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Review 1
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Review 2
ment of leaky interfacial voids and results in poor selectivity. that ILs act as a solvent and catalyst which controls a catalytic
Another big problem faced during membrane synthesis is filler conversion of cellulose, hemicellulose, lignin, and lignocellulos-
agglomeration, because it creates phase separation between fill- ic biomass into useful chemical products and fuel. Dai et al.
er and polymer, leading to weakening of the composite and [19] published a comprehensive review of ILs in numerous
forming non-selective defects [10]. So, the addition of the ter- important selective oxidation reactions. ILs were found to be
nary component can help minimize the polymer and inorganic highly efficient catalysts and solvents in these reactions.
interfacial voids issues. Literature has reported that the pres- In separation processes, the choice of appropriate solvents is
ence of ionic liquids (ILs) helps to CO2 absorption in a poly- challenging. Ventura et al. [20] reported a detailed review on
mer, resulting in an increase in CO2 permeance and CO2/CH4 the ILs in the extraction of bioactive compounds as a solvent.
selectivity [11]. The presence of ILs helps to form defect-free The use of ILs provides higher extraction yields compared to
interfacial morphology. It functionalizes the fillers present, im- conventional solvents.
proving the interfacial morphology issue. Different ILs are under study in membrane synthesis, e.g.,
Li et al. [8] reported that an MOF-polymer interfaces by emim dca, emim tf2n, and emim tcb have been reported by
incorporating an ionic liquid (IL)[bmim][Tf2N] into ZIF-8 J. Grunauer et al. [21] in supported liquid membranes for gas
cages. It was determined that the incorporation of MOF into separation. Mannan et al. [22] applied emim tf2n and polye-
polymers gives weak adhesion and non-selective interfacial thersulfone-based membranes for gas separation. ILs have
voids. However, the addition of 15 wt % IL@ZIF-8 improved shown good potential for gas separations [23]. Important cat-
the CO2 permeability and CO2/N2 selectivity by 45 % and 74 %, ions and anions used in gas separation membranes are summa-
respectively, and 92 % enhancement in CO2/CH4 selectivity rized in Figs. 1 and 2, respectively.
concerning the pure polymeric membrane was achieved. The
results showed that IL@MOFs are favorable fillers of MMMs
for gas separation. Both the MOFs and ILs are easily tunable. 2.1 Types of ILs
MMMs based on IL@MOFs can be designed to achieve better
gas separation performance for desired tasks. Ban et al. [12] TSILs act as a complexing agent which can be used for maxi-
also described a five times rise of CO2/CH4 ideal selectivity in mum loading in the base materials. In this way, these ILs can
IL@ZIF-8 membranes. The sections below provide comprehen- absorb high quantities of gas. Davis et al. reported the develop-
sive information about ILs and their applications in gas separa- ment of an IL-based amine functionality, capable of absorbing
tion membranes. 0.5 mole of CO2 per mole of IL [25]. Moreover, complexing
agents are also doped in ILs to increase the solubility uptake of
many solutes [26, 27].
2 Ionic Liquids (ILs) Comparatively, RTILs, more specifically, imidazolium-based
ILs due to the modular nature, are polymerized. Applications
ILs are organic salts that exist in liquid form at or below 25 °C. of RTILs cover broad aspects such as green solvents for reac-
They remain fluids at such a low temperature because of con- tions, bulk fluids, membrane separations, and electrochemical
siderable size and irregularity of the cation, attached with reso- systems [17]. Imidazolium- and pyridinium-based ILs are
nance-stabilized anions. ILs are characterized by negligible reported as feasible solvents for CO2 separation due to tunable
vapor pressure, nonflammability, and high thermal stability, cation or anion properties to meet the system requirements
which make them suitable for different gas separation process- [28].
es. Furthermore, polymeric ILs exhibit higher CO2 absorption
The first IL reported was ethyl ammonium nitrate by Paul and high mechanical strength [29] values compared to straight
Walden in 1914, and now ILs have become a major scientific RTILs [30]. Polymerization of the RTIL monomer by changing
area. More specifically, ILs were suggested as a CO2 separation the n-alkyl length is helpful to increase the permeability of tar-
medium by Blanchard et al. in 2001 [13]. Currently, in the last get gases, i.e., CO2, N2, and methane (CH4) [31].
