| 利用水热二次生长法制备用于H2/CO2分离的KAUST-8膜 |
| 作者：asad sharif， 王泓博， 鲁金明， 杨建华， 刘毅 |
| 单位： 大连理工大学 吸附与无机膜研究所， 精细化工国家重点实验室 |
| 关键词： CO2分离； KAUST-8膜； 氟化金属有机框架膜； 水热合成； H2纯化 |
| DOI号： 10.16159/j.cnki.issn1007-8924.2024.05.011 |
| 分类号： TQ028.8 |
| 出版年,卷(期):页码： 2024,44(5):90-99 |
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摘要： |
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KAUST-8纳米片比表面积和孔隙率较高、铝金属位点丰富，因此具有出色的二氧化碳吸附能力.在本研究中，采用水热二次生长技术，在粗糙的大孔α-Al2O3载体管上，引入氧化铝和硝酸镍作为前驱体，其中，Al2O3用于控制无机支柱\[AlF5(H2O)\]2-的生长，Ni(NO3)2·6H2O用于提高金属前驱体镍源在溶剂中的溶解度，促进 Ni(Ⅱ)吡嗪方格的形成，并与无机柱中心\[AlF5(H2O)\]2-反应，合成了多晶KAUST-8膜.并进一步探讨了反应物浓度、时间、温度等合成条件以及溶剂对KAUST-8膜性能的影响.优化后的 KAUST-8膜的H2渗透率为1.27×10-7 mol/(m2·s·Pa）（25 ℃、 0.1 MPa条件下），H2/CO2的理想选择性为19.3. |
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KAUST-8 nanosheets exhibit high surface area and pore volume, leading to exceptional CO2 adsorption due to Al metal sites. In this study, polycrystalline KAUST-8 membranes were developed using a hydrothermal secondary growth technique on coarse microporous α-Al2O3 tube supports, employing aluminum oxide and nickel nitrate precursors. Al2O3 was to control the growth of inorganic pillar \[AlF5(H2O)\]2- and Ni(NO3)2·6H2O for its enhanced solubility of precursor nickel sources, to form Ni(Ⅱ)-pyrazine square grids which reacted with the pillar to grow KAUST-8 crystals. Additionally, water was used as a solvent to promote membrane growth. Moreover, the synthesis conditions of reactant concentration, time, temperature, and effects of solvents were explored. The resulting optimized KAUST-8 membrane demonstrated H2 permeance rate of 1.27×10-7 mol/(m2·s·Pa） (at 25 ℃ and 0.1 MPa) and ideal selectivity of H2/CO2 of 19.3. |
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基金项目： |
| 国家自然科学基金项目（21776031, 22378044) |
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作者简介： |
| Asad Sharif（1995-），男，巴基斯坦人，硕士生，从事MOF膜的制备与应用.*通讯作者，E-mail：ljinming@dlut.edu.cn |
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参考文献： |
| ［1］Sholl D S, Lively R P. Seven chemical separations to change the world \[J\]. Nature, 2016, 532(7600): 435-437. \[2\]Dziejarski B, Krzyzyńska R, Andersson K. Current status of carbon capture, utilization, and storage technologies in the global economy: A survey of technical assessment \[J\]. Fuel, 2023, 342: 127776. \[3\] Awwad M, Bilal M, Sajid M, et al. MOF-based membranes for oil/water separation: Status, challenges, and prospects\[J\]. J Environ Chem Eng, 2023, 11(1): 109073. \[4\]Kitagawa S. Metalorganic frameworks (MOFs)\[J\]. Chem Soc Rev, 2014, 43(16): 5415-5418. \[5\] Yaghi O M, Li G, Li H. Selective binding and removal of guests in a microporous metalorganic framework\[J\]. Nature, 1995, 378(6558): 703-706. \[6\]Eddaoudi M, Kim J, Rosi N, et al. Systematic design of pore size and functionality in isoreticular MOFs and their application in methane storage \[J\]. Science, 2002, 295(5554): 469-472. \[7\]Furukawa H, Ko N, Go Y B, et al. Ultrahigh porosity in metalorganic frameworks\[J\]. Science, 2010, 329(5990): 424-428. \[8\]Ma S, Zhou H C. Gas storage in porous metal-organic frameworks for clean energy applications \[J\]. Chem Commun, 2010, 46(1): 44-53. \[9\]Chakraborty G, Park I H, Medishetty R, et al. Two-dimensional metal-organic framework materials: Synthesis, structures, properties and applications \[J\]. Chem Rev, 2021, 121(7): 3751-3891. \[10\]Song Y, Sun Y, Du D, et al. Fabrication of coriented ultrathin