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

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.
Authors:
 [1] ;  [1] ;  [1] ;  [2] ;
  1. Oak Ridge National Lab. (ORNL), Oak Ridge, TN (United States)
  2. Louisiana State Univ., Baton Rouge, LA (United States)
Publication Date:
OSTI Identifier:
1185988
Grant/Contract Number:
AC05-00OR22725
Type:
Accepted Manuscript
Journal Name:
Catalysis Today
Additional Journal Information:
Journal Volume: 253; Journal ID: ISSN 0920-5861
Publisher:
Elsevier
Research Org:
Oak Ridge National Laboratory (ORNL), Oak Ridge, TN (United States)
Sponsoring Org:
USDOE Office of Science (SC)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY CeO2(111); acetic acid; ketonization; vacancies; TPD; sXPS; NEXAFS; DFT; oxide catalysis; surface chemistry; acetic acid adsorption