On the effectiveness of partial oxidation of propylene by gold: A density functional theory study

The two different OMMP intermediates – OMMP1 (left) and OMMP2 (right) – involved in the primary chemistry of propylene partial oxidation on Au(111). The catalytic effectiveness of extended gold surfaces on the partial oxidation of olefins containing an allylic C–H bond is studied by means of periodi...

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Bibliographic Details
Published in:Journal of molecular catalysis. A, Chemical Chemical, 2009-07, Vol.306 (1-2), p.6-10
Main Authors: Roldan, Alberto, Torres, Daniel, Ricart, Josep M., Illas, Francesc
Format: Article
Language:English
Subjects:
Catalysis
Catalysis by Au
Chemistry
DFT
Exact sciences and technology
General and physical chemistry
Propene epoxidation
Theory of reactions, general kinetics. Catalysis. Nomenclature, chemical documentation, computer chemistry
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Summary:The two different OMMP intermediates – OMMP1 (left) and OMMP2 (right) – involved in the primary chemistry of propylene partial oxidation on Au(111). The catalytic effectiveness of extended gold surfaces on the partial oxidation of olefins containing an allylic C–H bond is studied by means of periodic density functional calculations applied to slab models representing Au(111). Results show that the H-stripping, leading to an adsorbed allyl and OH radicals is by far more probable than the one leading to the formation of oxametallacycle intermediates, which is the necessary step towards the partial oxidation of propylene. Our observations suggest that the failure of extended gold surfaces arises from the high sensitivity of the molecular mechanism toward changes in the basic character of adsorbed oxygen, in line with previous findings.
ISSN:1381-1169
1873-314X
DOI:10.1016/j.molcata.2009.02.013