ZIF-8-Based Membranes for Carbon Dioxide Capture and Separation

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ZIF-8 based membranes for carbon dioxide capture/separation Xiao Gong, Yongjin Wang, and Tairong Kuang ACS Sustainable Chem. Eng., Just Accepted Manuscript • Publication Date (Web): 03 Nov 2017 Downloaded from http://pubs.acs.org on November 7, 2017

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ACS Sustainable Chemistry & Engineering

ZIF-8 based Membranes for Carbon Dioxide Capture/Separation Xiao Gong*a, Yongjin Wang b, Tairong Kuang*c a. State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology,

No.

122,

Luoshi

Road,

Wuhan

430070,

China.

E-mail:

[email protected] b. Dalian Institute of Chemical Physics, Chinese Academy of Science, 457 Zhongshan Road, Dalian 116023, China. c. The Key Laboratory of Polymer Processing Engineering of Ministry of Education, South China University of Technology, NO. 381, Wushan R.D., Tianhe DIST., Guangzhou 510640, China E-mail: [email protected]

ACS Paragon Plus Environment


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ABSTRACT Zeolitic imidazolate framework-8 (ZIF-8) which is a class of metal-organic frameworks (MOF) is a newly synthesized porous materials. It presents thermally and chemically stable for the application of carbon dioxide (CO2) adsorption/separation due to its porous structure. In this article, we briefly summarized the most recent studies on ZIF-8 based membranes for CO2 adsorption and separation. We also discussed the ZIF-8 fabrication methods, different parameters such as composite materials, temperature and pressure effect on the permeability and selectivity of CO2. Moreover, the special features of selected adsorbed and separated membranes were discussed. Lastly, the future research directions and challenges were briefly discussed. KEYWORDS: ZIF-8, CO2, Membranes, Capture/separation


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INTRODUCTION Recently, the global carbon dioxide (CO2) levels approach worrisome milestone.1-2 It is very important and necessary to solve this global issue of CO2 pollution since it may lead to many environmental problems such as greenhouse effect, climate changes, and snow cover melts. So far, many techniques have been developed to solve this problem including physical/chemical adsorption, cryogenic distillation, temperature/pressure-swing adsorption, membrane separation technology and so on.3-5 Among these technologies, membrane separation method, especially metal organic frameworks (MOFs) composite membrane technology is highly attractive and has been reported recently6 because of their promising advantages such as low energy consumption, high economic benefit, easy-industrialized, and high efficiency. In 2006, Yaghi et al.7 reported that they have successfully synthesized a series of crystals named as zeolitic imidazolate frameworks (ZIFs), with metal ions (Zn or Co) and imidazolate-type links.7 Then ZIFs have been gaining particular attention as one of the most investigated MOFs since they are easy to be fabricated, present remarkable stability and have special molecular sieving effect. ZIF-8 with single crystal X-ray structure as shown in Figure 1, is a prototypical member of ZIFs with a SOD (sodalite) zeolite-type structure.8



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Figure 1 The single crystal x-ray structures of ZIFs-8. The net is shown as stick diagram (left) and as a tiling (center). The largest cage in ZIF-8 is shown with ZnN4 tetrahedra in blue (right). H atoms are omitted for clarity. (Reprinted with permission from ref.7.)

Though several reviews9-13 introduced the class of MOFs materials and their applications for CO2 adsorption and separation, a more detailed review that focuses on adsorbing/separating CO2 by ZIF-8 nanoparticles is rare. It is very important and necessary to gather attention on this particular topic since ZIF-8 shows a high porosity, high surface areas, the best thermal stability, outstanding chemical resistance and strong mechanical strength.7, 14-16 Hence, this review aimed to introduce the recent advances in ZIF-8 based membranes for the applications in CO2 adsorption and separation. Herein we separately summarized four applications, including pure CO2 adsorption, and CO2 separation from methane (CH4), hydrogen (H2), and nitrogen (N2) respectively.

