期刊
NATURE COMMUNICATIONS
卷 6, 期 -, 页码 -出版社
NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms9446
关键词
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资金
- U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
- Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
- Natural Science Foundation of China [21107096, 21506194]
- Natural Science Foundation of Zhejiang province [LY14E080008]
- commission of Science and Technology of Zhejiang province [2013C03021]
The development of noble-metal-free heterogeneous catalysts that can realize the aerobic oxidation of C-H bonds at low temperature is a profound challenge in the catalysis community. Here we report the synthesis of a mesoporous Mn0.5Ce0.5Ox solid solution that is highly active for the selective oxidation of hydrocarbons under mild conditions (100-120 degrees C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/ cyclohexanol (100 degrees C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140-160 degrees C, conversion: 3-5%). The high activity can be attributed to the formation of a Mn0.5Ce0.5Ox solid solution with an ultrahigh manganese doping concentration in the CeO2 cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C-H bonds and highly reducible Mn4+ ions for the rapid migration of oxygen vacancies from the bulk to the surface.
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