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

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.
Authors:
 [1] ;  [2] ;  [2] ;  [3] ;  [2] ;  [4] ;  [4] ;  [2] ;  [2] ;  [3]
  1. Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering; Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemistry
  2. Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemical and Petroleum Engineering; Univ. of Kansas, Lawrence, KS (United States). Dept. of Chemistry
  3. Queens Univ., Blefast (United Kingdom). School of Chemistry and Chemical Engineering
  4. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Science (CNMS)
Publication Date:
OSTI Identifier:
1319196
Grant/Contract Number:
AC05-00OR22725; FG02-12ER16353
Type:
Accepted Manuscript
Journal Name:
Nature Communications
Additional Journal Information:
Journal Volume: 6; Journal ID: ISSN 2041-1723
Publisher:
Nature Publishing Group
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States). Center for Nanophase Materials Sciences (CNMS)
Sponsoring Org:
USDOE Office of Science (SC), Basic Energy Sciences (BES) (SC-22)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; 36 MATERIALS SCIENCE