Metal‐Dependent Support Effects of Oxyhydride‐Supported Ru, Fe, Co Catalysts for Ammonia Synthesis

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  • Ya Tang
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Yoji Kobayashi
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Naoya Masuda
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Yoshinori Uchida
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Hiroki Okamoto
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Toki Kageyama
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Saburo Hosokawa
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • François Loyer
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Kei Mitsuhara
    SR Center Ritsumeikan University Kusatsu Shiga 525‐8577 Japan
  • Keisuke Yamanaka
    SR Center Ritsumeikan University Kusatsu Shiga 525‐8577 Japan
  • Yusuke Tamenori
    Japan Synchrotron Radiation Research Institute (JASRI) Sayo Hyogo 679‐5198 Japan
  • Cédric Tassel
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Takafumi Yamamoto
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Tsunehiro Tanaka
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan
  • Hiroshi Kageyama
    Graduate School of Engineering Kyoto University Nishikyo‐ku Kyoto 615‐8510 Japan

書誌事項

公開日
2018-11-08
資源種別
journal article
権利情報
  • http://onlinelibrary.wiley.com/termsAndConditions#am
  • http://onlinelibrary.wiley.com/termsAndConditions#vor
DOI
  • 10.1002/aenm.201801772
公開者
Wiley

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説明

<jats:title>Abstract</jats:title><jats:p>Ammonia is an attractive energy carrier for the hydrogen economy, given its high hydrogen density and ease of liquefaction. A titanate oxyhydride has recently been demonstrated that can catalyze ammonia synthesis without Ru or Fe metal, despite titanium being regarded as an inert element. Here, the synthesis activity of ammonia is examined when Ru, Fe, and Co particles are supported onto the oxyhydride BaTiO<jats:sub>2.5</jats:sub>H<jats:sub>0.5</jats:sub>. The activity of BaTiO<jats:sub>2.5</jats:sub>H<jats:sub>0.5</jats:sub> as support is significantly higher than BaTiO<jats:sub>3</jats:sub>. For example, the activity for Fe and Co increases by a factor of 70–400, making them more active than Ru/MgO, one conventional Ru catalyst. In terms of mechanism, for Ru, H/D isotope studies show participation of lattice hydride in the catalytic cycle, while kinetic analysis shows reduced H<jats:sub>2</jats:sub> poisoning probably due to spillover. For Fe (and Co), the presence of hydride results in significantly lower activation energy and N<jats:sub>2</jats:sub> reaction order, likely due to strong electron donation from the oxyhydride. This metal‐dependent support effect is further verified by N<jats:sub>2</jats:sub> isotopic exchange experiments. These perovskite‐type oxyhydrides can be easily modified in terms of <jats:italic>A</jats:italic>‐ and <jats:italic>B</jats:italic>‐site (<jats:italic>A</jats:italic> = Ba, <jats:italic>B</jats:italic> = Ti); the high potential for compositional variation and morphologies will expand the search for efficient catalysts for ammonia synthesis.</jats:p>

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