concentration, the driving force will
cations where the flue gas stream contains contaminants such as dust or reduce and a significant amount of valuable gas (product or CH4 loss in
suspended particles, the membrane fouling becomes a bigger concern. case of CO2/CH4) is lost. As a consequence, the performance of MGS can
Zhang et al. (2015) reported that the existence of fine particles in flue decline and the processing cost may increase. In term of energy con-
gas from coal-fired desulphurized power plant decreased the efficiency sumption, MGS required a relatively high energy consumption than MC,
of CO2 removal due to the deposition and adsorption of fine particles on which associated with the use of a dense membrane and the high op-
the surface and pores of the microporous membrane. In order to avoid erating pressure.
membrane fouling, the contaminants should be removed in the flue gas MC could provide very high selectivity and it can be used to treat
pre-treatment facilities. Alternatively, the use of membrane with anti- feed gas stream with a low concentration of CO2 effectively (Klaassen
fouling properties or self-cleaning ability can be used to prevent such et al., 2008). Unlike MGS, MC has a very high selectivity so that it could
problem without requiring pre-treatment facilities. It has been reported be applied in a wide range of gas flow rate and concentration without
that superhydrophobic surface also has the self-cleaning ability any loss of product gas. The high selectivity is provided by the chemical
(Bhushan et al., 2009; Xue et al., 2010). In membrane application, the or physical interaction between the gas and the absorbent. MC is
self-cleaning property of superhydrophobic membrane makes foulants usually operated under low operating pressure so the operating cost
are easy to be released from the membrane surface (Himma et al., 2016; will be lower than MGS. Despite the advantages, MC also has several
Himma et al., 2018, 2019; Zhao et al., 2013a,b). Therefore, the use of disadvantages, such as wetting phenomenon, fouling, and membrane
superhydrophobic membrane could mitigate the membrane fouling in degradation, as have been discussed in the previous sections. Other
MC. A study by Yu et al. (2015) showed that superhydrophobic ceramic disadvantages, which should also be considered, are as follow
membrane displayed a better anti-fouling property compared to the PP (Mansourizadeh and Ismail, 2009):
membrane without superhydrophobicity. The ceramic membrane sur-
face is not covered by dust even after being operated for treating flue - The membrane used in MC becomes another transport resistance
gas for one-month operation. because it could reduce the overall mass transfer and reduce the
selectivity. This resistance will be more pronounced if the mem-
4. Comparison of MGS and MC for carbon capture brane becomes wetted.
- Non-uniform hollow fiber distribution in the membrane module can
In CO2 removal applications, MGS and MC have their own ad- lead to channeling and bypassing which can reduce mass transfer
vantages and disadvantages. The comparison of both membrane-based efficiency. Therefore, the flow configuration and module geometry
processes is listed in Table 2. With regard to the status of commercia- should be considered.
lization, MGS has been commercialized and applied on a large scale - Operating conditions can significantly affect the performance of MC.
particularly for natural gas sweetening (see Section 2.2) competing with Temperature, pressure, and flow rates, both gas and solvent or li-
amine-based absorption system. quid streams, should be carefully controlled to (i) avoid gas bubble
The effect of gas flow rate and CO2 concentration in feed gas stream formation which could result in gas loss, (ii) avoid wetting by the
on the choice of CO2 removal methods from natural gas were illustrated solvent, and (iii) simultaneously increase residence time and gas
schematically by Baker and Lokhandwala (2008). According to the plot, absorption.
MGS is favorable when the gas stream contains relatively high CO2
concentration (up to 40 mol%) and a low gas flow rate (< 10 MMscfd). Generally, MC uses organic solvent such as amine solution for CO2
On the other hand, an amine-based absorption system is preferable for removal applications. Despite the high selectivity provided by the sol-
feed gas stream with a low concentration of CO2 (∼2–25 mol%) and vent, the use of this type of organic solvent also has several drawbacks.
high gas flow rate (up to 500 MMscfd). Meanwhile, for feed gas stream Amine solution has high vapor pressure, is corrosive, and needs high-
with high CO2 concentration and flow rate, a combination of MGS and energy for regeneration (Babamohammadi et al., 2015). Recently, a
amine is preferable. One of the important features of MGS is that it does new type of absorbent, ionic liquid (IL), has attracted researchers to
not require solvent, therefore it does not require chemical regeneration, apply it in MC for carbon capture. An IL is a salt which has a melting
solvent make up, and another associated handling. Since the separation point below 100 °C and is composed of an organic cation and an organic
is not dependent on the chemical sorbent, the use of MGS for separation or inorganic anion (Dai et al., 2016b). The interesting features of IL are
of high concentration is more economical than amine-based absorption high CO2 solubility, high selectivity, low vapor pressure, and high
(in certain feed gas characteristics). Furthermore, when the thermal stability (Dai et al., 2016b; Karadas et al., 2010). With those
Table 2
Comparison of membrane gas separation vs. membrane contactor for CO2 removal from natural gas.
Parameter MGS MC Ref.
Typical membrane used Dense Porous (Bernardo et al., 2009; Li and Chen, 2005;
Zhang et al., 2013a,b)
Solvent None Needed
Selectivity Determined by the membrane (20–50) Determined by the solvent (> 1000) (Li et al., 2013a,b)
Pre-treatment for impurities removal Highly required (Baker and Lokhandwala, Required
2008)
Energy consumption Normal to high Low Zhang et al. (2013a,b)
Cost Normal to high Low Zhang et al. (2013a,b)
Drawbacks ➢ Plasticization (polymeric-based membrane); ➢ Wetting phenomenon; (Luis et al., 2012, 2011; Wang et al., 2016)
➢ The trade-off between permeability and ➢ Fouling;
selectivity; ➢ Membrane degradation;
➢ Physical aging;
183
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
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
requirement. transfer rate. However, the membrane will be more susceptible to