CO2 adsorption and separation In this review, four technologies, including pure CO2 adsorption, the separations of CO2/CH4, CO2/H2 and CO2/N2 by ZIF-8 porous materials have been summarized


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respectively. Different parameters such as the size of ZIF-8, composite materials, temperature and pressure effects on the CO2 adsorption and separation performances have also been discussed herein. Pure CO2 adsorption ZIF-8 composite membranes are able to adsorb CO2 gas because the crystals within ZIF-8 can provide the Langmuir sites which can be replaced by CO2 molecules.17 The loading percentage of ZIF-8 in the membrane can influence the permeability of CO2.18-20 For example, Song et al.

18

reported that they have

synthesized a membrane by dispersing ZIF-8 nanoparticles into the polymer of Matrimid® 5218. Such membrane can highly increase the permeability of CO2 during the pure gas sorption tests. This is attributed to the special structure of loaded ZIF-8 in the membrane, which can provide a much larger free volume than that of neat polymer membranes. They also found that the permeability of CO2 increased with the loading of ZIF-8 in the matrix membranes: The permeability of CO2 reached to 28.72 Barrer when the ZIF-8 loading increased up to 30%, which was almost three times of that in the 5% ZIF-8 loading. However, the mechanical strength decreased at a very high loading of ZIF-8 (~80%), and the permeability started to decrease when the loading was higher than 50% for pure CO2 sorption test.19 ZIF-8 can also be obtained to be 3D hierarchical structures to improve CO2 adsorption21 and water can irreversibly react (Figure 2) with CO2 and ZIF-8, leading to a decrease of CO2 adsorption.22



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Figure 2 Irreversible chemical reaction among ZIF-8, water, and CO2, which creates both zinc carbonate (or zinc carbonate hydroxides) and single 2-methylimidazole crystals. (Reprinted with permission from ref.22)

Usually, ZIF-8 is prepared with the composite polymer as a nanoporous membrane for gas adsorption. The performance can be enhanced by this nanoporous membranes compared with neat polymer membranes.15, 23-24 Moreover, the membrane can also be prepared on a wide range of substrates such as copper net,25 alumina porous support,26 titania support,27-29 tubular α-alumina support28,

30-31

, Zn-related

nanofibers32-35 and Nylon membrane36. For example, Xu et al.37 prepared a ZIF-8 membrane on alumina hollow fibers using a concentrated ZIF-8 synthesis gel. They found that such membrane presented a strong adsorption capability of CO2 with a low permeance, which is attributed to the fact that the adsorbed CO2 blocks the pores of ZIF-8, gradually reducing the permeance of CO2. Additionally, ZIF-8 is more thermally stable than the commercial adsorbents such as Zeolite-13X: The activation temperature has almost no influence on the CO2 adsorption capability for ZIF-8.38 The modifications of post-synthetic method39, amine-modified method40-41, and so on42 have been used to improve the BET surface area of ZIF-8, to add new sorption site of –NH2 groups, which can enhance the adsorption efficiency. In order to improve the adsorption performance toward CO2,


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ZIF-8 was modified by a post-synthetic method using etheylenediamine.39 Results showed that the CO2 adsorption capacity of per surface area for the modified ZIF-8 could be almost two times of that on ZIF-8 at 298 K and 25 bar. Due to the electron-donating effect of amino functional groups, it is expected that amino-modification is an efficient method to improve CO2 adsorption of ZIF-8. Therefore, Liu et al.40 simulated the CO2 adsorption capacity of ZIF-8 and revealed that in the lower pressure regime the capacity is: ZIF-8 < ZIF-8-NH2 < ZIF-8-(NH2)2, while in the high-pressure regime the capacity is: ZIF-8 < ZIF-8-(NH2)2 < ZIF-8-NH2. Since the existence of -NH2 groups can generate new adsorption sites (Figure 3), amino-modification of ZIF-8 can obviously enhance its CO2 adsorption capacity. Above experimental and theoretical studies can help researchers better design ZIF-8 based membranes for CO2 adsorption in the future.

