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

被引:143
作者
Xie, Chao [1 ,2 ]
Lin, Longfei [3 ]
Huang, Liang [4 ]
Wang, Zixin [1 ,2 ]
Jiang, Zhiwei [1 ,2 ]
Zhang, Zehui [1 ,2 ]
Han, Buxing [3 ]
机构
[1] South Cent Univ Nationalities, Minist Educ, Key Lab Catalysis & Energy Mat Chem, Wuhan, Peoples R China
[2] South Cent Univ Nationalities, Hubei Key Lab Catalysis & Mat Sci, Wuhan, Peoples R China
[3] Chinese Acad Sci, Inst Chem, CAS Key Lab Colloid Interface & Chem Thermodynam, Beijing Natl Lab Mol Sci, Beijing, Peoples R China
[4] Wuhan Univ Sci & Technol, State Key Lab Refractories & Met, Wuhan, Peoples R China
基金
中国国家自然科学基金;
关键词
KETONES; CONVERSION; CATALYSTS; ESTERS; AIR; OXYGENATION; PERFORMANCE; ACTIVATION; EFFICIENT; ALDEHYDES;
D O I
10.1038/s41467-021-25118-0
中图分类号
O [数理科学和化学]; P [天文学、地球科学]; Q [生物科学]; N [自然科学总论];
学科分类号
07 ; 0710 ; 09 ;
摘要
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 degrees 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. Selective cleavage of C-C bonds is very important in organic chemistry, but remains challenging because of their inert chemical nature. Here, the authors report that Zn2+ coordinated with N species on N-doped carbon catalysts can catalyze the aerobic oxidative cleavage and esterification of C(CO)-C bonds with high efficiency and activity.
引用
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页数:12
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