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Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis

Author

Listed:
  • Masaaki Kitano

    (Materials Research Center for Element Strategy, Tokyo Institute of Technology)

  • Shinji Kanbara

    (Materials and Structures Laboratory, Tokyo Institute of Technology)

  • Yasunori Inoue

    (Materials and Structures Laboratory, Tokyo Institute of Technology)

  • Navaratnarajah Kuganathan

    (University College London)

  • Peter V. Sushko

    (Fundamental and Computational Sciences Directorate, Pacific Northwest National Laboratory
    ACCEL, Japan Science and Technology Agency)

  • Toshiharu Yokoyama

    (Materials Research Center for Element Strategy, Tokyo Institute of Technology
    ACCEL, Japan Science and Technology Agency)

  • Michikazu Hara

    (Materials and Structures Laboratory, Tokyo Institute of Technology
    ACCEL, Japan Science and Technology Agency
    Frontier Research Center, Tokyo Institute of Technology)

  • Hideo Hosono

    (Materials Research Center for Element Strategy, Tokyo Institute of Technology
    Materials and Structures Laboratory, Tokyo Institute of Technology
    ACCEL, Japan Science and Technology Agency
    Frontier Research Center, Tokyo Institute of Technology)

Abstract

Novel approaches to efficient ammonia synthesis at an ambient pressure are actively sought out so as to reduce the cost of ammonia production and to allow for compact production facilities. It is accepted that the key is the development of a high-performance catalyst that significantly enhances dissociation of the nitrogen–nitrogen triple bond, which is generally considered a rate-determining step. Here we examine kinetics of nitrogen and hydrogen isotope exchange and hydrogen adsorption/desorption reactions for a recently discovered efficient catalyst for ammonia synthesis—ruthenium-loaded 12CaO·7Al2O3 electride (Ru/C12A7:e−)—and find that the rate controlling step of ammonia synthesis over Ru/C12A7:e− is not dissociation of the nitrogen–nitrogen triple bond but the subsequent formation of N–Hn species. A mechanism of ammonia synthesis involving reversible storage and release of hydrogen atoms on the Ru/C12A7:e− surface is proposed on the basis of observed hydrogen absorption/desorption kinetics.

Suggested Citation

  • Masaaki Kitano & Shinji Kanbara & Yasunori Inoue & Navaratnarajah Kuganathan & Peter V. Sushko & Toshiharu Yokoyama & Michikazu Hara & Hideo Hosono, 2015. "Electride support boosts nitrogen dissociation over ruthenium catalyst and shifts the bottleneck in ammonia synthesis," Nature Communications, Nature, vol. 6(1), pages 1-9, November.
    • Handle: RePEc:nat:natcom:v:6:y:2015:i:1:d:10.1038_ncomms7731
    DOI: 10.1038/ncomms7731
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    Cited by:

    1. Huihuang Fang & Simson Wu & Tugce Ayvali & Jianwei Zheng & Joshua Fellowes & Ping-Luen Ho & Kwan Chee Leung & Alexander Large & Georg Held & Ryuichi Kato & Kazu Suenaga & Yves Ira A. Reyes & Ho Viet T, 2023. "Dispersed surface Ru ensembles on MgO(111) for catalytic ammonia decomposition," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    2. Navaratnarajah Kuganathan & Alexander Chroneos, 2020. "Lithium Storage in Nanoporous Complex Oxide 12CaO•7Al 2 O 3 (C12A7)," Energies, MDPI, vol. 13(7), pages 1-10, March.
    3. Zichuang Li & Yangfan Lu & Jiang Li & Miao Xu & Yanpeng Qi & Sang-Won Park & Masaaki Kitano & Hideo Hosono & Jie-Sheng Chen & Tian-Nan Ye, 2023. "Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    4. Navaratnarajah Kuganathan & Ruslan V. Vovk & Alexander Chroneos, 2020. "Mayenite Electrides and Their Doped Forms for Oxygen Reduction Reaction in Solid Oxide Fuel Cells," Energies, MDPI, vol. 13(18), pages 1-14, September.

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