Figure 3 Contour maps of the electrostatic potential (ESP) for (a) ZIF-8, (b) ZIF-8-NH2, and (c) ZIF-8-(NH2)2. (Reprinted with permission from ref.40.)

CO2/CH4 separation



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Natural gas usually contains lots of impurities including CH4, and some other light gases such as C2H6, C3H8, and acid gases such as CO2 and H2S, in which CO2 is regarded as the most crucial and needs to be removed since it can corrode pipelines and reduce the energy content of the natural gas.43 Many technologies have been developed to separate CO2 from natural gas such as chemical adsorption44-45 and cryogenic separation46. However, these technologies are limited by high loss of solvent, high consumption of energy and low efficiency during the separation.47-48 In order to solve these problems, membrane separation method was reported to have highly potential application in commercial CO2/CH4 separation.49-53 Among the separated membranes, mixed matrix membrane (MMM) was recently most highly developed due to its outstanding advantages such as high selectivity and good stability. In this part, we will focus on reviewing this typical membrane, which is composed of ZIF-8 and various polymers. The influence of incorporated polymers54, ZIF-8 nanoparticles parameters including size55-56, chemical modification57-58, structure59-60 and loading percentage54, 61-64, and fabrication conditions including temperature56, 65-66, method67-68, time69 and so on43, 70-73 on the performance of CO2 and CH4 separation are summarized herein. Chi et al.55 investigated the size of ZIF-8 effect on the CO2 capture. The different sizes of ZIF-874-75 with the same surface areas were achieved by controlling the sources of Zinc76-77 and their FE-SEM images are shown in Figure . The separation membranes (polystyrene-block-poly(ethylene-ran-butylene)-block-polystyrene (SEBS) /ZIF-8) were finally fabricated by dispersing ZIF-8 into block copolymer78-79


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homogeneously. It is found that the selectivity of CO2 and CH4 can be enhanced with ZIF-8 added membrane compared with neat polymer membrane, while the selectivity is almost independent of ZIF-8 particle sizes if the surface area of particles ZIF-8 keeps as the same. The selectivity α is 5.2, 5.4 and 5.2 for small, medium and larger ZIF-8 nanoparticles, respectively. A little higher performance of medium ZIF-8 may be attributed to the interactions and interfaces of SEBS/ZIF-8 membrane. The conclusion that CO2/CH4 selectivity changes with ZIF-8 particle sizes which is reported in previous work56 may be related to the different surface areas of ZIF-8 particles with different sizes.

Figure 4 FE-SEM images of ZIF-8 nanoparticles of different sizes; (a,b) ZIF-8(S), (c,d) ZIF-8(M), and (e,f) ZIF-8(L) (Reprinted with permission from ref. 55.)



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In

order to

change

their properties,

ZIF-8

nanoparticles were

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also

ammonia-modified to improve the selectivity performance as shown in Figure .57-58, 80 When MMM was prepared with the ZIF-8 that modified under 25 mL ammonium hydroxide solution at 60 ºC, it presented a largest selectivity of CO2/CH4.57 The largest BET surface area and the smallest mesopore volume observed on the ammonia-modified ZIF-8 may be attributed to the best separation performance. The loading of ZIF-8 in this membrane is only 0.5%, which is significantly smaller than previous work due to the asymmetric property61 of the membrane. Before mixing nanoparticles with incorporated polymers, ZIF-8 can also be prepared as special hetero-nanostructures81 such as hollow zeolite imidazole frameworks59 and mixed-linkers82-83 to generate lower density nanoparticles with larger BET surface area. With the help of these special structures, the membranes can achieve a similar separation performance with less ZIF-8 loading, which can reduce the cost of the membranes.84-85

Figure 5 Idealized crystal structure of amine-modified ZIF-8 (adapted from Liu et al.40 ). The NH2 –ZIF-8 represents the –NH2 attached on a single side of C=C, while (NH2)2 – ZIF-8 represents the –NH2 group attached on both sides of C=C in the imidazole linkers. (Reprinted with permission


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from ref.57.)

