title: Mesoporous MnCeOx solid solutions for low temperature and selective oxidation of hydrocarbons.
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.
authors.affiliation: Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
authors.forename: Pengfei
authors.initials: P
authors.lastname: Zhang
authors.affiliation: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
authors.forename: Hanfeng
authors.initials: H
authors.lastname: Lu
authors.affiliation: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
authors.forename: Ying
authors.initials: Y
authors.lastname: Zhou
authors.affiliation: Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
authors.forename: Li
authors.initials: L
authors.lastname: Zhang
authors.affiliation: Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
authors.forename: Zili
authors.initials: Z
authors.lastname: Wu
authors.affiliation: Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
authors.forename: Shize
authors.initials: S
authors.lastname: Yang
authors.affiliation: Materials Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.
authors.forename: Hongliang
authors.initials: H
authors.lastname: Shi
authors.affiliation: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
authors.forename: Qiulian
authors.initials: Q
authors.lastname: Zhu
authors.affiliation: Institute of Catalytic Reaction Engineering, College of Chemical Engineering, Zhejiang University of Technology, Hangzhou 310014, China.
authors.forename: Yinfei
authors.initials: Y
authors.lastname: Chen
authors.affiliation: Chemical Sciences Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, USA.|Department of Chemistry, University of Tennessee, Knoxville, Tennessee 37996, USA.
authors.forename: Sheng
authors.initials: S
authors.lastname: Dai