IDEAS home Printed from https://ideas.repec.org/a/nat/natcom/v14y2023i1d10.1038_s41467-023-42688-3.html
   My bibliography  Save this article

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
    as

    Download full text from publisher

    File URL: https://www.nature.com/articles/s41467-023-42688-3
    File Function: Abstract
    Download Restriction: no
    File URL: https://libkey.io/10.1038/s41467-023-42688-3?utm_source=ideas
    LibKey link: if access is restricted and if your library uses this service, LibKey will redirect you to where you can use your library subscription to access this item
    ---><---

    References listed on IDEAS

    as
    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.
    Full references (including those not matched with items on IDEAS)

    Most related items

    These are the items that most often cite the same works as this one and are cited by the same works as this one.
    1. Yuan Zhong & Jiangwei Zhang & Tingting Li & Wenwu Xu & Qiaofeng Yao & Min Lu & Xue Bai & Zhennan Wu & Jianping Xie & Yu Zhang, 2023. "Suppression of kernel vibrations by layer-by-layer ligand engineering boosts photoluminescence efficiency of gold nanoclusters," Nature Communications, Nature, vol. 14(1), pages 1-12, December.
    2. Zhihe Liu & Hua Tan & Bo Li & Zehua Hu & De-en Jiang & Qiaofeng Yao & Lei Wang & Jianping Xie, 2023. "Ligand effect on switching the rate-determining step of water oxidation in atomically precise metal nanoclusters," Nature Communications, Nature, vol. 14(1), pages 1-9, December.
    3. Claudia Pigliacelli & Angela Acocella & Isabel Díez & Luca Moretti & Valentina Dichiarante & Nicola Demitri & Hua Jiang & Margherita Maiuri & Robin H. A. Ras & Francesca Baldelli Bombelli & Giulio Cer, 2022. "High-resolution crystal structure of a 20 kDa superfluorinated gold nanocluster," Nature Communications, Nature, vol. 13(1), pages 1-8, December.

    More about this item

    Statistics

    Access and download statistics

    Corrections

    All material on this site has been provided by the respective publishers and authors. You can help correct errors and omissions. When requesting a correction, please mention this item's handle: RePEc:nat:natcom:v:14:y:2023:i:1:d:10.1038_s41467-023-42688-3. See general information about how to correct material in RePEc.

    If you have authored this item and are not yet registered with RePEc, we encourage you to do it here. This allows to link your profile to this item. It also allows you to accept potential citations to this item that we are uncertain about.

    If CitEc recognized a bibliographic reference but did not link an item in RePEc to it, you can help with this form .

    If you know of missing items citing this one, you can help us creating those links by adding the relevant references in the same way as above, for each refering item. If you are a registered author of this item, you may also want to check the "citations" tab in your RePEc Author Service profile, as there may be some citations waiting for confirmation.

    For technical questions regarding this item, or to correct its authors, title, abstract, bibliographic or download information, contact: Sonal Shukla or Springer Nature Abstracting and Indexing (email available below). General contact details of provider: http://www.nature.com .

    Please note that corrections may take a couple of weeks to filter through the various RePEc services.

    IDEAS is a RePEc service. RePEc uses bibliographic data supplied by the respective publishers.