Besides changing the properties of ZIF-8 nanoparticles, more modifications can be done when mixing ZIF-8 with incorporated polymers to enhance the separation capability. Bushell et al.54 found that the largest separation factor of CO2/CH4 could be observed when the loading of ZIF-8 was around 28 vol%. Either smaller or higher loading could reduce the selectivity of CO2/CH4.54, 61, 86 The fabrication conditions of MMMs such as heat treatment56, post-treatment65, combined with other MOFs87 fabrication technologies including secondary growth67 and sonication method68 were also investigated for the application in CO2/CH4 separation. For example, Nordin et al. 56

reported that ZIF-8 heat-treated at 100 °C for a minimum of 12 hours could

enhance its phase crystallinity, leading to a surface area of 981.1 m2 g-1. When the heat-treated ZIF-8 of the smallest size was incorporated into a polysulfone (PSf) matrix (Figure 6), the MMMs could exhibit CO2/CH4 selectivity of 28.5, which is obviously larger than the 19.43 obtained for the neat PSf membrane. Thompson et al. showed high-intensity ultrasonication could induce Ostwald ripening on ZIF-8 nanoparticles.68 The ZIF-8 based membranes fabricated by both direct and indirect sonication exhibited good adhesion between the polymer and ZIF-8 nanoparticles. However, membranes prepared by indirect sonication had an agglomeration of nanoparticles, while membranes prepared by direct sonication showed the well dispersion of nanoparticles. Permeation tests revealed the significant improvement in permeability of CO2 and enhancement of CO2/CH4 selectivity in membranes fabricated with high-intensity sonication. Above studies have proven to be



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straightforward methods to simultaneously improve CO2 permeability and ideal CO2/CH4 selectivity, which are beneficial for future applications in gas separation membranes.

Figure 6 Cross-section morphology of the heat-treated ZIF-8 MMM, with (a) 100 nm, (b) 300 nm, and (c) 500 nm (Red circle represent the presence of ZIF-8 cluster). (Reprinted with permission from ref.56.)

CO2/N2 separation The capture of CO2 in the atmosphere mostly generated from the burning of fossil fuel is another critical environment problem.88 Since more than two-thirds of fuel gas is nitrogen, many technologies have been developed to separate CO2 from


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nitrogen-rich streams.89-95 Herein, we will focus on summarizing the separate of CO2 and N2 with ZIF-8 added membranes.96 Dai et al.97 first successfully fabricated a mixed matrix hollow fibers membranes, which were composed by ZIF-8 and Ultem® 1000 (a polyetherimide)98, by the method of dry jet-wet quench for the application of CO2/N2 separation. The selectivity was enhanced by as high as 20% for these membranes over pure polymer hollow fibers membranes. They also investigated the temperature and feed pressure effect on the permeance and the selectivity as shown in Figure : A maximum selectivity of 32 could be achieved under larger feed pressure (50 psia) and small temperature (25 ºC). Moreover, it is noticed that this study is the first time reported to extend gas separation

membrane

to

asymmetric

membrane.

Additionally,

ZIF-8

was

pre-synthetized with the polymer of poly(vinylamine) (PVAm), following with dispersing into PSf polymer, to fabricate a PVAm/ZIF-9/PSf MMM, which can further improve the separation performance.99

Figure 7 Mixed gas permeation results using a feed containing 20% CO2 with a N2 balance. (A) Permeance of CO2 (closed symbols) and N2 (open symbols). (B) Permselectivity results for mixed gas measurements. Measurements were conducted at 25 ºC (circles), 35 ºC (triangles) and 45 ºC



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(squares). (Reprinted with permission from ref.97.)

