期刊
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 144, 期 31, 页码 14322-14329出版社
AMER CHEMICAL SOC
DOI: 10.1021/jacs.2c05448
关键词
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资金
- National Key R&D Program of China [2017YFE0301504]
- National Natural Science Foundation of China [21878261, 21890764]
- Zhejiang Provincial Natural Science Foundation of China [LR21B060002]
- state of Schleswig-Holstein, Germany
This study demonstrates a strategy to refine the pore structure of metal-organic frameworks by tuning the size and number of polycycloalkane-dicarboxylate ligands, leading to improved separation efficiency for structurally similar molecules. The resulting materials exhibit excellent performance in the separation of alkane mixtures and Xe/Kr mixtures.
The fine-tuning of the pore structure of metal-organic frameworks (MOFs) is of critical importance to developing energy-efficient processes for the challenging separation of structurally similar molecules. Herein, we demonstrate a strategy to realize a quasi-three-dimensional refinement of the pore structure that utilizes the tunability of ring size and number in polycycloalkane-dicarboxylate ligands. Two hydrolytically stable MOFs with a confined aliphatic pore environment, ZUL-C1 and ZUL-C2, were, for the first time, synthesized and applied in separating low-concentration C2-C3 hydrocarbons from natural gas and ultralow-concentration Xe from used nuclear fuel (UNF) off-gas. Validated by X-ray diffraction and modeling, an expansion of the polycycloalkane moiety enables sub-angstrom contraction in specific directions and forms a pore surface with more alkyl sites, which affords stronger trapping of guest molecules with relatively higher polarizability. The resultant material exhibits record C2H(6)/CH4 and C3H8/CH4 selectivities coupled with a benchmark low-pressure C2H6 capacity in alkane mixture separation and also a benchmark Xe capacity at extremely diluted feed concentration and record Kr productivity for the Xe/Kr (20:80, v/v) mixture in Xe/Kr separation.
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