TCPP-derived 2D MOF membrane for precise molecular sieving \[J\]. J Membr Sci, 2021, 634: 119393. \[11\]Pan Y, Lai Z. Sharp separation of C2/C3 hydrocarbon mixtures by zeolitic imidazolate framework8 (ZIF8) membranes synthesized in aqueous solutions\[J\]. Chem Commun, 2011, 47(37): 10275-10277. \[12\]Wei R, Chi H Y, Li X, et al. Aqueously cathodic deposition of ZIF-8 membranes for superior propylene/propane separation\[J\]. Adv Funct Mater, 2020, 30(7): 1907089. \[13\]Moon J D, Freeman B D, Hawker C J, et al. Can selfassembly address the permeability/selectivity tradeoffs in polymer membranes?\[J\]. ACS Publ, 2020, 53: 5649-5654. \[14\]Hao J, Babu D J, Liu Q, et al. Synthesis of highperformance polycrystalline metal-organic framework membranes at room temperature in a few minutes\[J\]. J Mater Chem A, 2020, 8(16): 7633-7640. \[15\]Liu Y, Ng Z, Khan E A, et al. Synthesis of continuous MOF5 membranes on porous αalumina substrates\[J\]. Microporous and Mesoporous Mater, 2009, 118(1): 296-301. \[16\]Jeazet H B T, Staudt C, Janiak C. Metalorganic frameworks in mixedmatrix membranes for gas separation \[J\]. Dalton Trans, 2012, 41(46): 14003-14027. \[17\]Cadiau A, Belmabkhout Y, Adil K, et al. Hydrolytically stable fluorinated metalorganic frameworks for energyefficient dehydration \[J\]. Science, 2017, 356(6339): 731-735. \[18\]Lyu J, Zhou X, Yang J, et al. Insitu synthesis of KAUST7 membranes from fluorinated molecular building block for H2/CO2 separation\[J\]. J Membr Sci, 2022, 658: 120585. \[19\]Tchalala M, Bhatt P, Chappanda K, et al. Fluorinated MOF platform for selective removal and sensing of SO2 from flue gas and air \[J\]. Nat Commun, 2019, 10(1): 1328. \[20\]Georgiadis A G, Charisiou N, Yentekakis I V, et al. Hydrogen sulfide (H2S) removal via MOFs\[J\]. Materials, 2020, 13(16): 3640. \[21\]Datta S J, Mayoral A, Murthy S B N, et al. Rational design of mixedmatrix metal-organic framework membranes for molecular separations\[J\]. Science, 2022, 376(6597): 1080-1087. \[22\]Hou R, Wang S, Wang L, et al. Enhanced CO2 separation performance by incorporating KAUST8 nanosheets into crosslinked poly (ethylene oxide) membrane\[J\]. Sep Purif Technol, 2023, 309: 123057. \[23\]Zhou S, Shekhah O, Jin T, et al. A CO2-recognition metal-organic framework membrane for continuous carbon capture\[J\]. Chem, 2023, 9(5): 1182-1194. \[24\]Huang A, Bux H, Steinbach F, et al. Molecular‐sieve membrane with hydrogen permselectivity: ZIF22 in LTA topology prepared with 3‐aminopropyltriethoxysilane as covalent linker \[J\]. Angew Chem Int Ed, 2010, 29(49): 4958-4961. \[25\]Zhou S, Zou X, Sun F, et al. Challenging fabrication of hollow ceramic fiber supported Cu3(BTC)2 membrane for hydrogen separation \[J\]. J Mater Chem, 2012, 22(20): 10322-10328. \[26\]Nian P, Cao Y, Li Y, et al. Preparation of a pure ZIF-67 membrane by self-conversion of cobalt carbonate hydroxide nanowires for H2 separation\[J\]. Cryst Eng Comm, 2018, 20(17): 2440-2448. \[27\]Liu J, Liu C, Huang A. Cobased zeolitic imidazolate framework ZIF-9 membranes prepared on α-Al2O3 tubes through covalent modification for hydrogen separation\[J\]. Int J Hydro Energy, 2020, 45(1): 703-711. \[28\]Lyu J, Cui Y, Yang J, et al. Inorganic pillar centerfacilitated counterdiffusion synthesis for highly H2 perm-selective KAUST7 membranes\[J\]. ACS Appl Mater Interfaces, 2022, 14(3): 4297-4306. |
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