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

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

Nature communications (2015-10-16)
Pengfei Zhang, Hanfeng Lu, Ying Zhou, Li Zhang, Zili Wu, Shize Yang, Hongliang Shi, Qiulian Zhu, Yinfei Chen, Sheng Dai
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 Mn(4+) ions for the rapid migration of oxygen vacancies from the bulk to the surface.

MATERIALS
Product Number
Brand
Product Description

Supelco
Ethanol solution, certified reference material, 2000 μg/mL in methanol
Sigma-Aldrich
Nitrogen, ≥99.998%
Sigma-Aldrich
Ethanol, purum, fine spirit, denaturated with 4.8% methanol, F25 METHYL1, ~96% (based on denaturant-free substance)
Sigma-Aldrich
Ethanol, ACS reagent, prima fine spirit, without additive, F15 o1