期刊
JOURNAL OF CHEMICAL PHYSICS
卷 141, 期 6, 页码 -出版社
AMER INST PHYSICS
DOI: 10.1063/1.4892670
关键词
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资金
- European Research Council (ERC-StG) [GA 256962]
- Deutsche Forschungsgemeinschaft (DFG) [GA HE 3543/7-2]
The role of nuclear quantum effects on the adsorption of molecular hydrogen in metal-organic frameworks (MOFs) has been investigated on grounds of Grand-Canonical Quantized Liquid Density-Functional Theory (GC-QLDFT) calculations. For this purpose, we have carefully validated classical H-2-host interaction potentials that are obtained by fitting Born-Oppenheimer ab initio reference data. The hydrogen adsorption has first been assessed classically using Liquid Density-Functional Theory and the Grand-Canonical Monte Carlo methods. The results have been compared against the semi-classical treatment of quantum effects by applying the Feynman-Hibbs correction to the Born-Oppenheimer-derived potentials, and by explicit treatment within the GC-QLDFT. The results are compared with experimental data and indicate pronounced quantum and possibly many-particle effects. After validation calculations have been carried out for IRMOF-1 (MOF-5), GC-QLDFT is applied to study the adsorption of H-2 in a series of MOFs, including IRMOF-4, -6, -8, -9, -10, -12, -14, 16, -18, and MOF-177. Finally, we discuss the evolution of the H2 quantum fluid with increasing pressure and lowering temperature. (C) 2014 AIP Publishing LLC.
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