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Description:

Oxyhydrides have attracted attention as materials with various unique properties derived from lattice hydride ions (H−). However, their instability makes synthesis by conventional thermal synthesis methods difficult, so an appropriate synthesis strategy is required. Here, the mechanochemical synthesis of perovskite oxyhydrides BaREO2H (RE = Y, Sc) for catalyst applications is reported. The formation of BaYO2H is known to be thermodynamically unstable; however, a mechanochemical process that inevitably proceeds under non-equilibrium conditions enables the synthesis of such a metastable oxyhydride material without any heat treatment. Furthermore, BaScO2H, which is typically obtained at very high temperatures (1000 °C) and pressure (>4 GPa), is successfully synthesized at room temperature by the mechanochemical method. The ammonia synthesis reaction over these oxyhydrides supporting Ru is significantly enhanced at low temperatures, and the ammonia synthesis rates are significantly higher than conventional oxide-supported Ru catalysts. The mechanochemically synthesized BaREO2H has many anionic electrons with low work function at the site of H− vacancies, which enables strong electron donation to Ru and the storage of excess hydrogen adatoms from the Ru surface, which results in high catalytic performance.

Rights:

• Creative Commons BY Attribution 4.0 International
  

Keyword: ammonia synthesis, oxyhydride, mechanochemical synthesis

Date published: 2024-08-03

Publisher: Wiley

Journal:

• Advanced Energy Materials (ISSN: 16146832) vol. 14 issue. 47 2402353

Funding:

• JST JPMJMI21E9 (JST-Mirai Program)
• JST JPMJFR203A (FOREST Program)
• JST JPMJSP2106 (JST SPRING)
• JSPS JP22H00272 (Kakenhi Grant-in-Aid)
• Tokyo Tech Fund (Tokyo Tech Advanced Researchers Grant)
• JSPS JP24H02204 (Kakenhi Grant-in-Aid)

Manuscript type: Publisher's version (Version of record)

MDR DOI:

First published URL: https://doi.org/10.1002/aenm.202402353

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Updated at: 2025-02-23 22:47:36 +0900

Published on MDR: 2025-02-23 22:47:36 +0900