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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.

権利情報:

• Creative Commons BY Attribution 4.0 International
  

キーワード: ammonia synthesis, oxyhydride, mechanochemical synthesis

刊行年月日: 2024-08-03

出版者: Wiley

掲載誌:

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

研究助成金:

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

原稿種別: 出版者版 (Version of record)

MDR DOI:

公開URL: https://doi.org/10.1002/aenm.202402353

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更新時刻: 2025-02-23 22:47:36 +0900

MDRでの公開時刻: 2025-02-23 22:47:36 +0900