4.8 Article

Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons

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NATURE COMMUNICATIONS
卷 6, 期 -, 页码 -

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NATURE PUBLISHING GROUP
DOI: 10.1038/ncomms9446

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  1. U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division
  2. Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division
  3. Natural Science Foundation of China [21107096, 21506194]
  4. Natural Science Foundation of Zhejiang province [LY14E080008]
  5. commission of Science and Technology of Zhejiang province [2013C03021]

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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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