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1.
Advanced porous framework membranes with excellent selectivity and high permeability of small molecules and ions are highly desirable for many important industrial separation applications. There has been significant progress in the fabrication of polycrystalline microporous framework membranes (PMFMs) in recent years, such as metal–organic framework and covalent organic framework membranes. These membranes possess small pore sizes, which are comparable to the kinetic diameter of small molecules and ions on the angstrom scale, very low thickness, down to tens to hundreds of nanometers, highly oriented crystalline structures, hybrid membrane structures, and specific functional groups for enhancing membrane selectivity and permeability. Recent advances in the fabrication methods of advanced PMFMs are summarized. Following this, four emerging separation applications of these advanced microporous framework membranes, including gas separation, water desalination, ion separation, and chiral separation, are highlighted and discussed in detail. Finally, a summary and some perspectives of future developments and challenges in this exciting research field are presented.  相似文献   

2.
Graphene-based materials have generated tremendous interest in a wide range of research activities. A wide variety of graphene related materials have been synthesised for potential applications in electronics, energy storage, catalysis, and gas sorption, storage, separation and sensing. Recently, gas sorption, storage and separation in porous nanocarbons and metal–organic frameworks have received increasing attention. In particular, the tuneable porosity, surface area and functionality of the lightweight and stable graphene-based materials open up great scope for those applications. Such structural features can be achieved by the design and control of the synthesis routes. Here, we highlight recent progresses and challenges in the syntheses of graphene-based materials with hierarchical pore structures, tuneable high surface area, chemical doping and surface functionalization for gas (H2, CH4, CO2, N2, NH3, NO2, H2S, SO2, etc.) sorption, storage and separation.  相似文献   

3.
Membrane-based carbon dioxide (CO2) capture and separation technologies have aroused great interest in industry and academia due to their great potential to combat current global warming, reduce energy consumption in chemical separation of raw materials, and achieve carbon neutrality. The emerging covalent organic frameworks (COFs) composed of organic linkers via reversible covalent bonds are a class of porous crystalline polymers with regular and extended structures. The inherent structure and customizable organic linkers give COFs high and permanent porosity, short transport channel, tunable functionality, and excellent stability, thereby enabling them rising-star alternatives for developing advanced CO2 separation membranes. Therefore, the promising research areas ranging from development of COF membranes to their separation applications have emerged. Herein, this review first introduces the main advantages of COFs as the state-of-the-art membranes in CO2 separation, including tunable pore size, modifiable surfaces property, adjustable surface charge, excellent stability. Then, the preparation approaches of COF-based membranes are systematically summarized, including in situ growth, layer-by-layer stacking, blending, and interface engineering. Subsequently, the key advances of COF-based membranes in separating various CO2 mixed gases, such as CO2/CH4, CO2/H2, CO2/N2, and CO2/He, are comprehensively discussed. Finally, the current issues and further research expectations in this field are proposed.  相似文献   

4.
Vertically oriented ordered mesoporous silica membranes have been successfully synthesized in our laboratory in the form of silica plugs filling the macron-sized straight pores of hydrophobic track-etched polycarbonate membrane support. However, these membranes have shown gaps between the plugs and support pore wall which make the membranes unfeasible for use. This paper reports on techniques of synthesis of defect-free ordered mesoporous silica membranes by filling the gaps with microporous silica. Here, the elimination of defects is achieved by filling the membrane gaps with an alkoxysilane followed by exposure to humid air to allow controlled hydrolysis and condensation resulting in the formation of microporous silica within the gaps. Molecular probing gas permeation and helium/nitrogen (or oxygen) binary separation tests, coupled with surface characterization methods, show that the final membranes contain ordered mesopores of about 2.7 nm pore diameter, running through the membrane, with gaps sealed by microporous silica having a pore size <0.55 nm.  相似文献   

