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

Chao Xie, Longfei Lin, Liang Huang, Zixin Wang, Zhiwei Jiang, Zehui Zhang () and Buxing Han ()
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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

Nature Communications, 2021, vol. 12, issue 1, 1-12

Abstract: 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.

Date: 2021
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DOI: 10.1038/s41467-021-25118-0

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