The reactions of acetone with the surfaces of uranium dioxide single crystal and thin film

R. I. King, S. D. Senanayake, S. V. Chong, Hicham Idriss

Research output: Contribution to journalArticle

12 Citations (Scopus)

Abstract

The reaction of acetone, as an example of a carbonyl compound, is studied over UO2 (111) single crystal and thin film surfaces. Over the stoichiometric single crystal surface, acetone is molecularly and weakly adsorbed with a computed activation energy for desorption in the range of 95-65 kJ/mol with pre-exponential factors between 10(11) and 10(13) s(-1). On the contrary, acetone reacts very strongly on the O-defected single crystal and thin film surfaces. In addition to total decomposition evidence of aldolization and cyclization reactions were seen. The thin film of UO2 was studied by synchrotron light, providing high resolution photoelectron spectroscopy in the core level, and high sensitivity in the both the core and valence band regions. The U5f line was considerably enhanced at grazing angle when compared to that obtained at normal angle for the O-defected surface, showing that the surface is more reduced than the next layers. The U4f lines indicated the presence of U cations in lower oxidation states than +4 for the O-defected surface. These lines were considerably attenuated upon adsorption of acetone.. due to surface oxidation by C=O bond dissociation. The reaction pathway for acetone on the O-defected surface is presented, and compared to that of the previously studied acetaldehyde molecule.

Original languageEnglish
Pages (from-to)5690-5700
Number of pages11
JournalSurface Science
Volume601
Issue number24
Early online date6 Jul 2007
DOIs
Publication statusPublished - 15 Dec 2007

Keywords

  • acetone adsorption
  • UO2 (111) single crystal
  • UO2 thin film
  • valence band
  • X-ray photoelectron spectroscopy
  • temperature programmed desorption
  • oxygen defects
  • core level
  • temperature-programmed desorption
  • oxide catalysts
  • carbon-monoxide
  • molecular-structure
  • furan formation
  • gas-phase
  • acetaldehyde
  • chemistry
  • ethanol
  • TIO2

Cite this

The reactions of acetone with the surfaces of uranium dioxide single crystal and thin film. / King, R. I.; Senanayake, S. D.; Chong, S. V.; Idriss, Hicham.

In: Surface Science , Vol. 601, No. 24, 15.12.2007, p. 5690-5700.

Research output: Contribution to journalArticle

King, R. I. ; Senanayake, S. D. ; Chong, S. V. ; Idriss, Hicham. / The reactions of acetone with the surfaces of uranium dioxide single crystal and thin film. In: Surface Science . 2007 ; Vol. 601, No. 24. pp. 5690-5700.
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N2 - The reaction of acetone, as an example of a carbonyl compound, is studied over UO2 (111) single crystal and thin film surfaces. Over the stoichiometric single crystal surface, acetone is molecularly and weakly adsorbed with a computed activation energy for desorption in the range of 95-65 kJ/mol with pre-exponential factors between 10(11) and 10(13) s(-1). On the contrary, acetone reacts very strongly on the O-defected single crystal and thin film surfaces. In addition to total decomposition evidence of aldolization and cyclization reactions were seen. The thin film of UO2 was studied by synchrotron light, providing high resolution photoelectron spectroscopy in the core level, and high sensitivity in the both the core and valence band regions. The U5f line was considerably enhanced at grazing angle when compared to that obtained at normal angle for the O-defected surface, showing that the surface is more reduced than the next layers. The U4f lines indicated the presence of U cations in lower oxidation states than +4 for the O-defected surface. These lines were considerably attenuated upon adsorption of acetone.. due to surface oxidation by C=O bond dissociation. The reaction pathway for acetone on the O-defected surface is presented, and compared to that of the previously studied acetaldehyde molecule.

AB - The reaction of acetone, as an example of a carbonyl compound, is studied over UO2 (111) single crystal and thin film surfaces. Over the stoichiometric single crystal surface, acetone is molecularly and weakly adsorbed with a computed activation energy for desorption in the range of 95-65 kJ/mol with pre-exponential factors between 10(11) and 10(13) s(-1). On the contrary, acetone reacts very strongly on the O-defected single crystal and thin film surfaces. In addition to total decomposition evidence of aldolization and cyclization reactions were seen. The thin film of UO2 was studied by synchrotron light, providing high resolution photoelectron spectroscopy in the core level, and high sensitivity in the both the core and valence band regions. The U5f line was considerably enhanced at grazing angle when compared to that obtained at normal angle for the O-defected surface, showing that the surface is more reduced than the next layers. The U4f lines indicated the presence of U cations in lower oxidation states than +4 for the O-defected surface. These lines were considerably attenuated upon adsorption of acetone.. due to surface oxidation by C=O bond dissociation. The reaction pathway for acetone on the O-defected surface is presented, and compared to that of the previously studied acetaldehyde molecule.

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KW - UO2 thin film

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KW - X-ray photoelectron spectroscopy

KW - temperature programmed desorption

KW - oxygen defects

KW - core level

KW - temperature-programmed desorption

KW - oxide catalysts

KW - carbon-monoxide

KW - molecular-structure

KW - furan formation

KW - gas-phase

KW - acetaldehyde

KW - chemistry

KW - ethanol

KW - TIO2

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