Reactions of acetaldehyde on UO2(111) single crystal surfaces. Evidence of benzene formation

S V Chong, Hicham Idriss

Research output: Contribution to journalArticle

24 Citations (Scopus)

Abstract

The reactions of aldehydes on metal oxide surfaces have exposed some of the most exquisite chemistry in comparison to their alcohol and carboxylic acid counterparts. Due to the intermediate oxidation state of the carbonyl carbon on an aldehyde, reactions such as the Cannizzaro disproportionation (forming alkoxides and carboxylates) and Tishchenko (forming ester) have been observed on various metal oxide surfaces, in addition to direct oxidation and reduction. Furthermore, condensation reactions have also been observed with aldehydes possessing alpha-H atom(s) over stoichiometric metal oxide surfaces, while surface defect sites are able to reductively couple two aldehyde adsorbates to yield alkene. Herein, we present the reactions of acetaldehyde over the stoichiometric, electron-irradiated, H-2-reduced, and argon ion-sputtered surfaces of a UO2 (1 1 1) single crystal. Temperature programmed desorption results over the four surfaces show evidence of benzene formation, and it appears that electron-irradiation slightly increases the conversion to benzene, H-2 reduction doubles it, and argon ion-sputtering increases it by fourfold. Thus the amount of benzene formed from acetaldehyde over a UO2 single crystal might be a novel way to quantitatively estimate the extent of surface defects. (C) 2001 American Vacuum Society.

Original languageEnglish
Pages (from-to)1933-1937
Number of pages5
JournalJournal of Vacuum Science & Technology. A, Vacuum, Surfaces, and Films
Volume19
Issue number4
Publication statusPublished - 2001

Keywords

  • TEMPERATURE-PROGRAMMED DESORPTION
  • SITU FT-IR
  • FURAN FORMATION
  • ETHANOL REACTIONS
  • URANIUM-DIOXIDE
  • UO2 SURFACES
  • CATALYSTS
  • OXIDE
  • ADSORPTION
  • CHEMISTRY

Cite this

Reactions of acetaldehyde on UO2(111) single crystal surfaces. Evidence of benzene formation. / Chong, S V ; Idriss, Hicham.

In: Journal of Vacuum Science & Technology. A, Vacuum, Surfaces, and Films, Vol. 19, No. 4, 2001, p. 1933-1937.

Research output: Contribution to journalArticle

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AU - Idriss, Hicham

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N2 - The reactions of aldehydes on metal oxide surfaces have exposed some of the most exquisite chemistry in comparison to their alcohol and carboxylic acid counterparts. Due to the intermediate oxidation state of the carbonyl carbon on an aldehyde, reactions such as the Cannizzaro disproportionation (forming alkoxides and carboxylates) and Tishchenko (forming ester) have been observed on various metal oxide surfaces, in addition to direct oxidation and reduction. Furthermore, condensation reactions have also been observed with aldehydes possessing alpha-H atom(s) over stoichiometric metal oxide surfaces, while surface defect sites are able to reductively couple two aldehyde adsorbates to yield alkene. Herein, we present the reactions of acetaldehyde over the stoichiometric, electron-irradiated, H-2-reduced, and argon ion-sputtered surfaces of a UO2 (1 1 1) single crystal. Temperature programmed desorption results over the four surfaces show evidence of benzene formation, and it appears that electron-irradiation slightly increases the conversion to benzene, H-2 reduction doubles it, and argon ion-sputtering increases it by fourfold. Thus the amount of benzene formed from acetaldehyde over a UO2 single crystal might be a novel way to quantitatively estimate the extent of surface defects. (C) 2001 American Vacuum Society.

AB - The reactions of aldehydes on metal oxide surfaces have exposed some of the most exquisite chemistry in comparison to their alcohol and carboxylic acid counterparts. Due to the intermediate oxidation state of the carbonyl carbon on an aldehyde, reactions such as the Cannizzaro disproportionation (forming alkoxides and carboxylates) and Tishchenko (forming ester) have been observed on various metal oxide surfaces, in addition to direct oxidation and reduction. Furthermore, condensation reactions have also been observed with aldehydes possessing alpha-H atom(s) over stoichiometric metal oxide surfaces, while surface defect sites are able to reductively couple two aldehyde adsorbates to yield alkene. Herein, we present the reactions of acetaldehyde over the stoichiometric, electron-irradiated, H-2-reduced, and argon ion-sputtered surfaces of a UO2 (1 1 1) single crystal. Temperature programmed desorption results over the four surfaces show evidence of benzene formation, and it appears that electron-irradiation slightly increases the conversion to benzene, H-2 reduction doubles it, and argon ion-sputtering increases it by fourfold. Thus the amount of benzene formed from acetaldehyde over a UO2 single crystal might be a novel way to quantitatively estimate the extent of surface defects. (C) 2001 American Vacuum Society.

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KW - CATALYSTS

KW - OXIDE

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KW - CHEMISTRY

M3 - Article

VL - 19

SP - 1933

EP - 1937

JO - Journal of Vacuum Science & Technology. A, Vacuum, Surfaces, and Films

JF - Journal of Vacuum Science & Technology. A, Vacuum, Surfaces, and Films

SN - 0734-2101

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ER -