two decades, ILs have gained tremendous popularity covering
multidisciplinary fields such as chemistry, material science,
chemical engineering, and environmental science [14]. How- 2.2 Applications of ILs in Separation Processes
ever, the use of ILs is also limited because of high cost, unclear
toxicities, and potential environmental effects. ILs in separation processes cover a wide range, such as electro-
ILs are classified into few categories, such as room-tempera- chemical applications, extractive separation [32, 33], and also
ture ILs (RTILs) [11], task-specific ILs (TSILs) [15], and poly- membrane gas separations [34]. Membranes based on ILs
ionic liquids (PILs) [16]. They are recommended as solvents, exhibit significant benefits for separation of gas mixtures com-
catalysts, and reagents in many chemical reactions. Properties pared to conventional solvent-based membranes because ILs
of ILs can be modified with alternation of cations or anions for have much higher solubility values for different gaseous species
specific applications [17]. The cations or anions via functional- [34–36]. Furthermore, IL gas separation membranes work by
ization can change the properties of the materials such as gas solubility in the IL comparison to diffusivity [37]. A
hydrophobicity/hydrophilicity and specific chemical interac- detailed description of properties and applications of IL mem-
tions. In polymers, ILs can act as wetting agents and these fea- branes is presented in Fig. 3.
tures open applications of ILs as solvents in membranes. ILs
have also been reported by Zhang et al. [18], who described
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Review 3
Chem. Eng. Technol. 2019, 42, No. 00, 1–15 ª 2019 WILEY-VCH Verlag GmbH & Co. KGaA www.cet-journal.com
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Review 4
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Review 5
3.2 Ionic Liquid Mixed-Matrix Membranes (ILMMMs) based on polyamides. Polyamide and cellulose acetate were
reported for gas separation membranes for CO2 and CH4 sepa-
Generally, the ILMMM synthesis involves several additional ration [48]. Fluorinated polyimides comprising 2,2-bis(3,4-
steps compared to the synthesis of pure polymeric membranes: dicarboxyphenyl) hexafluoropropane dianhydride (6FDA) are
(1) Dispersion of inorganic particles in the solvent, (2) sonica- described as attractive membrane materials because of their
tion of the solution to keep particles in suspension, (3) priming remarkable gas permeability and selectivity compared to non-
of the polymer with the inorganic particles, (4) casting of the fluoropolyimides [49–51]. Similarly, improved CO2/CH4 selec-
solution, (5) drying of the membranes. The fabrication of tivity was found using a 6FDA-based co-PI membrane cross-
ILMMMs is illustrated in Fig. 5. Fig. 6 presents schematically linked by ethylene glycerol [52].
the ILMMMs synthesis. The recent gas separation membrane technologies are lead-
ing by polymeric materials due to low cost, excellent mechani-
cal stability at higher pressure, and easy synthesis ability. Poly-
4 Applications of ILs in Gas Separation mer-polymer blending is also reported by many authors
Membranes [53, 54]. However, these membranes suffer from low perme-
ability or selectivity. There is an inverse relationship between
4.1 Polymeric Membranes permeability and selectivity stated by many authors [55–57].
Moreover, plasticization is an issue which arises in dense
Membrane technology is applied since 1980 [46]. Commercial- polymeric membranes when CO2 concentration in the feed
scale CO2 separation from natural gas is installed at Kvaerner- stream rises. CO2-induced plasticization is a phenomenon
GSM. Many polymeric materials have been reported for the where the permeability of CO2 increases as a function of pres-
synthesis of dense polymeric membranes. Initially, DuPont sure, whereas selectivity decreases [58]. The presence of CO2
(USA) and Ube Industries Ltd. (Japan) [47] used membranes acts as a plasticizer, and dissolved CO2 in polymer causes
Figure 5. ILMMMs.
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Review 6
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Review 7
network because of swelling and leaching in the liquid phase, from 19 to 30 [89]. Rehman et al. [93] stated an improvement
e.g., in pervaporation [84]. in selectivity of up to 53 in ethanolamine-based IL membranes.
To overcome this issue, IL polymeric membranes (ILPMs) Details of a few ILPM performances are given in Tab. 2.
were synthesized. The difference in ILPMs and SILMs is that Field-emission scanning electron microscopy (FESEM)
ILPMs require polymerizable groups along with proper prepa- images of ILPMs are depicted in Figs. 9 and 10 for surface and
ration techniques or physical blending of the IL with a suitable correctional views, respectively. These images demonstrate a
polymer in the presence of a compatible solvent. Tab. 1 pro- dense and smooth morphology.
vides a summary of permeability and selectivity data for gas
separation in SILMs.
