期刊
CHEMICAL SCIENCE
卷 9, 期 20, 页码 4579-4588出版社
ROYAL SOC CHEMISTRY
DOI: 10.1039/c8sc00971f
关键词
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资金
- Swiss National Science Foundation [PYAPP2_160581]
- Swiss Commission for Technology and Innovation (CTI)
- National Center of Competence in Research (NCCR) Materials' Revolution: Computational Design and Discovery of Novel Materials (MARVEL) of the Swiss National Science Foundation (SNSF)
- Center for Gas Separations Relevant to Clean Energy Technologies, an Energy Frontier Research Center - U.S. Department of Energy, Office of Science, Basic Energy Sciences [DE-SC0001015]
- National Science Foundation [DGE 1106400]
- Office of Science of the U.S. Department of Energy [DE-AC02-05CH11231]
We present a comprehensive investigation of the CO2 adsorption properties of an isostructural series of metal-organic frameworks, M-BTT (M 1/4 Cr, Mn, Fe, Cu; BTT3 = 1/4 1,3,5-benzenetristetrazolate), which exhibit a high density of open metal sites capable of polarizing and binding guest molecules. Coupling gas adsorption measurements with in situ neutron and X-ray diffraction experiments provides molecularlevel insight into the adsorption process and enables rationalization of the observed adsorption isotherms. In particular, structural data confirms that the high initial isosteric heats of CO2 adsorption for the series are directly correlated with the presence of open metal sites and further reveals the positions and orientations of as many as three additional adsorption sites. Density functional theory calculations that include van der Waals dispersion corrections quantitatively support the observed structural features associated with the primary and secondary CO2 binding sites, including CO2 positions and orientations, as well as the experimentally determined isosteric heats of CO2 adsorption.
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