Theoretical prediction by DFT and experimental observation of heterocation-doping effects on hydrogen adsorption and migration over the CeO2(111) surface

Kota Murakami, Yuta Mizutani, Hiroshi Sampei, Atsushi Ishikawa, Yuta Tanaka, Sasuga Hayashi, Sae Doi, Takuma Higo, Hideaki Tsuneki, Hiromi Nakai, Yasushi Sekine

Research output: Contribution to journalArticlepeer-review

Abstract

Hydrogen (H) atom adsorption and migration over the CeO2-based materials surface are of great importance because of its wide applications to catalytic reactions and electrochemical devices. Therefore, comprehensive knowledge for controlling the H atom adsorption and migration over CeO2-based materials is crucially important. For controlling H atom adsorption and migration, we investigated irreducible divalent, trivalent, and quadrivalent heterocation-doping effects on H atom adsorption and migration over the CeO2(111) surface using density functional theory (DFT) calculations. Results revealed that the electron-deficient lattice oxygen (Olat) and the flexible CeO2matrix played key roles in strong adsorption of H atoms. Heterocations with smaller valence and smaller ionic radius induced the electron-deficient Olat. In addition, smaller cation doping enhanced the CeO2matrix flexibility. Moreover, we confirmed the influence of H atom adsorption controlled by doping on surface proton migration (i.e.surface protonics) and catalytic reaction involving surface protonics (NH3synthesis in an electric field). Results confirmed clear correlation between H atom adsorption energy and surface protonics.

Original languageEnglish
Pages (from-to)4509-4516
Number of pages8
JournalPhysical Chemistry Chemical Physics
Volume23
Issue number8
DOIs
Publication statusPublished - 2021 Feb 28

ASJC Scopus subject areas

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

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