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Multiple reaction pathway on alkaline earth imide supported catalysts for efficient ammonia synthesis

Author

Listed:
  • Zichuang Li

    (Shanghai Jiao Tong University)

  • Yangfan Lu

    (Chongqing University)

  • Jiang Li

    (Tokyo Institute of Technology)

  • Miao Xu

    (Shanghai Institute of Space Power-Sources)

  • Yanpeng Qi

    (School of Physical Science and Technology Shanghai Tech University
    ShanghaiTech University
    ShanghaiTech University)

  • Sang-Won Park

    (Tokyo Institute of Technology)

  • Masaaki Kitano

    (Tokyo Institute of Technology)

  • Hideo Hosono

    (Tokyo Institute of Technology)

  • Jie-Sheng Chen

    (Shanghai Jiao Tong University)

  • Tian-Nan Ye

    (Shanghai Jiao Tong University)

Abstract

The tunability of reaction pathways is required for exploring efficient and low cost catalysts for ammonia synthesis. There is an obstacle by the limitations arising from scaling relation for this purpose. Here, we demonstrate that the alkali earth imides (AeNH) combined with transition metal (TM = Fe, Co and Ni) catalysts can overcome this difficulty by utilizing functionalities arising from concerted role of active defects on the support surface and loaded transition metals. These catalysts enable ammonia production through multiple reaction pathways. The reaction rate of Co/SrNH is as high as 1686.7 mmol·gCo−1·h−1 and the TOFs reaches above 500 h−1 at 400 °C and 0.9 MPa, outperforming other reported Co-based catalysts as well as the benchmark Cs-Ru/MgO catalyst and industrial wüstite-based Fe catalyst under the same reaction conditions. Experimental and theoretical results show that the synergistic effect of nitrogen affinity of 3d TMs and in-situ formed NH2− vacancy of alkali earth imides regulate the reaction pathways of the ammonia production, resulting in distinct catalytic performance different from 3d TMs. It was thus demonstrated that the appropriate combination of metal and support is essential for controlling the reaction pathway and realizing highly active and low cost catalysts for ammonia synthesis.

Suggested Citation

  • 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.
  • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42050-7
    DOI: 10.1038/s41467-023-42050-7
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    References listed on IDEAS

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