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Construction of N−E bonds via Lewis acid-promoted functionalization of chromium-dinitrogen complexes

Author

Listed:
  • Zhu-Bao Yin

    (Peking University)

  • Gao-Xiang Wang

    (Peking University)

  • Xuechao Yan

    (Peking University)

  • Junnian Wei

    (Peking University)

  • Zhenfeng Xi

    (Peking University)

Abstract

Direct conversion of dinitrogen (N2) into N-containing compounds beyond ammonia under ambient conditions remains a longstanding challenge. Herein, we present a Lewis acid-promoted strategy for diverse nitrogen-element bonds formation from N2 using chromium dinitrogen complex [Cp*(IiPr2Me2)Cr(N2)2]K (1). With the help of Lewis acids AlMe3 and BF3, we successfully trap a series of fleeting diazenido intermediates and synthesize value-added compounds containing N−B, N−Ge, and N−P bonds with 3 d metals, offering a method for isolating unstable intermediates. Furthermore, the formation of N−C bonds is realized under more accessible conditions that avoid undesired side reactions. DFT calculations reveal that Lewis acids enhance the participation of dinitrogen units in the frontier orbitals, thereby promoting electrophilic functionalization. Moreover, Lewis acid replacement and a base-induced end-on to side-on switch of [NNMe] unit in [(Cp*(IiPr2Me2)CrNN(BEt3)(Me)] (8) are achieved.

Suggested Citation

  • Zhu-Bao Yin & Gao-Xiang Wang & Xuechao Yan & Junnian Wei & Zhenfeng Xi, 2025. "Construction of N−E bonds via Lewis acid-promoted functionalization of chromium-dinitrogen complexes," Nature Communications, Nature, vol. 16(1), pages 1-8, December.
    • Handle: RePEc:nat:natcom:v:16:y:2025:i:1:d:10.1038_s41467-025-55998-5
    DOI: 10.1038/s41467-025-55998-5
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    References listed on IDEAS

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    1. Sean F. McWilliams & Daniël L. J. Broere & Connor J. V. Halliday & Samuel M. Bhutto & Brandon Q. Mercado & Patrick L. Holland, 2020. "Author Correction: Coupling dinitrogen and hydrocarbons through aryl migration," Nature, Nature, vol. 586(7828), pages 10-10, October.
    2. Yuya Ashida & Kazuya Arashiba & Kazunari Nakajima & Yoshiaki Nishibayashi, 2019. "Molybdenum-catalysed ammonia production with samarium diiodide and alcohols or water," Nature, Nature, vol. 568(7753), pages 536-540, April.
    3. Sean F. McWilliams & Daniël L. J. Broere & Connor J. V. Halliday & Samuel M. Bhutto & Brandon Q. Mercado & Patrick L. Holland, 2020. "Coupling dinitrogen and hydrocarbons through aryl migration," Nature, Nature, vol. 584(7820), pages 221-226, August.
    4. John S. Anderson & Jonathan Rittle & Jonas C. Peters, 2013. "Catalytic conversion of nitrogen to ammonia by an iron model complex," Nature, Nature, vol. 501(7465), pages 84-87, September.
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