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

作者：Chao Xie, Longfei Lin, Liang Huang, Zixin Wang, Zhiwei Jiang, Zehui Zhang, Buxing Han · 发表于：Nature Communications · 年份：2021 · DOI：10.1038/s41467-021-25118-0 · 被引用次数：200 · 研究领域：Catalytic Processes in Materials Science、Covalent Organic Framework Applications、Advanced Photocatalysis Techniques

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 Zn 2+ 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 Zn 2+ 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.