Abstract
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 °C). Notably, the catalytic performance achieved in the oxidation of cyclohexane to cyclohexanone/cyclohexanol (100 °C, conversion: 17.7%) is superior to those by the state-of-art commercial catalysts (140-160 °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.
Original language | English |
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Article number | 8446 |
Journal | Nature Communications |
Volume | 6 |
DOIs | |
State | Published - Oct 15 2015 |
Funding
P.F.Z., L.Z., Z.L.W. and S.D. were supported by the U.S. Department of Energy, Office of Science, Basic Energy Sciences, Chemical Sciences, Geosciences, and Biosciences Division. The DRIFTS study was conducted at the Center for Nanophase Materials Sciences, which is a DOE Office of Science User Facility. H.L.S. was supported by the Department of Energy, Office of Science, Basic Energy Sciences, Materials Sciences and Engineering Division. H.F.L, Y.Z., Q.L.Z. and Y.F.C. were supported by the Natural Science Foundation of China (NO. 21107096, 21506194), the Natural Science Foundation of Zhejiang province (No. LY14E080008) and the commission of Science and Technology of Zhejiang province (No. 2013C03021).
Funders | Funder number |
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U.S. Department of Energy | |
Office of Science | |
Basic Energy Sciences | |
Division of Materials Sciences and Engineering | |
Chemical Sciences, Geosciences, and Biosciences Division | |
National Natural Science Foundation of China | 21107096, 21506194 |
Natural Science Foundation of Zhejiang Province |