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This content will become publicly available on December 23, 2016

Title: Hydrogen and methoxy coadsorption in the computation of the catalytic conversion of methanol on the ceria (111) surface

Methanol decomposition to formaldehyde catalyzed by the ceria (111) surface has been investigated using the DFT + U method. Our results rationalize experimental temperature programmed desorption experiments on the fully oxidized surface. Particular attention has been paid to the model correctness of methoxy with coadsorbed hydrogen on the surface. This issue has been raised by the experimental observation of water desorption at low temperature removing hydrogen from the system. Our investigation also includes hydrogen diffusion as a means of hydrogen removal. We find that the presence of methoxy reduces the reaction energy for water formation considerably. In addition, the preference of the electron to locate at the methoxy oxygen results in a dehydrated surface that does not contain Ce3+ ions, despite the existence of a vacancy.
 [1] ;
  1. Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Publication Date:
OSTI Identifier:
Grant/Contract Number:
Accepted Manuscript
Journal Name:
Surface Science
Additional Journal Information:
Journal Volume: 648; Journal Issue: C; Journal ID: ISSN 0039-6028
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
Country of Publication:
United States
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY formaldehyde; DFT + U; NEB; dehydrogenation; hydrogen diffusion; water formation