5.
Although polycrystalline metal‐organic framework (MOF) membranes offer several advantages over other nanoporous membranes, thus far they have not yielded good CO2 separation performance, crucial for energy‐efficient carbon capture. ZIF‐8, one of the most popular MOFs, has a crystallographically determined pore aperture of 0.34 nm, ideal for CO2/N2 and CO2/CH4 separation; however, its flexible lattice restricts the corresponding separation selectivities to below 5. A novel postsynthetic rapid heat treatment (RHT), implemented in a few seconds at 360 °C, which drastically improves the carbon capture performance of the ZIF‐8 membranes, is reported. Lattice stiffening is confirmed by the appearance of a temperature‐activated transport, attributed to a stronger interaction of gas molecules with the pore aperture, with activation energy increasing with the molecular size (CH4 > CO2 > H2). Unprecedented CO2/CH4, CO2/N2, and H2/CH4 selectivities exceeding 30, 30, and 175, respectively, and complete blockage of C3H6, are achieved. Spectroscopic and X‐ray diffraction studies confirm that while the coordination environment and crystallinity are unaffected, lattice distortion and strain are incorporated in the ZIF‐8 lattice, increasing the lattice stiffness. Overall, RHT treatment is a facile and versatile technique that can vastly improve the gas‐separation performance of the MOF membranes.  相似文献   

6.
《工程(英文)》2020,6(12):1432-1442
Sustainable processes for purifying water, capturing carbon, producing biofuels, operating fuel cells, and performing energy-efficient industrial separations will require next-generation membranes. Solvent-less fabrication for membranes not only eliminates potential environmental issues with organic solvents, but also solves the swelling problems that occur with delicate polymer substrates. Furthermore, the activation procedures often required for synthesizing microporous materials such as metal–organic frameworks (MOFs) can be reduced when solvent-less vapor-phase approaches are employed. This perspective covers several vacuum deposition processes, including initiated chemical vapor deposition (iCVD), initiated plasma-enhanced chemical vapor deposition (iPECVD), solvent-less vapor deposition followed by in situ polymerization (SLIP), atomic layer deposition (ALD), and molecular layer deposition (MLD). These solvent-less vapor-phase methods are powerful in creating ultrathin selective layers for thin-film composite membranes and advantageous in conformally coating nanoscale pores for the precise modification of pore size and internal functionalities. The resulting membranes have shown promising performance for gas separation, nanofiltration, desalination, and water/oil separation. Further development of novel membrane materials and the scaling up of high-throughput reactors for solvent-less vapor-phase processes are necessary in order to make a real impact on the chemical industry in the future.  相似文献   

7.
The hydrogen and carbon monoxide separation is an important step in the hydrogen production process. If H2 can be selectively removed from the product side during hydrogen production in membrane reactors, then it would be possible to achieve complete CO conversion in a single‐step under high temperature conditions. In the present work, the multilayer amorphous‐Si‐B‐C‐N/γ‐Al2O3/α‐Al2O3 membranes with gradient porosity have been realized and assessed with respect to the thermal stability, geometry of pore space and H2/CO permeance. The α‐Al2O3 support has a bimodal pore‐size distribution of about 0.64 and 0.045 µm being macroporous and the intermediate γ‐Al2O3 layer—deposited from boehmite colloidal dispersion—has an average pore‐size of 8 nm being mesoporous. The results obtained by the N2‐adsorption method indicate a decrease in the volume of micropores—0.35 vs. 0.75 cm3 g?1—and a smaller pore size ?6.8 vs. 7.4 Å—in membranes with the intermediate mesoporous γ‐Al2O3 layer if compared to those without. The three times Si‐B‐C‐N coated multilayer membranes show higher H2/CO permselectivities of about 10.5 and the H2 permeance of about 1.05 × 10?8 mol m?2 s?1 Pa?1. If compared to the state of the art of microporous membranes, the multilayer Si‐B‐C‐N/γ‐Al2O3/α‐Al2O3 membranes are appeared to be interesting candidates for hydrogen separation because of their tunable nature and high‐temperature and high‐pressure stability.  相似文献   

8.
Abstract

Future fossil fuel power generation is likely to include technologies which increase process efficiency and reduce its impact on the environment, for example, CO2 sequestration. Some of the key technologies identified for clean coal and natural gas combustion to produce power or hydrogen or both include O2 generation/separation, H2 and CO2 separation. Hydrogen is considered as a potentially excellent substitute for transport fuels due to the concern over dwindling oil reserves and global warming. This paper discusses various separation processes that may be used in the industrial production of hydrogen from fossil fuels, with an emphasis on membrane separation technologies. Membrane separation has the advantage over other separation methods in that it is simple and potentially less energy intensive. Depending on the particular separation process utilised, however, the membrane materials can differ substantially. The materials used for H2, O2 and CO2 separation are discussed and the major similarities and differences between the membranes highlighted. Critical design aspects of the membrane such as multiple phase design, nano-structure control, the need for surface layers and fabrication processes are also reviewed as they represent the areas where most research and development effort is likely to be directed in the future.  相似文献   

