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Mesoporous MnCeO(x) solid solutions for low temperature and selective oxidation of hydrocarbons
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 Mn(0.5)Ce(0.5)O(x) solid solution that is highly active for the selectiv...
Autores principales: | , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Pub. Group
2015
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC4633985/ https://www.ncbi.nlm.nih.gov/pubmed/26469151 http://dx.doi.org/10.1038/ncomms9446 |
Sumario: | 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 Mn(0.5)Ce(0.5)O(x) 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 Mn(0.5)Ce(0.5)O(x) solid solution with an ultrahigh manganese doping concentration in the CeO(2) cubic fluorite lattice, leading to maximum active surface oxygens for the activation of C–H bonds and highly reducible Mn(4+) ions for the rapid migration of oxygen vacancies from the bulk to the surface. |
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