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Investigation of Ethylene Oxide on Clean and Oxygen-Covered Ag(110) Surfaces

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Abstract

Temperature-programmed desorption (TPD) and Density Functional Theory (DFT) were used to investigate the reactions of oxametallacycles derived from ethylene oxide on clean and oxygen-covered Ag(110) surfaces. Ethylene oxide ring-opens following adsorption at 250 K on both clean and O-covered Ag(110) to form a stable oxametallacycle. On the clean Ag(110) surface, the oxametallacycle reacts to reform the parent epoxide at 280 K during TPD, while the aldehyde isomer, acetaldehyde, is observed at higher oxametallacycle coverages. In the presence of coadsorbed oxygen atoms, a portion of the oxametallacycles dissociate to release ethylene. However, of those that react to form oxygen-containing products, the fraction forming ethylene oxide is similar to that on the clean surface. The acetaldehyde product of oxametallacycle reactions combusts via formation of acetate species; the acetates react to form CO2 at temperatures as low as 360 K on the O-covered surface. No evidence was observed for other combustion channels. This work provides experimental evidence for the connection of oxametallacycles to combustion via acetaldehyde formation as well as to ring-closure to form ethylene oxide.

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Acknowledgement

We gratefully acknowledge the support of the US Department of Energy, Chemical Sciences Program, Grant FG02-84ER13290 for this research.

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Correspondence to Mark A. Barteau.

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Lukaski, A.C., Barteau, M.A. Investigation of Ethylene Oxide on Clean and Oxygen-Covered Ag(110) Surfaces. Catal Lett 128, 9–17 (2009). https://doi.org/10.1007/s10562-008-9802-0

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