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

Beste, Ariana

doi:10.1016/j.susc.2015.12.002

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

Journal Article · Wed Dec 23 00:00:00 EST 2015 · Surface Science

DOI:https://doi.org/10.1016/j.susc.2015.12.002· OSTI ID:1238739

Beste, Ariana ^[1]

Univ. of Tennessee, Knoxville, TN (United States); Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)

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.

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Research Organization:: Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States). Oak Ridge Leadership Computing Facility (OLCF)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1238739

Alternate ID(s):: OSTI ID: 1251758

Journal Information:: Surface Science, Vol. 648, Issue C; ISSN 0039-6028

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 8 works

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

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