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Title: Nuclear quantum effects on adsorption of H 2 and isotopologues on metal ions

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.
Authors:
 [1] ;  [2] ;  [3] ;  [4] ;  [5]
  1. Jacobs University, Bremen (Germany). School of Engineering and Science
  2. Univ. of Rochester, NY (United States). Department of Chemistry
  3. Leipzig University (Germany). Wilhelm-Ostwald-Institute of Physical and Theoretical Chemistry
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science, and Computer Science and Mathematics Division
  5. University of South Carolina, Columbia, SC (United States). Department of Chemistry and Biochemistry
Publication Date:
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Chemical Physics Letters
Additional Journal Information:
Journal Volume: 670; Journal Issue: C; Journal ID: ISSN 0009-2614
Publisher:
Elsevier
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
36 MATERIALS SCIENCE; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
OSTI Identifier:
1338543