4.5 ILPMs
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Review 8
Table 2. Permeability and selectivity data for gas separation in IL polymeric mem- stated an increment in the permeability with
branes. the incorporation of an IL in poly(RTIL)
[100]. Results showed that the presence of
Ionic liquid Polymer CO2 permeability [Barrer] CO2/CH4 selectivity RTIL increases polymer zeolite adhesion in
10 wt % PIM-COP [89] 812 19 MMMs since RTIL also acts as the wetting
[C6mim][Tf2N] agent for the zeolite. Three components,
SAPO-34, RTIL, and zeolite, were mixed to
[EMIM][BF4] CTA [94] 20 42
determine the optimum ratios. Improve-
[EMIM][TFSA] PVDF [95] 985 19 ment in CO2 permeance was observed
increasing with the loading of IL [101].
[EMIM][BF4] CTA [94] 20 28
Oral et al. described the RTIL loadings of
[EMIM][TFSA] PVDF [95] 985 39 emim[Tf2N] and emim[CF3SO3] towards
MMMs composed of polyimide-zeolite
(SAPO-34) and concluded that reinforce-
ment of emim[CF3SO3] had increased the CO2/CH4 selectivity
whereas emim[CF3SO3] was more selective towards CO2/CH4.
Tab. 4 provides permeability and selectivity data for gas separa-
tion in ILMMMs.
ILPMs with the addition of ILs into the polymeric membranes As an IL comprises an anion and a cation, the effect of these
is a crucial challenge. To overcome this issue, the addition of ions towards separation is further highlighted in the next sec-
an inorganic filler is considered to enhance the mechanical tion. FESEM images of ILMMMs depicted in Fig. 11 indicate
strength of the gas separation membranes without compromis- that ILMMMs were dense and homogeneous, which resulted in
ing the gas separation performance. In the upcoming section, high gas separation performance of ILMMMs with providing
ILMMMs are described. ILs are also suitable to improve the higher mechanical strength of the membrane due to the pres-
interphase morphologies of membranes [97] since ILs are ence of the inorganic filler.
reported to be excellent contributors to improve the polymer Fig. 12 represents the comparison of SILMs, PILMs, and
and inorganic filler compatibility [98]. ILMMMs on a Robeson’s upper bound curves graph and com-
mercial region of membranes. It is obvious that ILPMs and
SILMs both have good permeability values; however, the selec-
4.6 ILMMMs tivity values are just touching the commercial region. ILMMMs
exhibit a lower permeability compared to ILPMs and SILMs
ILMMMs reported by Hudiono et al. [99] showed the combi- with improved selectivity and are present above the commer-
nation of RTILs and zeolite in the polymer matrix. Bara et al. cial region.
Membrane Young’s modulus [MPa] Tensile strength [MPa] Extension at break [%]
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Review 9
Figure 12. Robeson’s upper bound curves showing the general tradeoff between permeability and selectivity for CO2/CH4 separation
from this literature review data.
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Review 10
solubility of non-reactive gases was not affected by the change tion performance of the reported membranes. It was examined
in the acid-base interaction within the IL. that the incorporation of MOFs into the polymers almost
Many types of anions are famous and well-studied, such as or- doubles the H2 permeabilities, which demonstrates that MOF/
ganic anions, carboxylates, sulfonates, sulfonamide, and polymer and MMMs are a better option for H2/N2 separation
inorganic anions (BF4, NO3, and Cl) had a distinctive effect on technologies.
CO2 sorption properties. Overall, it is concluded that increasing Less experimental studies have been performed using ZIF-8
the basicity of anions is known to enhance CO2 sorption [107]. because of complex synthesis. Molecular simulation can be
Another valuable property which affects solubility is the density helpful to resolve such limitations. Additionally, it contains a
of the IL. Higher selectivity values for P[DADMA][Ac] were tool that supports understanding about the processes occurring
reported because of the lower viscosity of P[DADMA][Ac] primarily at a molecular level by providing a path from the
compared to other PILs used in this study [106]. So, the varia- microscopic details of a system to macroscopic properties of
tion of the anion with increasing anion-basicity and decreasing the experimental interest [25]. This approach has been applied
IL density improves the sorption value of CO2. successfully in zeolites, MOFs, and ZIFs [26–30] and with other
Another property affecting the permeability is the viscosity. inorganic fillers [112].
