Low-Temperature Synthesis of Perovskite Oxynitride-Hydrides as Ammonia Synthesis Catalysts

Masaaki Kitano, Jun Kujirai, Kiya Ogasawara, Satoru Matsuishi, Tomofumi Tada, Hitoshi Abe, Yasuhiro Niwa, Hideo Hosono

研究成果: ジャーナルへの寄稿記事

抜粋

Mixed anionic materials such as oxyhydrides and oxynitrides have recently attracted significant attention due to their unique properties, such as fast hydride ion conduction, enhanced ferroelectrics, and catalytic activity. However, high temperature (≥800 °C) and/or complicated processes are required for the synthesis of these compounds. Here we report that a novel perovskite oxynitride-hydride, BaCeO3-xNyHz, can be directly synthesized by the reaction of CeO2 with Ba(NH2)2 at low temperatures (300-600 °C). BaCeO3-xNyHz, with and without transition metal nanoparticles, functions as an efficient catalyst for ammonia synthesis through the lattice N3- and H- ion-mediated Mars-van Krevelen mechanism, while ammonia synthesis occurs over conventional catalysts through a Langmuir-Hinshelwood mechanism with high energy barriers (85-121 kJ mol-1). As a consequence, the unique reaction mechanism leads to enhancement of the activity of BaCeO3-based catalysts by a factor of 8-218 and lowers the activation energy (46-62 kJ mol-1) for ammonia synthesis. Furthermore, isotopic experiments reveal that this catalyst shifts the rate-determining step for ammonia synthesis from N2 dissociation to N-H bond formation.

元の言語英語
ページ(範囲)20344-20353
ページ数10
ジャーナルJournal of the American Chemical Society
141
発行部数51
DOI
出版物ステータス出版済み - 12 26 2019

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All Science Journal Classification (ASJC) codes

  • Catalysis
  • Chemistry(all)
  • Biochemistry
  • Colloid and Surface Chemistry

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