Similar with CO2 adsorption, ZIF-8 nanoparticles can not only be directly mixed with polymers but also be grown on different substrates to fabricate the separation membranes. Marti et al.100 fabricated a continuous inorganic membrane with ZIF-8 nanoparticles on a polymeric hollow fiber support by the continuous flow synthesis method as shown in Figure . This method is simple, scalable, low cost and environmentally friendly and the selectivity of CO2/N2 can be highly enhanced compared to MMMs. Similarly, Isaeva et al.101 used in situ synthesis method to grow ZIF-8 membranes on polymeric and inorganic supports for the application in CO2 and N2 separation. In addition, ZIF-8/polysulfone102, ZIF-8/(Polyether block polyamide with

flexible

polyether

segments

(PEBAX)-2533)103,

ZIF-8/(1,3-Di-n-butyl-2-methylimidazolium chloride (DnBMCl))104 and so on were reported to be used as a separated membrane for CO2 and N2 separation.

Figure 8 (A) Processing of supported ZIF-8 hollow fiber membrane. (B) Cross-section diagram showing the hollow core, porous Torlon structure, and ZIF-8 on the surface of the support. (Reprinted with permission from ref.100)

CO2/H2 separation


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The separation of CO2 and H2 usually needs to treat the products of water-gas shift reaction in order to obtain high purity hydrogen.105 Similar with CO2/CH4 and CO2/N2 separations, ZIF-8 nanoparticles composite membranes also present very good properties for CO2/H2 separation. The mechanism of pair gas separation includes diffusion selectivity and solubility selectivity.106-107 The kinetic diameter of CH4 and N2 is 3.80 Å and 3.64 Å, respectively, which is larger than CO2 (3.30 Å), while the kinetic diameter of H2 is 2.89 Å which is smaller than CO2. The diffusion selectivity favors the transport of the smaller molecules of CO2, CO2, and H2 for the separation of CO2/CH4, CO2/N2, and CO2/H2, respectively, and the solubility selectivity favors the sorption of the more condensable gas, which is CO2 for all the separations. Therefore CO2/H2 separation is more complex and difficult than CO2/CH4 and CO2/N2 separations since the solubility selectivity and the diffusion selectivity of CO2/H2 separation present opposite trends.49,

108

Generally, this separation is

conducted under high temperature in order to reduce the adsorption of CO2. It was reported that pure ZIF-8 membrane which was grown on hollow ceramic fiber tube displayed a large H2 permeability and good separation performance.109 Additionally, ZIF-8 deposited with graphene oxide (GO) to fabricate a ZIF-8/rGO membrane (Figure ) showed a high hydrogen selectivity.110-112 ZIF-8 particles in situ crystallized between the sheets of graphene membranes, were strongly anchored with graphene by coordination bonds. The mechanical flexibility,113 thermal stability,114 fabrication methods115 of ZIF-8 membranes effects on separation performance have also been reported. Since mechanical flexible and stable MOF composite membranes



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are highly desirable, Hess et al. developed a new synthesis method that could form the flexible, noncontinuous ZIF-8 − poly(ether sulfone) (PES) composite membranes.113 They showed that ZnO seed-nanoparticles could enter into pores of a polymeric membrane during solvent casting and these nanoparticles could make ZIF-8 in situ growth by solvothermal synthesis. This technique leads to mechanically flexible self-supporting ZIF-8 polymeric membranes which could be applied for the synthesis of a variety of MOF systems and served as a platform for flexible MOF gas separation. James et al. systematically investigated the thermal stability of ZIF-8 membranes which is important for high temperature gas separation applications.114 Results showed that ZIF-8 membranes kept their crystallinity and structural integrity when temperature was below 150 °C. However, ZIF-8 membranes obviously underwent thermally induced carbonization when temperature was above 150 °C. Lo et al. demonstrated a novel method using pseudopolymorphic seeding for the rational synthesis of hybrid membranes with ZIFs which can enhance the separation performance of the ZIF-L@ZIF-8 hybrid membranes which may be attributed to the interlayer spacing among ZIF-L crystals allowing for the rapid diffusion of hydrogen.115


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Figure 9 Assembly of a ZIF-8/rGO membrane. (a and b) Synthesis process of the ZIF-8/rGO membrane by in situ crystallization. (c and e) Crystalline structure of rGO and ZIF-8. (d) Coordination bonds between rGO and ZIF-8. Carbon, oxygen, nitrogen and zinc atoms are shown in grey, red, blue and yellow, respectively. (Reprinted with permission from ref.111.)

