Theoretical Study of Trimethylacetic Acid Adsorption on CeO 2 (111) Surface

Wang, Weina; Thevuthasan, S.; Wang, Wenliang; Yang, Ping

doi:10.1021/acs.jpcc.5b09790

Title: Theoretical Study of Trimethylacetic Acid Adsorption on CeO ₂ (111) Surface

Journal Article · Mon Jan 11 00:00:00 EST 2016 · Journal of Physical Chemistry. C

DOI:https://doi.org/10.1021/acs.jpcc.5b09790· OSTI ID:1240621

Wang, Weina ^[1]; Thevuthasan, S. ^[2]; Wang, Wenliang ^[3]; Yang, Ping ^[4]

Shaanxi Normal Univ. (China); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Pacific Northwest National Lab. (PNNL), Richland, WA (United States)
Shaanxi Normal Univ. (China)
Los Alamos National Lab. (LANL), Los Alamos, NM (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

We investigated trimethylacetic acid (TMAA) adsorption on stoichiometric and oxygen-deficient CeO₂(111) surfaces using density functional theory that accounts for the on-site Coulomb interaction via a Hubbard term (DFT+U) and long-range dispersion correction. Both the molecular state and dissociative state (TMAA → TMA– + H⁺) were identified on stoichiometric and oxygen-deficient CeO₂(111) surfaces. For the stoichiometric surface, two thermodynamically favorable configurations with adsorption energies of the order of -30 kcal/mol are identified; one is a molecule adsorption state, and the other one is a dissociative state. For the oxygen-deficient surface, dissociative states are more favorable than molecular states. Moreover, the most favorable configuration is the dissociative adsorption of TMAA with the adsorption energy of the order of -77 kcal/mol. The dissociated TMA moiety takes the position of oxygen vacancy, forming three Ce–O bonds. The signature vibrational frequencies for these thermodynamically stable structures are reported as well as their electronic structures. The effects of long-range dispersion interactions are found to be negligible for geometries but important for adsorption energies.

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Research Organization:: Los Alamos National Lab. (LANL), Los Alamos, NM (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES); USDOE National Nuclear Security Administration (NNSA)

Grant/Contract Number:: 201303004; GK:201101004; AC52-06NA25396; 21173139; 2013KCT-17

OSTI ID:: 1240621

Report Number(s):: LA-UR-15-27576

Journal Information:: Journal of Physical Chemistry. C, Vol. 120, Issue 5; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 13 works

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