Nuclear quantum effects on adsorption of H2 and isotopologues on metal ions

Savchenko, Ievgeniia; Gu, Bing; Heine, Thomas; Jakowski, Jacek; Garashchuk, Sophya

doi:10.1016/j.cplett.2016.12.069

Nuclear quantum effects on adsorption of H₂ and isotopologues on metal ions

Journal Article · Mon Jan 02 23:00:00 EST 2017 · Chemical Physics Letters

DOI:https://doi.org/10.1016/j.cplett.2016.12.069· OSTI ID:1338543

Savchenko, Ievgeniia ^[1]; Gu, Bing ^[2]; Heine, Thomas ^[3]; Jakowski, Jacek ^[4]; Garashchuk, Sophya ^[5]

Jacobs University, Bremen (Germany). School of Engineering and Science
Univ. of Rochester, NY (United States). Department of Chemistry
Leipzig University (Germany). Wilhelm-Ostwald-Institute of Physical and Theoretical Chemistry
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science, and Computer Science and Mathematics Division
University of South Carolina, Columbia, SC (United States). Department of Chemistry and Biochemistry

The nuclear quantum effects on the zero-point energy (ZPE), influencing adsorption of H$$_2$$ and isotopologues on metal ions, are examined in this study using normal mode analysis of ab initio electronic structure results for complexes with 17 metal cations. To estimate for the anharmonicity, a nuclear wavepacket dynamics on the ground state electronic potential energy surfaces (PES) have been employed for complexes of Li$^+$ and Cu$$^{+2}$$ with H$$_2$$, D$$_2$$, HD. The dynamics analysis shows that incorporation of the PES anharmonicity changes the ZPE by up to 9%. Finally, the lightest metallic nuclei, Li and Be, are found to be the most 'quantum'. The largest selectivity in adsorption is predicted for Cu, Ni and Co ions.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1338543

Journal Information:: Chemical Physics Letters, Journal Name: Chemical Physics Letters Journal Issue: C Vol. 670; ISSN 0009-2614

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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An assessment of strategies for the development of solid-state adsorbents for vehicular hydrogen storage Allendorf, Mark D.; Hulvey, Zeric; Gennett, Thomas Energy & Environmental Science, Vol. 11, Issue 10 https://doi.org/10.1039/c8ee01085d	journal	January 2018
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