9.
Future fossil fuel power generation is likely to include technologies which increase process efficiency and reduce its impact on the environment, for example, CO2 sequestration. Some of the key technologies identified for clean coal and natural gas combustion to produce power or hydrogen or both include O2 generation/separation, H2 and CO2 separation. Hydrogen is considered as a potentially excellent substitute for transport fuels due to the concern over dwindling oil reserves and global warming. This paper discusses various separation processes that may be used in the industrial production of hydrogen from fossil fuels, with an emphasis on membrane separation technologies. Membrane separation has the advantage over other separation methods in that it is simple and potentially less energy intensive. Depending on the particular separation process utilised, however, the membrane materials can differ substantially. The materials used for H2, O2 and CO2 separation are discussed and the major similarities and differences between the membranes highlighted. Critical design aspects of the membrane such as multiple phase design, nano-structure control, the need for surface layers and fabrication processes are also reviewed as they represent the areas where most research and development effort is likely to be directed in the future.  相似文献   

10.
Most metal–organic‐framework‐ (MOF‐) based hybrid membranes face the challenge of low gas permeability in CO2 separation. This study presents a new strategy of interweaving UiO‐66 and PIM‐1 to build freeways in UiO‐66‐CN@sPIM‐1 membranes for fast CO2 transport. In this strategy, sPIM‐1 is rigidified via thermal treatment to make polymer voids permanent, and concurrently polymer chains are mutually linked onto UiO‐66‐CN crystals to minimize interfacial defects. The pore chemistry of UiO‐66‐CN is kept intact in hybrid membranes, allowing full utilization of MOF pores and selective adsorption for CO2. Separation results show that UiO‐66‐CN@sPIM‐1 membranes possess exceptionally high CO2 permeability (15433.4–22665 Barrer), approaching to that of UiO‐66‐NH2 crystal (65–75% of crystal‐derived permeability). Additionally, the CO2/N2 permeation selectivity for a representative membrane (23.9–28.6) moves toward that of single crystal (24.6–29.6). The unique structure and superior CO2/N2 separation performance make UiO‐66‐CN@sPIM‐1 membranes promising in practical CO2 separations.  相似文献   

11.
Abstract

Enhancing the fluxes in gas separation membranes is required for utilizing the membranes on a mass scale for CO2 capture. Membrane thinning is one of the most promising approaches to achieve high fluxes. In addition, sophisticated molecular transport across membranes can boost gas separation performance. In this review, we attempt to summarize the current state of CO2 separation membranes, especially from the viewpoint of thinning the selective layers and the membrane itself. The gas permeation behavior of membranes with ultimate thicknesses and their future directions are discussed.  相似文献   

12.
Molecular sieving membranes have great potential for energy-saving separations, but they suffer from permeability-selectivity trade-off limitation. In this report, simultaneous hetero-crystallization and hetero-linker coordination of metal–organic framework (MOF) hollow fiber membranes through one-pot synthesis for precise gas separation is reported. It is found that the hetero-polycrystalline membranes consist of 2D and 3D MOF phases and are defect-free and roughly orientated, hetero-linker exchange of 3D phase by larger geometric ones can narrow transport pathway, and framework rigidification occurs and thus fixes MOF channels. The prepared membranes are robust and reproducible, and exhibit substantially improved performance, with H2/CO2, H2/N2, and H2/CH4 selectivities up to 361, 482, and 541, respectively, accompanied by high H2 permeance over 1100 gas permeation units, which can easily outclass trade-off upper bounds of state-of-the-art membranes.  相似文献   

