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Enable biomass-derived alcohols mediated alkylation and transfer hydrogenation

Author

Listed:
  • Xixi Liu

    (South-Central Minzu University
    Sichuan University)

  • Liang Huang

    (Wuhan University of Science and Technology)

  • Yuandie Ma

    (South-Central Minzu University)

  • Guoqiang She

    (South-Central Minzu University)

  • Peng Zhou

    (South-Central Minzu University)

  • Liangfang Zhu

    (Sichuan University)

  • Zehui Zhang

    (South-Central Minzu University)

Abstract

A single-atom catalyst with generally regarded inert Zn–N4 motifs derived from ZIF-8 is unexpectedly efficient for the activation of alcohols, enabling alcohol-mediated alkylation and transfer hydrogenation. C-alkylation of nitriles, ketones, alcohols, N-heterocycles, amides, keto acids, and esters, and N-alkylation of amines and amides all go smoothly with the developed method. Taking the α-alkylation of nitriles with alcohols as an example, the α-alkylation starts from the (1) nitrogen-doped carbon support catalyzed dehydrogenation of alcohols into aldehydes, which further condensed with nitriles to give vinyl nitriles, followed by (2) transfer hydrogenation of C=C bonds in vinyl nitriles on Zn–N4 sites. The experimental results and DFT calculations reveal that the Lewis acidic Zn-N4 sites promote step (2) by activating the alcohols. This is the first example of highly efficient single-atom catalysts for various organic transformations with biomass-derived alcohols as the alkylating reagents and hydrogen donors.

Suggested Citation

  • Xixi Liu & Liang Huang & Yuandie Ma & Guoqiang She & Peng Zhou & Liangfang Zhu & Zehui Zhang, 2024. "Enable biomass-derived alcohols mediated alkylation and transfer hydrogenation," Nature Communications, Nature, vol. 15(1), pages 1-15, December.
  • Handle: RePEc:nat:natcom:v:15:y:2024:i:1:d:10.1038_s41467-024-51307-8
    DOI: 10.1038/s41467-024-51307-8
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    References listed on IDEAS

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