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Atomically precise ultrasmall copper cluster for room-temperature highly regioselective dehydrogenative coupling

Author

Listed:
  • Teng Jia

    (Zhengzhou University)

  • Yi-Xin Li

    (Zhengzhou University)

  • Xiao-Hong Ma

    (Zhengzhou University)

  • Miao-Miao Zhang

    (Zhengzhou University)

  • Xi-Yan Dong

    (Zhengzhou University
    Henan Polytechnic University)

  • Jie Ai

    (Zhengzhou University)

  • Shuang-Quan Zang

    (Zhengzhou University)

Abstract

Three-component dehydrogenative coupling reactions represent important and practical methodologies for forging new C–N bonds and C–C bonds. Achieving highly all-in-one dehydrogenative coupling functionalization by a single catalytic system remains a great challenge. Herein, we develop a rigid-flexible-coupled copper cluster [Cu3(NHC)3(PF6)3] (Cu3NC(NHC)) using a tridentate N-heterocyclic carbene ligand. The shell ligand endows Cu3NC(NHC) with dual attributes, including rigidity and flexibility, to improve activity and stability. The Cu3NC(NHC) is applied to catalyze both highly all-in-one dehydrogenative coupling transformations. Mechanistic studies and density functional theory illustrate that the improved regioselectivity is derived from the low energy of ion pair with copper acetylide and endo-iminium ions and the low transition state, which originates from the unique physicochemical properties of the Cu3NC(NHC) catalyst. This work highlights the importance of N-heterocyclic carbene in the modification of copper clusters, providing a new design rule to protect cluster catalytic centers and enhance catalysis.

Suggested Citation

  • Teng Jia & Yi-Xin Li & Xiao-Hong Ma & Miao-Miao Zhang & Xi-Yan Dong & Jie Ai & Shuang-Quan Zang, 2023. "Atomically precise ultrasmall copper cluster for room-temperature highly regioselective dehydrogenative coupling," Nature Communications, Nature, vol. 14(1), pages 1-15, December.
    • Handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42688-3
    DOI: 10.1038/s41467-023-42688-3
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    References listed on IDEAS

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    1. Yitao Cao & Victor Fung & Qiaofeng Yao & Tiankai Chen & Shuangquan Zang & De-en Jiang & Jianping Xie, 2020. "Control of single-ligand chemistry on thiolated Au25 nanoclusters," Nature Communications, Nature, vol. 11(1), pages 1-7, December.
    2. Qi Liu & Haibo Xu & Yuling Li & Yuan Yao & Xue Zhang & Yinlong Guo & Shengming Ma, 2021. "Pyrinap ligands for enantioselective syntheses of amines," Nature Communications, Nature, vol. 12(1), pages 1-10, December.
    3. Wu Fan & Weiming Yuan & Shengming Ma, 2014. "Unexpected E-stereoselective reductive A3-coupling reaction of terminal alkynes with aldehydes and amines," Nature Communications, Nature, vol. 5(1), pages 1-9, September.
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