Moreover, in order to further improve the selectivity of CO2/H2, ZIF-8 particles were mixed with polymers to fabricate MMMs for CO2/H2 separation.116-122 For example, Sanchez-Lainez et al.116 prepared a membrane with ZIF-8 and polybenzimidazole (PBI), which increased the selectivity of CO2/H2 nearly by 55% compared to pure PBI polymer membrane. The relationship between ZIF-8 particle size and separation performance was discussed. The better performance of larger ZIF-8 particles may be due to the lower degree of agglomeration. They also indicated that although the performance of MMMs with dry ZIF-8s was better, wet ZIF-8s could not be removed since they were much easier to be industrialized. This issue could be reduced or eliminated by increasing the loading percentage of ZIF-8s and by increasing the separation temperature.116, 119

Diestel et al. prepared MMMs with

bulky ZIF-8 nanoparticles and investigated the permeation behavior of these membranes for the gas mixture H2/CO2.117 They found that the ZIF-8 based



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membranes obviously improved the hydrogen permeability, while the mixed gas separation factor kept constant at 3.5 ± 0.3. In order to obtain high gas flux and high selectivity, Wijenayake et al.118 showed that cross-linking the surface of the MMM by reacting with ethylenediamine vapor (Figure 10) could yield a 10-fold increase in H2/CO2, H2/N2, and H2/CH4 selectivities with respect to 6FDA-durene, which remained 55% of the H2 permeability of 6FDA-durene. Yang et al.119 fabricated MMMs by incorporating ZIF-8 nanoparticles into a polybenzimidazole (PBI) polymer. The experiments of mixed gas tests for H2/CO2 separation were carried out from 35 to 230 °C. Results showed the membranes exhibited remarkably high H2 permeability and H2/CO2 selectivity. The membrane containing 30 wt% ZIF-8 has an H2/CO2 selectivity of 26.3 with an H2 permeability of 470.5 Barrer, while the membrane containing 60 wt% ZIF-8 had an H2/CO2 selectivity of 12.3 with an H2 permeability of 2014.8 Barrer. According to the above works, the newly developed membranes may have bright prospects for CO2/H2 separation in realistic industrial applications.

Figure 10 Schematic representation of the formation of the crosslinked skin in 33.3 wt% ZIF-8/6FDA-durene MMM upon reaction with ethylenediamine (EDA) vapor. (Reprinted with permission from ref.118.)

Conclusions and Future Perspectives


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Table 1 summarized the permeability/selectivity of CO2 by selected ZIF-8 based membranes. The incorporated materials, the fabrication techniques for the membranes, and the special features have been listed for each membrane. In this review, the ZIF-8 based membranes for the applications of CO2 adsorption and separation have been discussed. We respectively summarized four technologies, including pure CO2 adsorption, the separations of CO2/CH4, CO2/H2, and CO2/N2. ZIF-8 nanoparticles can be pre-treated by chemistry modification and structure modification to increase their surface area, leading to a better separation and adsorption capability. Moreover, ZIF-8 can be incorporated with other materials by being immediately grown on some substrates or being directly mixed with polymers to fabricate membranes for CO2 adsorption and separation applications. The loading percentage of ZIF-8 among the membrane, the type of incorporated materials and the membrane fabrication methods can all affect the CO2 adsorption and separation. Last but not least, the effect of reaction parameters such as temperature, pressure, and surrounding environment are also summarized in this review. To date, the ZIF-8 nanoparticles based membranes are highly attractive since this kind of membrane has outstanding benefits for the applications in CO2 adsorption and separation. Given the fact they are promising materials for gas separation which could be applied in many industrial applications and gas transport mechanisms are still not fully understood, it is still quite challenging to design effective ZIF-8 nanoparticles based polymeric membranes for a given application condition. The following key issues and challenges still need to be addressed in future research.



