Visible-light-induced aerobic oxidation of alcohols to aldehydes/ketones via solvated dispersion intermediates

被引:0
|
作者
Lei, Wenlong [1 ,2 ]
Liu, Runze [3 ]
Li, Rengui [1 ,2 ]
Liu, Yan [1 ,2 ]
Li, Can [1 ,2 ]
机构
[1] Chinese Acad Sci, Dalian Inst Chem Phys, State Key Lab Catalysis, Dalian Natl Lab Clean Energy, Dalian, Peoples R China
[2] Univ Chinese Acad Sci, Beijing, Peoples R China
[3] Shandong Univ, Inst Mol Sci & Engn, Inst Frontier & Interdisciplinary Sci, Qingdao, Peoples R China
基金
中国国家自然科学基金;
关键词
SELECTIVE PHOTOCATALYTIC OXIDATION; BENZYLIC ALCOHOLS; HIGHLY EFFICIENT; METAL-FREE; OXYGEN; CATALYSIS; TIO2; COMPLEXES; GREEN;
D O I
10.1039/d4gc01210k
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
Selective oxidation of alcohols to aldehydes/ketones is an important reaction in the fine and bulk chemicals fields. However, the classical alcohol oxidation methods are often performed under unfriendly conditions or use stoichiometric oxidants. Herein, we report an ingenious system that enables high selectivity (up to 99%) and high conversion (up to 97%) with high reaction rates in the aerobic oxidation of alcohols to aldehydes/ketones for a broad range of alcohols, proceeding smoothly via mixing the solvent ethyl acetate and HBr under ambient conditions with visible light irradiation. Experimental characterization and theoretical calculations reveal that solvated dispersion intermediates are formed spontaneously in situ through noncovalent interactions among the molecules in the reaction system, which is proposed to be the origin of the high selectivity and high activity of this reaction. The dispersion system provides a feasible activation approach for aerobic oxidation of alcohols to aldehydes/ketones with high performance under visible light.
引用
收藏
页码:7902 / 7910
页数:9
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