Hydride ions in oxide hosts hidden by hydroxide ions.

Hayashi, Katsuro; Sushko, Peter V; Hashimoto, Yasuhiro; Shluger, Alexander L; Hosono, Hideo · Nat Commun · 2014

basic_science · Level V

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Abstract

The true oxidation state of formally 'H(-)' ions incorporated in an oxide host is frequently discussed in connection with chemical shifts of (1)H nuclear magnetic resonance spectroscopy, as they can exhibit values typically attributed to H(+). Here we systematically investigate the link between geometrical structure and chemical shift of H(-) ions in an oxide host, mayenite, with a combination of experimental and ab initio approaches, in an attempt to resolve this issue. We demonstrate that the electron density near the hydrogen nucleus in an OH(-) ion (formally H(+) state) exceeds that in an H(-) ion. This behaviour is the opposite to that expected from formal valences. We deduce a relationship between the chemical shift of H(-) and the distance from the H(-) ion to the coordinating electropositive cation. This relationship is pivotal for resolving H(-) species that are masked by various states of H(+) ions.