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Nitrogen reduction by the Fe sites of synthetic [Mo3S4Fe] cubes

Author

Listed:
  • Yasuhiro Ohki

    (Kyoto University)

  • Kenichiro Munakata

    (Nagoya University)

  • Yuto Matsuoka

    (Kyoto University)

  • Ryota Hara

    (Nagoya University)

  • Mami Kachi

    (Nagoya University)

  • Keisuke Uchida

    (Nagoya University)

  • Mizuki Tada

    (Nagoya University)

  • Roger E. Cramer

    (University of Hawaii)

  • W. M. C. Sameera

    (Hokkaido University
    University of Colombo)

  • Tsutomu Takayama

    (Daido University)

  • Yoichi Sakai

    (Daido University)

  • Shogo Kuriyama

    (The University of Tokyo)

  • Yoshiaki Nishibayashi

    (The University of Tokyo)

  • Kazuki Tanifuji

    (Kyoto University)

Abstract

Nitrogen (N2) fixation by nature, which is a crucial process for the supply of bio-available forms of nitrogen, is performed by nitrogenase. This enzyme uses a unique transition-metal–sulfur–carbon cluster as its active-site co-factor ([(R-homocitrate)MoFe7S9C], FeMoco)1,2, and the sulfur-surrounded iron (Fe) atoms have been postulated to capture and reduce N2 (refs. 3–6). Although there are a few examples of synthetic counterparts of the FeMoco, metal–sulfur cluster, which have shown binding of N2 (refs. 7–9), the reduction of N2 by any synthetic metal–sulfur cluster or by the extracted form of FeMoco10 has remained elusive, despite nearly 50 years of research. Here we show that the Fe atoms in our synthetic [Mo3S4Fe] cubes11,12 can capture a N2 molecule and catalyse N2 silylation to form N(SiMe3)3 under treatment with excess sodium and trimethylsilyl chloride. These results exemplify the catalytic silylation of N2 by a synthetic metal–sulfur cluster and demonstrate the N2-reduction capability of Fe atoms in a sulfur-rich environment, which is reminiscent of the ability of FeMoco to bind and activate N2.

Suggested Citation

  • Yasuhiro Ohki & Kenichiro Munakata & Yuto Matsuoka & Ryota Hara & Mami Kachi & Keisuke Uchida & Mizuki Tada & Roger E. Cramer & W. M. C. Sameera & Tsutomu Takayama & Yoichi Sakai & Shogo Kuriyama & Yo, 2022. "Nitrogen reduction by the Fe sites of synthetic [Mo3S4Fe] cubes," Nature, Nature, vol. 607(7917), pages 86-90, July.
    • Handle: RePEc:nat:nature:v:607:y:2022:i:7917:d:10.1038_s41586-022-04848-1
    DOI: 10.1038/s41586-022-04848-1
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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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