Reactivity and reaction intermediates for acetic acid adsorbed on CeO2(111)

Calaza, Florencia C.; Chen, Tsung -Liang; Mullins, David R.; Xu, Ye

doi:10.1016/j.cattod.2015.03.033

Reactivity and reaction intermediates for acetic acid adsorbed on CeO₂(111)

Journal Article · Sat May 02 00:00:00 EDT 2015 · Catalysis Today

DOI:https://doi.org/10.1016/j.cattod.2015.03.033· OSTI ID:1185988

Calaza, Florencia C. ^[1]; Chen, Tsung -Liang ^[1]; Mullins, David R. ^[1]; Xu, Ye ^[2]

Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
Louisiana State Univ., Baton Rouge, LA (United States)

Adsorption and reaction of acetic acid on a CeO₂(1 1 1) surface was studied by a combination of ultra-highvacuum based methods including temperature desorption spectroscopy (TPD), soft X-ray photoelectronspectroscopy (sXPS), near edge X-ray absorption spectroscopy (NEXAFS) and reflection absorption IRspectroscopy (RAIRS), together with density functional theory (DFT) calculations. TPD shows that thedesorption products are strongly dependent upon the initial oxidation state of the CeO₂ surface, includingselectivity between acetone and acetaldehyde products. The combination of sXPS and NEXAFS demon-strate that acetate forms upon adsorption at low temperature and is stable to above 500 K, above whichpoint ketene, acetone and acetic acid desorb. Furthermore, DFT and RAIRS show that below 500 K, bridge bondedacetate coexists with a moiety formed by adsorption of an acetate at an oxygen vacancy, formed bywater desorption.

View Accepted Manuscript (DOE)

Research Organization:: Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)

Sponsoring Organization:: USDOE; USDOE Office of Science (SC)

Grant/Contract Number:: AC05-00OR22725

OSTI ID:: 1185988

Alternate ID(s):: OSTI ID: 1229315
OSTI ID: 1251819

Journal Information:: Catalysis Today, Journal Name: Catalysis Today Vol. 253; ISSN 0920-5861

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Related Subjects

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY
CeO2(111)
DFT
NEXAFS
TPD
acetic acid
acetic acid adsorption
ketonization
oxide catalysis
sXPS
surface chemistry
vacancies