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First, new methods and techniques such as the development of facile fabrication methods, scale up technique for industrialization in real life, and increasement of the economic effectiveness of the membranes are required to develop and exploit. For example, Chen et al. recently presented a new approach for preparing stable ZIF-8 coatings by a unique hot-pressing method which was both solvent-free and binder-free.123 During the procedure, high temperature and pressure were applied at the same time which made the rapid growth of ZIF-8 nanocrystals onto desired substrates. This continuous production of ZIF-8 membranes using a roll-to-roll machine makes the industrial applications of ZIF-8 based membranes more feasible. Second, the poor distribution and accumulation of ZIF-8 nanoparticles within the polymeric membranes are significant problems. As the dispersed phase, ZIF-8 nanoparticles should be well dispersed in the polymeric membranes in order to obtain gas separation membranes with high performance. Therefore, the ideal ZIF-8 based membranes should have well-dispersed inorganic fillers and the loading is as high as possible. Furthermore, the adhesion between ZIF-8 nanoparticles and polymer materials should be good to avoid the imperfect void structures and pinholes. In order to achieve this, ZIF-8 surface is usually modified with functional groups which can interact with suitable pendent groups of polymers. For instance, good compatibility between ZIF-8 and polymers could be achieved by designing hydrogen-bonding and covalent bonding between them. Experimental, computational and theoretical efforts are all required to address these issues. For example, different theoretical models such as the barrier film model and the Maxwell model should be introduced and/or


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modified to describe the separation behavior of the membranes which can be beneficial to the design of membranes with high separation performance. Third, environmental parameters such as humidity need to be systematically investigated since vast majority of gas separation applications are in ambient conditions and the adsorption of moisture is inevitable. This is critical to the real-life application. However, only few research works pay attention to this. Therefore, investigation of the effect of humidity on different gas separation membranes should be carried out since it is a key requirement and essential to the design of applications of gas separation membranes in real life. Fourth, mechanical stability as an important parameter should be considered and addressed for the gas separation applications of ZIF-8 based membranes. To obtain high performance of the gas separation of ZIF-8 based membranes, it is greatly desirable to improve the ZIF-8 loading amount. However, it will result in the loss of mechanical property of the membranes. Therefore, a suitable amount of ZIF-8 should be used during ZIF-8 based membrane fabrication. Moreover, new polymer materials should be synthesized and developed by a variety of methods such as copolymerization, blending, grafting, and crosslinking to overcome shortcomings including swelling, and plasticization. In summary, similar to any gas separation membranes, concerns such as long-term

stability

under

practical

conditions

(pressure,

temperature

and

contaminants), chemical modifications, good compatibility, permeability and plasticization resistance should be addressed in order to make ZIF-8 based



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membranes for real-life applications. Although significant amounts of works have been done on these topics, there is still a long way to go before large-scale application of ZIF-8 based membranes as gas separation membranes.


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Table 1 The permeability/selectivity of CO2 by selected ZIF-8 based membranes. Type of incorporated materials Matrimid® 5218 polymer Alumina hollow fiber PSf

Fabrication technique Solution mixing Concentrated synthesis gel Dry/wet phase inversion Dry/wet phase inversion

Feature

Permeability/Selectivity of CO2

Scale up for industrial applications Application for CO2 adsorption.

