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Remarkable catalytic activity of dinitrogen-bridged dimolybdenum complexes bearing NHC-based PCP-pincer ligands toward nitrogen fixation

Author

Listed:
  • Aya Eizawa

    (School of Engineering, The University of Tokyo)

  • Kazuya Arashiba

    (School of Engineering, The University of Tokyo)

  • Hiromasa Tanaka

    (Institute for Materials Chemistry and Engineering, Kyushu University)

  • Shogo Kuriyama

    (School of Engineering, The University of Tokyo)

  • Yuki Matsuo

    (Institute for Materials Chemistry and Engineering, Kyushu University)

  • Kazunari Nakajima

    (School of Engineering, The University of Tokyo)

  • Kazunari Yoshizawa

    (Institute for Materials Chemistry and Engineering, Kyushu University
    Elements Strategy Initiative for Catalysts and Batteries, Kyoto University)

  • Yoshiaki Nishibayashi

    (School of Engineering, The University of Tokyo)

Abstract

Intensive efforts for the transformation of dinitrogen using transition metal–dinitrogen complexes as catalysts under mild reaction conditions have been made. However, limited systems have succeeded in the catalytic formation of ammonia. Here we show that newly designed and prepared dinitrogen-bridged dimolybdenum complexes bearing N-heterocyclic carbene- and phosphine-based PCP-pincer ligands [{Mo(N2)2(PCP)}2(μ-N2)] (1) work as so far the most effective catalysts towards the formation of ammonia from dinitrogen under ambient reaction conditions, where up to 230 equiv. of ammonia are produced based on the catalyst. DFT calculations on 1 reveal that the PCP-pincer ligand serves as not only a strong σ-donor but also a π-acceptor. These electronic properties are responsible for a solid connection between the molybdenum centre and the pincer ligand, leading to the enhanced catalytic activity for nitrogen fixation.

Suggested Citation

  • Aya Eizawa & Kazuya Arashiba & Hiromasa Tanaka & Shogo Kuriyama & Yuki Matsuo & Kazunari Nakajima & Kazunari Yoshizawa & Yoshiaki Nishibayashi, 2017. "Remarkable catalytic activity of dinitrogen-bridged dimolybdenum complexes bearing NHC-based PCP-pincer ligands toward nitrogen fixation," Nature Communications, Nature, vol. 8(1), pages 1-12, April.
    • Handle: RePEc:nat:natcom:v:8:y:2017:i:1:d:10.1038_ncomms14874
    DOI: 10.1038/ncomms14874
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    Cited by:

    1. Yuya Ashida & Yuto Onozuka & Kazuya Arashiba & Asuka Konomi & Hiromasa Tanaka & Shogo Kuriyama & Yasuomi Yamazaki & Kazunari Yoshizawa & Yoshiaki Nishibayashi, 2022. "Catalytic nitrogen fixation using visible light energy," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

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