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Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds

Author

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  • Chao Xie

    (South-Central University for Nationalities)

  • Longfei Lin

    (Chinese Academy of Sciences)

  • Liang Huang

    (Wuhan University of Science and Technology)

  • Zixin Wang

    (South-Central University for Nationalities)

  • Zhiwei Jiang

    (South-Central University for Nationalities)

  • Zehui Zhang

    (South-Central University for Nationalities)

  • Buxing Han

    (Chinese Academy of Sciences)

Abstract

Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Herein, we report that Zn/NC-X catalysts, in which Zn2+ coordinate with N species on microporous N-doped carbon (NC) and X denotes the pyrolysis temperature, can effectively catalyze aerobic oxidative cleavage of C(CO)-C bonds and quantitatively convert acetophenone to methyl benzoate with a yield of 99% at 100 °C. The Zn/NC-950 can be applied for a wide scope of acetophenone derivatives as well as more challenging alkyl ketones. Detail mechanistic investigations reveal that the catalytic performance of Zn/NC-950 can be attributed to the coordination between Zn2+ and N species to change the electronic state of the metal, synergetic effect of the Zn single sites with their surrounding N atoms, as well as the microporous structure with the high surface area and structural defects of the NC.

Suggested Citation

  • Chao Xie & Longfei Lin & Liang Huang & Zixin Wang & Zhiwei Jiang & Zehui Zhang & Buxing Han, 2021. "Zn-Nx sites on N-doped carbon for aerobic oxidative cleavage and esterification of C(CO)-C bonds," Nature Communications, Nature, vol. 12(1), pages 1-12, December.
    • Handle: RePEc:nat:natcom:v:12:y:2021:i:1:d:10.1038_s41467-021-25118-0
    DOI: 10.1038/s41467-021-25118-0
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    Cited by:

    1. Tianjiao Wang & Yu Xin & Bingfeng Chen & Bin Zhang & Sen Luan & Minghua Dong & Yuxuan Wu & Xiaomeng Cheng & Ye Liu & Huizhen Liu & Buxing Han, 2024. "Selective hydrodeoxygenation of α, β-unsaturated carbonyl compounds to alkenes," Nature Communications, Nature, vol. 15(1), pages 1-10, December.
    2. Xin Yuan & Xiaoling Wu & Jun Xiong & Binhang Yan & Ruichen Gao & Shuli Liu & Minhua Zong & Jun Ge & Wenyong Lou, 2023. "Hydrolase mimic via second coordination sphere engineering in metal-organic frameworks for environmental remediation," Nature Communications, Nature, vol. 14(1), pages 1-13, December.

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