Understanding complete oxidation of methane on spinel oxides at a molecular level

Franklin Feng Tao (), Jun-jun Shan, Luan Nguyen, Ziyun Wang, Shiran Zhang, Li Zhang, Zili Wu, Weixin Huang, Shibi Zeng and P. Hu ()
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Franklin Feng Tao: University of Kansas
Jun-jun Shan: University of Kansas
Luan Nguyen: University of Kansas
Ziyun Wang: School of Chemistry and Chemical Engineering, Queens University
Shiran Zhang: University of Kansas
Li Zhang: Oak Ridge National Laboratory Oak Ridge
Zili Wu: Oak Ridge National Laboratory Oak Ridge
Weixin Huang: University of Kansas
Shibi Zeng: University of Kansas
P. Hu: School of Chemistry and Chemical Engineering, Queens University

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

Abstract: Abstract It is crucial to develop a catalyst made of earth-abundant elements highly active for a complete oxidation of methane at a relatively low temperature. NiCo2O4 consisting of earth-abundant elements which can completely oxidize methane in the temperature range of 350–550 °C. Being a cost-effective catalyst, NiCo2O4 exhibits activity higher than precious-metal-based catalysts. Here we report that the higher catalytic activity at the relatively low temperature results from the integration of nickel cations, cobalt cations and surface lattice oxygen atoms/oxygen vacancies at the atomic scale. In situ studies of complete oxidation of methane on NiCo2O4 and theoretical simulations show that methane dissociates to methyl on nickel cations and then couple with surface lattice oxygen atoms to form –CH3O with a following dehydrogenation to −CH2O; a following oxidative dehydrogenation forms CHO; CHO is transformed to product molecules through two different sub-pathways including dehydrogenation of OCHO and CO oxidation.

Date: 2015
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DOI: 10.1038/ncomms8798

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