Compared to MGS, economic analysis of MC for carbon capture can plasticization. In addition, the loss of CH4 during the process is in-
hardly be found in the literature. Comparison of MC and conventional evitable. Therefore, in this case, MC would be an interesting alternative
amines system for CO2 capture from flue gas has been conducted by Yan process. Generally, the feed gas from the field has high pressure that
et al. (2008), where the performance and economic of the processes allows the use of physical absorption for CO2 removal (see section 4.3).
were investigated. According to their result, the performance and gas The absorption of CO2 can be performed in MC using water such as
processing cost of MC were significantly affected by the wetting phe- from seawater as the solvent or absorbent. The use of water from sea-
nomenon. MC exhibited a larger overall mass transfer coefficient, about water could potentially reduce the cost of CO2 capture due to its large
2.9 times, than the conventional amine system when a fresh membrane resource (and inexpensive), even when a high flow rate of gas should be
was utilized. As a result, the gas processing cost of MC was lower than handled and a large volume of absorbent is required (due to the high
MGS (Table 4). However, the superiority of MC could not be maintained concentration of CO2). In addition, the use of water instead of alka-
when half of the membrane pores was wetted. When the membrane was nolamine solutions can reduce the tendency of membrane wetting (for
wetted, a considerable reduction of the overall mass transfer was ob- hydrophobic and superhydrophobic membranes) because it has high
served. Therefore, to keep the superiority of MC, this wetting phe- surface tension. Since the absorbent has high CO2 concentration and
nomenon should be addressed. From the economic analysis, it was still has high pressure, it could be directly injected into a nearby oil well
found that the capital investment and CO2 capture cost of MC were for pressure maintenance that it is beneficial for enhancing oil pro-
significantly influenced by membrane price and lifetime, and the SO2 duction. Another benefit from this scheme is carbon credit obtained
concentration in the feed gas stream. If the lifetime of the membrane from the carbon storage. As the overall result, a cost involved in gen-
was less than the critical value, the cost of CO2 capture of the MC would erating high-pressure water in the absorption process would be ac-
be higher than the amine plant system. commodated by the benefits of the carbon storage. By using the pro-
The study of Yan et al. (2008) indicated that the carbon capture posed scheme, the processing of a gas stream with a very high CO2
from flue gas stream using MC had lower CO2 capture cost than MGS concentration may make sense economically.
reported by several studies. This may be associated with the high se-
lectivity, high mass transfer of porous membrane, the low operating 5. Conclusion and perspectives
pressure of MC, and lower membrane cost. Nevertheless, MC also has
several disadvantages (see section 4.2) that should be addressed for its In recent years, there have been increasing efforts in reducing CO2
industrial applications. In the case of MGS, the major challenge for flue emissions, including energy efficiency improvement, implementation of
gas treatment is the scale of the process, which is associated with the low/no fossil carbon, and carbon capture & storage (CCS) as well as
large volume of the gas stream and the low CO2 concentration (Luis geo-engineering. Among these, CCS is likely to become an attractive
et al., 2012). It will particularly affect the separation performance of and efficient way of mitigating CO2 emissions since it requires
MGS (mass transfer rate and selectivity) and the required membrane minimum fundamental changes in the existing design, production, and
area. Even though the driving force of MGS can be improved using products schemes. For CO2 capture, solvent absorption is currently the
several strategies, such as by increasing feed pressure, recirculating an well-established technology and the most promising methods in the
enriched CO2 stream, decreasing the permeate pressure, and reducing near future due to the high selectivity and capacity, as well as simplicity
CO2 concentration in the permeate pressure via a sweep gas, those will in the regeneration of solvents. However, absorption has some dis-
require an additional energy consumption and extra cost (Luis et al., advantages related to regeneration energy, limited mass transfer area
2012). Favre has pointed out several aspects that should be taken into and flow rates, and operational problems including flooding, loading,
consideration if it would be applied in carbon capture from a flue gas channeling, and foaming. This opens opportunities for emerging alter-
stream (Favre, 2007). The points are as follows: (i) MGS will require a natives technologies, such as membrane-based processes, to be applied
higher energy consumption than absorption for feed gas stream con- in CO2 capture and natural gas processing fields in the longer term
taining 10% of CO2 even when the membrane has selectivity above 120; because of the potential to overcome the limitations of current tech-
(ii) energy consumption of MGS will be competitive for treating feed nology. The main advantages of CO2 separation from natural gas and
gas stream with more than 20% of CO2; (iii) to be competitive in the CO2 capture using membrane-based technologies are low cost, low
latter case, the selectivity of the membrane should be around 60 or energy requirement, flexible operation, and modularity.
higher; (iv) the energy consumption can be significantly reduced when Despite the potential application of membrane-based carbon cap-
a vacuum condition is applied in permeate side; (v) since the mass ture, i.e. MGS and MC, they also have some limitations for the industrial
transfer of MGS is much lower than MC (4–6 times), permeability im- application that should be addressed. For MGS, the effort for industrial
provement is needed; and (vi) the best type of operation should be application should be focused on developing a new generation of
identified to fit with the target of residual water concentration because membrane that has high mechanical stability against high temperature
it is rarely be analyzed. Improving membrane performance to obtain and pressure, has anti-plasticization property to ensure its durability
CO2 permeance of 3 m3(STP)/m2 h bar) and CO2/N2 selectivity more (Zhang et al., 2013a,b), as well as high permeability and selectivity.
than 40 is required in the development of membrane materials (He, Meanwhile, for MC future research should aim to find new membrane
2018). In addition, further improvement to reduce the cost of CO2 materials that are compatible with the absorbent (Zhang et al.,
capture to $20/tonne CO2 is also necessary to make the MGS eco- 2013a,b). In addition, future studies of MC should also assess the
nomically feasible for industrial applications. techno-economic evaluation in large scale application, development of
Another interesting case for the selection of membrane-based novel module configuration to achieve a better mass transfer, and
carbon capture is when it should be applied for sweetening natural gas performance test under a real gas condition and high operating pressure
with very high CO2 concentration, for example, a natural gas reserved and temperature (Mansourizadeh and Ismail, 2009). The use of super-
in Natuna field, Indonesia. As the biggest natural gas field in Asia hydrophobic that has high wetting resistance against aqueous solvent in
Pacific, the utilization of natural gas in Natuna field is challenged by the MC is one of the interesting ways to avoid wetting and to ensure a long-
high concentration of CO2 (up to 71%) (Batubara et al., 2014; Muslim term stability. The interesting features of new developed ionic liquids
et al., 2015). It leads to a very expensive processing cost and only a could be one of the promising candidates of solvent for improving the
small portion of CH4 remains in the sales gas. As this natural gas field is performance of MC. However, confirmation of the performance of ionic
projected to fulfill the long-term national gas demand, the development liquids is needed before it can be used for commercial applications.
of the reliable process is strongly needed. The high concentration will Another interesting case for the selection of membrane-based carbon
be beneficial for MGS since it will result in a high driving force and high capture is when it should be applied for sweetening natural gas with
186
very high CO2 concentration. 00184-2.

