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

Tao, Franklin Feng; Shan, Jun-jun; Nguyen, Luan; Wang, Ziyun; Zhang, Shiran; Zhang, Li; Wu, Zili; Huang, Weixin; Zeng, Shibi; Hu, P.

doi:10.1038/ncomms8798

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

Journal Article · Tue Aug 04 00:00:00 EDT 2015 · Nature Communications

DOI:https://doi.org/10.1038/ncomms8798· OSTI ID:1319196

Tao, Franklin Feng ^[1]; Shan, Jun-jun ^[2]; Nguyen, Luan ^[2]; Wang, Ziyun ^[3]; Zhang, Shiran ^[2]; Zhang, Li ^[4]; Wu, Zili ^[4]; Huang, Weixin ^[2]; Zeng, Shibi ^[2]; Hu, P. ^[3]

Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering; Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemistry
Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering; Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemistry
Queens Univ., Blefast (United Kingdom). School of Chemistry and Chemical Engineering
Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)

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. Finally, 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.

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Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)

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

Grant/Contract Number:: AC05-00OR22725; FG02-12ER16353

OSTI ID:: 1319196

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: 213 works

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