Effects of A-site composition of perovskite (Sr1−xBaxZrO3) oxides on H atom adsorption, migration, and reaction

Yuta Tanaka, Kota Murakami, Sae Doi, Kazuharu Ito, Koki Saegusa, Yuta Mizutani, Sasuga Hayashi, Takuma Higo, Hideaki Tsuneki, Hiromi Nakai, Yasushi Sekine

Research output: Contribution to journalArticlepeer-review

Abstract

Hydrogen (H) atomic migration over a metal oxide is an important surface process in various catalytic reactions. Control of the interaction between H atoms and the oxide surfaces is therefore important for better catalytic performance. For this investigation, we evaluated the adsorption energies of the H atoms over perovskite-type oxides (Sr1−xBaxZrO3; 0.00 ≤x≤ 0.50) using DFT (Density Functional Theory) calculations, then clarified the effects of cation-substitution in the A-site of perovskite oxides on H atom adsorption, migration, and reaction. Results indicated local distortion at the oxide surface as a key factor governing H atom adsorption. Subtle Ba2+substitution for Sr2+sites provoked local distortion at the Sr1−xBaxZrO3oxide surface, which led to a decrement in the H atom adsorption energy. Furthermore, the effect of Sr2+/Ba2+ratio on the H atoms' reactivities was examined experimentally using a catalytic reaction, which was promoted by activated surface H atoms. Results show that the surface H atoms activated by the substitution of Sr2+sites with a small amount of Ba2+(x= 0.125) contributed to enhancement of ammonia synthesis rate in an electric field, which showed good agreement with predictions made using DFT calculations.

Original languageEnglish
Pages (from-to)7621-7626
Number of pages6
JournalRSC Advances
Volume11
Issue number13
DOIs
Publication statusPublished - 2021 Feb 17

ASJC Scopus subject areas

  • Chemistry(all)
  • Chemical Engineering(all)

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