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

Pengfei Zhang, Hanfeng Lu (), Ying Zhou, Li Zhang, Zili Wu, Shize Yang, Hongliang Shi, Qiulian Zhu, Yinfei Chen and Sheng Dai ()
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Pengfei Zhang: Oak Ridge National Laboratory
Hanfeng Lu: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology
Ying Zhou: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology
Li Zhang: Oak Ridge National Laboratory
Zili Wu: Oak Ridge National Laboratory
Shize Yang: Oak Ridge National Laboratory
Hongliang Shi: Oak Ridge National Laboratory
Qiulian Zhu: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology
Yinfei Chen: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology
Sheng Dai: Oak Ridge National Laboratory

Nature Communications, 2015, vol. 6, issue 1, 1-10

Abstract: 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.

Date: 2015
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DOI: 10.1038/ncomms9446

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