Permeability: 28.72 Barrer (30wt% loading, annealed under vacuum at 230 ºC for 18h) Adsorption of CO2 with very low CO2 permeance Selectivity CO2/CH4: 23.16 (0.5wt% loading, feed pressure 4 bar, 27 ºC ) Selectivity CO2/CH4: 34.09 (0.5wt% loading, feed pressure 4 bar, 27 ºC )

Asymmetric MMMs

PVC-g-POEM

Solution mixing

Copolymer (SEBS)

Solution mixing

Ammonia modified ZIF-8 Solvothermal surface coating and selective removal for structure Investigate ZIF-8 particle sizes effect

PIM-1

Casting

ZIF-8 loading effect

PSf

Polyetherimide Dry jet-wet (Ultem® 1000) quench method Solution PSf/PVAm mixing Flow synthesis Polyimide-ami Bore/shell de polymer reagent flow Crystallizing-r Hollow ubbing seed ceramic fibe deposition Graphene oxide PBI PBI

Layer-by-layer deposition Solution mixing Solution mixing

Asymmetric hollow fibers membranes PVAm pre-modifed ZIF-8 Simple, scalable, less cost and environmentally friendly Pure ZIF-8 membrane ZIF-8 combine with two-dimensional materials Validation through interlaboratory test CO or water vapor impurity effect

Selectivity CO2/CH4: 12.2 (10wt% loading, 35 ºC) Selectivity CO2/CH4: 12.0 ± 0.3 (30wt% loading, 35 ºC) Selectivity CO2/CH4: 18.6 ± 1.9 (28vol% loading) Selectivity CO2/N2: 32 (13 wt% loading, feed pressure 50 psia, 25 ºC) Selectivity CO2/N2: 112 (13.1wt% loading, feed pressure 0.3 Mpa, 22 ºC)

Ref. 18

37

61

57

59

55

54

97

99

Selectivity CO2/N2: 52 (25 ºC)

100

Selectivity CO2/H2: 5.2 (room temperature)

109

Selectivity CO2/H2: 14.9 (1 bar, 250 ºC)

110

Selectivity CO2/H2: 7.5 (20wt% loading, feed pressure 3 bar, 150 ºC) Selectivity CO2/H2: 26.3 (63.6 vol% loading, 0-30 atm, 230 ºC)


116

119


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Acknowledgements The authors thank the National Natural Science Foundation of China (no. 21774098, 21104069) for the financial support. This study is also supported by “the Fundamental Research Funds for the Central Universities (WUT: 2017IVA089) ”. We also thank the State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology (SYSJJ2017-01) for the support. T. Kuang would like to acknowledge the support of National Postdoctoral Program for Innovation Talents (NO. BX201700079).

Notes The authors declare no competing financial interest.

Biographies

Dr. Xiao Gong is currently a Full Professor in the State Key Laboratory of Silicate Materials for Architectures, Wuhan University of Technology, China. He received his Ph.D. in materials science from Zhejiang University in 2009. Prior to joining Wuhan University of Technology, he was a postdoctoral associate in Prof. Lei Li’s group at the University of Pittsburgh, USA. His research interests are on self-assembly and


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polymeric nanomaterials; polymer thin films; colloid surface and interface chemistry; fabrication and characterization of nanostructured materials; interfacial behavior of ionic liquid on solid surfaces.

Dr. Yongjin Wang is currently an assistant professor in Dalian Institute of Chemical Physics, Chinese Academy of Sciences. She received her B.S. degree in the department of Chemical Engineering from Dalian University of Technology, China (2010) and her Ph.D. degree in the department of Chemical Engineering from the University of Pittsburgh, US (2016). Her research interests are surface and interface.

Dr. Tairong Kuang received his Ph.D. in Materials Processing Engineering from South China University of Technology, Guangzhou, P. R. China. He is currently a lecturer in the key laboratory of polymer processing engineering of ministry of



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education, South China University of Technology. The primary focus of his research areas are in synthesis, processing and characterization of advanced polymeric materials and their functional applications in tissue engineering, energy, gas absorption/separation, biosensors, drug delivery, etc.

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TOC ZIF-8 based membranes have been reported for CO2 adsorption and separation.


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ZIF-8-Based Membranes for Carbon Dioxide Capture and Separation

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