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

Contents lists available at ScienceDirect

Journal of Natural Gas Science and Engineering

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

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

Abdulhameed et al. (2017)

Pengrui et al. (2017)

Franco et al. (2011)

Lin et al. (2016)

Lin et al. (2009)

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

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

CO2 absorption using water (Feed gas: pure CO2)

and N2 with the molar ratio of 13:87)

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

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

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

superhydrophobicity can be achieved. Blending polymer solution with

low surface energy material such as surface modifying macromolecule

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

Spray deposition of silica/PDMS

However, the superhydrophobicity seems diﬃcult to be achieved by

Coating with rough PP layer

using such a method which might be due to insuﬃcient surface

Superhydrophobic polymeric membrane can also be fabricated by

Grafting with FAS

surface modiﬁcation of the existing polymeric membrane, in which the

surface energy materials can be used for simultaneous surface rough-

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

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

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

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

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

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

membrane surface followed by hydrophobization using low-surface-

energy material or vice versa. Sequential modiﬁcations through

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

Merkel et al. (2010)

Yan et al. (2008)

Techno-economic assessment of membrane-based carbon capture

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;

α(CO2/N4): 500; PCO2: 1000 GPU;

α(CO2/N4): 20; PCO2: 72 Barrer;

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

Absorbent: MEA (20%; 40 °C)

they found that the three-stage membrane conﬁguration oﬀers the

Absorbent: MEA (30%)

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

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

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

5–10 kPa; 25 °C;

11.3 kPa; 40 °C;

0.2 MPa; 30 °C;

0.4 MPa; 30 °C;

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

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

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