期刊
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
卷 60, 期 42, 页码 22865-22870出版社
WILEY-V C H VERLAG GMBH
DOI: 10.1002/anie.202107963
关键词
acetylene adsorption; boron clusters; C2H2; CO2 separation; synergistic interaction; ultramicroporous MOFs
资金
- Natural Science Foundation of China [21908193, 21938011, 21725603]
The study presents a new type of dodecaborate-pillared MOF material ZNU-1 for selective separation of C2H2 from CO2, achieving high capacity and selectivity, optimal pore chemistry, and exceptional separation performance with high efficiency.
The separation of C2H2/CO2 is an important process in industry but challenged by the trade-off of capacity and selectivity owning to their similar physical properties and identical kinetic molecular size. We report the first example of symmetrically interpenetrated dodecaborate pillared MOF, ZNU-1, for benchmark selective separation of C2H2 from CO2 with a high C2H2 capacity of 76.3 cm(3) g(-1) and record C2H2/CO2 selectivity of 56.6 (298 K, 1 bar) among all the robust porous materials without open metal sites. Single crystal structure analysis and modeling indicated that the interpenetration shifting from asymmetric to symmetric mode provided optimal pore chemistry with ideal synergistic 2+2 dihydrogen bonding sites for tight C2H2 trapping. The exceptional separation performance was further evidenced by simulated and experimental breakthroughs with excellent recyclability and high productivity (2.4 mol kg(-1)) of 99.5 % purity C2H2 during stepped desorption process.
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