13.
Membrane technology is one of the most promising technologies for separation and purification that is routinely and commercially employed in aqueous solutions. In comparison, its applications in organic solvents are severely underdeveloped mainly due to the poor stability of traditional polymer membranes in organic solvents. The emerging materials such as crosslinked polymers, covalent organic frameworks, metal–organic frameworks, conjugated microporous polymers, carbon molecular sieves, and graphene provide the solutions to address this problem. The membranes constructed with these novel materials show outstanding separation performance in regard to both high selectivity and solvent permeability, greatly pushing forward utilization of membrane technology in organic media. Here, an overview of the most important organic mixtures that need to be separated, the major separation processes adopted nowadays in organic solvents, and the recent progress in new developed membranes is provided.  相似文献   

14.
Covalent organic frameworks (COFs) are porous crystalline polymeric materials formed by the covalent bonding of organic units. The abundant organic units library gives the COFs species diversity, easily tuned pore channels, and pore sizes. In addition, the periodic arrangement of organic units endows COFs regular and highly connected pore channels, which has led to the rapid development of COFs in membrane separations. Continuous defect-free and high crystallinity of COF membranes is the key to their application in separations, which is the most important issue to be addressed in the research. This review article describes the linkage types of covalent bonds, synthesis methods, and pore size regulation strategies of COFs materials. Further, the preparation strategies of continuous COFs membranes are highlighted, including layer-by-layer (LBL) stacking, in situ growth, interfacial polymerization (IP), and solvent casting. The applications in separation fields of continuous COFs membranes are also discussed, including gas separation, water treatment, organic solvent nanofiltration, ion conduction, and energy battery membranes. Finally, the research results are summarized and the future prospect for the development of COFs membranes are outlined. More attention may be paid to the large-scale preparation of COFs membranes and the development of conductive COFs membranes in future research.  相似文献   

15.
Hybrid polyetherimide (PEI)–silica membranes were synthesized. The aim was to obtain improved materials for gas separation media. The inorganic material was prepared via the sol–gel method through the hydrolysis of tetraethoxysilane (TEOS). The influence of the reaction conditions on the final membrane morphology and properties were studied. Scanning electron microscopy (SEM), energy-dispersive X-ray analysis (SEM–EDX), and Fourier transform infrared spectroscopy (FTIR) were used to characterize the PEI and PEI–silica composite membranes. The evolution of TEOS hydrolysis and the condensation processes were verified by FTIR studies. The silica–polymer interaction was also analyzed. The SEM micrographs showed how the membranes distinct morphologies depended upon synthesis parameters and preparation techniques (presence of coupling agent, TEOS polymerization in situ or not, silica content and membranes redissolution). The permeation rates of CO2, CH4, O2, N2, and H2 through the pure polymer and hybrid membranes were measured and showed an increase of gas permeability for hybrid membranes but, the CO2/CH4 and O2/N2 selectivities decreased compared to PEI membranes.  相似文献   

16.
Despite the great advantages of microporous carbons for applications in gas phase separation, liquid phase enrichment, and energy storage devices, direct experiment data and theoretical calculations on the relevance of properties and structures are quite limited. Herein, two model carbon materials are designed and synthesized, i.e., microporous carbon nanosheets (MCN) and microporous carbon spheres (MCS). They both have nearly same composition, surface chemistry, and specific surface area, known morphology, but distinguishable diffusion paths. Based on these two types of materials, a reliable relationship between the morphology with different diffusion paths and adsorption kinetics in both gas phase and liquid phase environments is established. When used for CO2 capture, MCN shows a high saturated CO2 capacity of 8.52 μmol m−2 and 18.4 mmol cm−3 at 273 K and ambient pressure, and its calculated first‐order rate constant is ≈7.4 times higher than that of MCS. Moreover, MCN shows a quick and high uptake of Cr (VI) and a higher‐rate performance for supercapacitors than MCS does. These results strongly confirm that MCN exhibits improved kinetics in gas phase separation, liquid phase enrichment, and energy storage devices due to its shorter diffusion paths and larger exposed geometrical area resulting from the nanosheet structure.  相似文献   

