Hydrogen adsorption in metal-organic frameworks: the role of nuclear quantum effects
| Autor: | Mohammad Wahiduzzaman, Thomas Heine, Christian F. J. Walther |
|---|---|
| Rok vydání: | 2014 |
| Předmět: |
Chemical Physics (physics.chem-ph)
Quantum fluid Materials science Hydrogen Born–Oppenheimer approximation Ab initio FOS: Physical sciences General Physics and Astronomy chemistry.chemical_element 02 engineering and technology 010402 general chemistry 021001 nanoscience & nanotechnology 01 natural sciences 0104 chemical sciences symbols.namesake Adsorption chemistry Ab initio quantum chemistry methods Quantum mechanics Physics - Chemical Physics symbols Density functional theory Physical and Theoretical Chemistry 0210 nano-technology Quantum |
| Zdroj: | The Journal of chemical physics. 141(6) |
| ISSN: | 1089-7690 |
| Popis: | 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 H2 -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 (LDFT) and the Grand-Canonical Monte Carlo (GCMC) 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 Grand-Canonical Quantized Liquid Density-Functional Theory (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 H2 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. |
| Databáze: | OpenAIRE |
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