Results have shown that ILs having higher viscosity exhibit
lower solubility. For example, emim tfo had a permeability val-
ue of CO2 684 Barrer compared to emim tf2n that exhibited 6 Prospects of ILs in Gas Separation
811 Barrer at 288 K [108]. Also, high CO2 separation perfor- Membranes
mances were observed for IL mixtures comprising anions with
cyano groups, namely as dicyanamide and thiocyanate, which Currently developed membranes for gas separations are defi-
have lower viscosity values. This means that less viscous anions cient in durability and performance. Research indicates that a
are essential to achieve improved CO2 separation performances filler dispersed in a polymer nonuniformly can produce a noni-
[109]. An increase in the alkyl chain length of a cation also deal filler-polymer interfacial morphology, e.g., interface voids,
causes a higher viscosity of ILs and consequently a weaker per- a rigid polymer layer around the inorganic fillers, and particle
meation of CO2 molecules. pore blockage (in case of porous fillers) [9]. Moreover, when
glassy polymers are used as matrix material, poor polymer-
filler contact arises that leads to the development of leaky inter-
5 Experimental and Computational facial voids and results in poor selectivity. Another sincere
Studies problem faced during membrane synthesis is filler agglomera-
tion because it creates phase separation between filler and poly-
Experimental and computational studies provide a way for in- mer, leading to weakening of the composite and forming non-
corporation of ILs in the membranes. A computational study selective defects [10].
plays a vital role in finding the correct combination of ILs with Therefore, the issues mentioned above lead to challenges for
fillers and polymers. Amro et al. [110] examined the tailoring better gas separation performance. These membranes get dam-
of zeolitic imidazolate framework-8 (ZIF-8), an important aged and dramatically reduce the selectivity due to weak
MOF, by restraining the pairs of bmim[Tf2N] IL within the mechanical strength at higher pressure streams. According to
cages of ZIF-8 (IL@ZIF-8). Molecular force fields were estab- literature, such problems arise due to the incompatibility of
lished for both the ZIF-8 framework and the bmim[Tf2N], and inorganic filler with polymer, resulting in poor adhesion of the
these were used in molecular simulations of the system. Monte filler with the polymer and nonhomogeneous dispersion of fill-
Carlo simulations were applied for sorption of CO2/CH4 and er in polymers. Consequently, exploring efficient technology is
CO2/N2 computations. The results exhibited an increment of urgently required. To overcome the plasticization issue, thermal
CO2 sorption because of the existence of the IL, which im- treatment, cross-linking, and polymer blending has to be modi-
proved significantly the CO2 selectivity and capacity. fied.
Moreover, the reason for the variation of CO2 selectivity with Mohshim et al. stated that the presence of ILs in polymers
the IL composition in the IL@ZIF-8 complex was examined increases the plasticization pressure of a membrane [113]. In
and the optimum IL composition for the separation efficiency the case of CO2/CH4, IL helps to CO2 absorption in a polymer,
was determined. The simulations agreed well with reported resulting in an improvement in both permeance CO2 and selec-
experimental points. The simulation data for CO2/N2 and tivity of CO2/CH4 gas [11]. The presence of ILs help to form a
CO2/CH4 showed an improvement in separation as IL wt % defect-free interfacial morphology. It functionalizes the present
increased. The overall modeling evaluation proved that incor- fillers, enhancing the interfacial morphology issue. Moreover, it
poration of ILs provided a good accuracy compared to the is recommended to improve polymer-filler adhesion and to
experimental work. So, in this way, with the help of similar form defect-free interfacial morphology. ILs, new solvents, new
research studies, it will be helpful to determine different combi- fillers as well as surface-modified fillers should be explored
nations of IL@ZIFs for CO2 capture and to suggest new [114] and high-quality composite membranes can be synthe-
IL@ZIFs composites which can achieve better CO2 selectivity sized. Moreover, computational studies are also effective to pre-
and capacity. dict the gas separation performance for complex synthesis sys-
Azar et al. [111] reported the simulation results for binary tems.
mixtures, which also could be well compared with the separa-
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Review 11
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Review 12
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