17.
Pure bone material obtained from cow meat, as apatite-rich material, and TiO2-bone composite materials are prepared and studied to be used for heavy metal ions separation from waste water solutions. Meat wastes are chemically and thermally treated to control their microstructure in order to prepare the composite materials that fulfill all the requirements to be used as selective membranes with high performance, stability and mechanical strength. The prepared materials are analyzed using Hg-porosimetry for surface characterization, energy dispersive X-ray spectroscopy (EDAX) for elemental analysis and Fourier transform infrared spectroscopy (FTIR) for chemical composition investigation. Structural studies are performed using X-ray diffraction (XRD). Microstructural properties are studied using scanning electron microscopy (SEM) and specific surface area studies are performed using Brunauer-Emmet-Teller (BET) method. XRD studies show that multiphase structures are obtained as a result of 1h sintering at 700?C1200 °C for both pure bone and TiO2-bone composite materials. The factors affecting the transport of different heavy metal ions through the selected membranes are determined from permeation flux measurements. It is found that membrane pore size, membrane surface roughness and membrane surface charge are the key parameters that control the transport or rejection of heavy metal ions through the selected membranes.  相似文献   

18.
2D materials hold promising potential for novel gas separation. However, a lack of in‐plane pores and the randomly stacked interplane channels of these membranes still hinder their separation performance. In this work, ferrocene based‐MOFs (Zr‐Fc MOF) nanosheets, which contain abundant of in‐plane micropores, are synthesized as porous supports to fabricate Zr‐Fc MOF supported ionic liquid membrane (Zr‐Fc‐SILM) for highly efficient CO2 separation. The micropores of Zr‐Fc MOF nanosheets not only provide extra paths for CO2 transportation, and thus increase its permeance up to 145.15 GPU, but also endow the Zr‐Fc‐SILM with high selectivity (216.9) of CO2/N2 through the nanoconfinement effect, which is almost ten times higher than common porous polymer SILM. Furthermore, based on the photothermal‐responsive properties of Zr‐Fc MOF, the performance is further enhanced (35%) by light irradiation through a photothermal heating process. This provides a brand new way to design light facilitating gas separation membranes.  相似文献   

19.
The permeability properties of a new type of silica membrane for the small gas molecules CO2, CO, Ne, CH4, He, and H2 are presented. The new membrane, denoted as Nanosil, has unusually high permeance for H2, but also allows passage of He and to a smaller extent Ne, while excluding all other molecules. The membrane is formed by the decomposition of a silica precursor (tetraethyl orthosilicate) onto a Vycor glass substrate. Nitrogen physisorption isotherms of the Vycor glass substrate indicate that it is a microporous solid with slit-like pores of 3.6 nm diameter, that remains unchanged after the silica deposition. Atomic force microscopy (AFM) shows that the Vycor substrate is made up of rectangular plate-like elements of size 90 nm × 30 nm. Between the plates are found rectangular features of 4 nm breadth which are likely to be the pore mouths. The deposited silica forms a thin layer on top of these plates so as to erase fine structures and increase the average feature size to 110 nm × 50 nm.  相似文献   

20.
With increasing oil spill accidents, the development of effective and low-cost adsorbents with good hydrophobicity is highly desirable. To cope with the clean-up of oil spill, a hydrophobic adsorbent was synthesized by electrospinning using inexpensive raw materials. By ingeniously combining melamine with polyacrylonitrile (PAN) as well as SiO2 nanoparticles, a novel composite nanoadsorbent named SiO2@MUF/PAN nanofibrous membrane was prepared and characterized. The adsorbents were conducted based on uniform nanofibre networks and were abundant with narrow slit-like pores, which are significant for the retention of oil and organic solvents. The hydrophobicity of the as-prepared membranes was enhanced with an increasing amount of SiO2, and the highest water contact angle was 128.3°. Furthermore, the combination of SiO2 and melamine increased the thermal stability of the membranes. With the unique pore structures and hydrophobicity, the membranes were able to selectively remove not only oil but also organic solvents from water surface. The adsorption capacities of the membranes with SiO2 nanoparticles (0.9 wt%) were the highest and that for peanut oil, diesel, pump oil and engine oil were 19.09, 13.12, 18.48 and 22.67 g g?1, respectively, while that for organic solvents ranged from 12.92 to 22.16 g g?1. After 10 adsorption–regeneration cycles, the adsorption capacity was still around 35% of the initial value. Due to its high oil adsorption capacity, excellent reusability and the cost-effective hydrophobic, SiO2@MUF/PAN have a great potential for oil spill clean-up.  相似文献   

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