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

Zhang, Pengfei; Lu, Hanfeng; Zhou, Ying; Zhang, Li; Wu, Zili; Yang, Shize; Shi, Hongliang; Zhu, Qiulian; Chen, Yinfei; Dai, Sheng

doi:10.1038/ncomms9446

Title: Mesoporous MnCeO_x solid solutions for low temperature and selective oxidation of hydrocarbons

Journal Article · Thu Oct 15 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms9446· OSTI ID:1259683

Zhang, Pengfei ^[1]; Lu, Hanfeng ^[2]; Zhou, Ying ^[2]; Zhang, Li ^[1]; Wu, Zili ^[1]; Yang, Shize ^[1]; Shi, Hongliang ^[1]; Zhu, Qiulian ^[2]; Chen, Yinfei ^[2]; Dai, Sheng ^[3]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Zhejiang Univ. of Technology, Hangzhou (China)
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States); Univ. of Tennessee, Knoxville, TN (United States)

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_0.5Ce_0.5O_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%). Finally, the high activity can be attributed to the formation of a Mn_0.5Ce_0.5O_x 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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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: 21107096; 21506194; LY14E080008; 2013C03021

OSTI ID:: 1259683

Journal Information:: Nature Communications, Vol. 6; ISSN 2041-1723

Publisher:: Nature Publishing GroupCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 234 works

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