Partial oxidation of propene on oxygen-covered Au(111)

Xingyi Deng, Byoung Koun Min, Xiaoying Liu, Cynthia M. Friend

Research output: Contribution to journalArticle

54 Citations (Scopus)

Abstract

Partial oxidation of propene is promoted by Au following deposition of atomic oxygen (0.3 ML) via O 3 decomposition on Au(111) at 200 K. Several partial oxidation products-acrolein, acrylic acid, and carbon suboxide (O=C=C=C=O)-are produced in competition with combustion to CO 2 and H 2O. Acrolein is the primary partial oxidation product, and it is further oxidized to the other products by excess oxygen. We propose that acrolein is derived from allyloxy intermediate that is formed via insertion of oxygen into the allylic C-H bond. While no propene epoxide formation is detected from oxidation of C 3H 6, a small amount of epoxidation is observed during reaction of C 3D 6 and CD 3CH=CH 2. These results are strong indications that small changes in the energy required for allylic C-H activation, in this case due to a kinetic isotope effect, may dramatically change the selectivity; thus, small modifications of the properties of oxygen on Au may lead to the more desirable epoxidation process. Our results are discussed in the context of the origin of activity of Au-based catalysts.

Original languageEnglish
Pages (from-to)15982-15987
Number of pages6
JournalJournal of Physical Chemistry B
Volume110
Issue number32
DOIs
Publication statusPublished - 2006 Aug 17
Externally publishedYes

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Acrolein
Propylene
Oxygen
Oxidation
oxidation
epoxidation
Epoxidation
oxygen
products
carbon suboxides
epoxy compounds
acrylic acid
Carbon Monoxide
Isotopes
isotope effect
Acrylics
insertion
indication
selectivity
Chemical activation

ASJC Scopus subject areas

  • Physical and Theoretical Chemistry

Cite this

Deng, X., Min, B. K., Liu, X., & Friend, C. M. (2006). Partial oxidation of propene on oxygen-covered Au(111). Journal of Physical Chemistry B, 110(32), 15982-15987. https://doi.org/10.1021/jp062305r

Partial oxidation of propene on oxygen-covered Au(111). / Deng, Xingyi; Min, Byoung Koun; Liu, Xiaoying; Friend, Cynthia M.

In: Journal of Physical Chemistry B, Vol. 110, No. 32, 17.08.2006, p. 15982-15987.

Research output: Contribution to journalArticle

Deng, X, Min, BK, Liu, X & Friend, CM 2006, 'Partial oxidation of propene on oxygen-covered Au(111)', Journal of Physical Chemistry B, vol. 110, no. 32, pp. 15982-15987. https://doi.org/10.1021/jp062305r
Deng, Xingyi ; Min, Byoung Koun ; Liu, Xiaoying ; Friend, Cynthia M. / Partial oxidation of propene on oxygen-covered Au(111). In: Journal of Physical Chemistry B. 2006 ; Vol. 110, No. 32. pp. 15982-15987.
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