期刊
CHEMISTRY OF MATERIALS
卷 31, 期 15, 页码 5856-5866出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.chemmater.9b01995
关键词
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资金
- MINECO (Spain) [CTQ2016-75671-P, MAT2017-86992-R, MAT-80285-P]
- Excellence Unit Maria de Maeztu [MDM-2015-0538]
- Ministero dell'Istruzione, dell'Universita e della Ricerca (Italy)
- MINECO
- MIUR (project PON R&I FSE-FESR 2014-2020)
- European Research Council under the European Union's Horizon 2020 research and innovation programme/ERC grant [814804]
Understanding/visualizing the established interactions between gases and adsorbents is mandatory to implement better performance materials in adsorption/separation processes. Here we report the unique behavior of a rare example of a hemilabile chiral three-dimensional metal-organic framework (MOF) with an unprecedented qtz-e-type topology, with formula Cu-2(II)(S,S)-hismox center dot 5H(2)O (1) (hismox = bis[(S)-histidine]oxalyl diamide). 1 exhibits a continuous and reversible breathing behavior, based on the hemilability of carboxylate groups from L-histidine. In situ powder (PXRD) and single crystal X-ray diffraction (SCXRD) using synchrotron radiation allowed us to unveil the crystal structures of four different host-guest adsorbates (Ar@1, N-2@1, CO2@1, and C3H6@1), rationalize the breathing motion, and unravel the mechanisms governing the adsorption of these gases. Then this information was transferred to implement efficient separations of mixtures of industrial and environmental relevance, CO2/N-2, CO2/CH4, and C3H8/C3H6, using 1 in packed columns as the stationary phase and dispersed in a mixed matrix membrane.
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