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Abstract Recent heterogeneous catalysis studies have demonstrated that synergy between Ag and Cu can lead to more selective partial oxidation chemistries. We performed a series of scanning tunneling microscope experiments to gain a better understanding of the AgCu system under oxidative conditions. These experiments were carried out by exposing sub‐monolayer coverages of Ag on Cu(111), in the form of a near‐surface alloy (NSA), to range of oxygen exposures and temperatures. This enabled us to study the initial stages of oxidation of well‐defined Ag/Cu interfaces with atomic resolution and thereby understand the dynamic response of the AgCu NSA to oxygen environments. At low oxygen exposures, oxidation was observed on exposed Cu terraces and at the interface between the AgCu NSA and Cu(111). Higher oxygen exposure led to the segregation of Cu atoms up through the Ag layer and the appearance of surface adsorbed oxygen. Significant phase segregation of Cu was then observed at higher oxygen exposures at elevated temperatures, evidenced by the formation of Cu oxide patches within and on the top of the Ag layer. These results provide a more detailed picture of how AgCu NSAs interact with, and restructure in response to, oxygen.
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Heterogeneously Catalyzed Partial Oxidation of Styrene on a Silver Surface
Abstract The epoxidation of olefins on Ag/O systems is a significant industrial‐scale process within heterogeneous catalysis. However, the details of the surface reaction remain controversial, and it has been highly challenging to reconcile the findings from cataltyic studies under reaction conditions with the highly detailed static studies under carefully controlled ultra‐high vacuum (UHV) conditions. In this study, we combine molecular beam surface scattering and ion imaging techniques to explore the partial oxidation of styrene. This experimental approach enhances the sensitivity to the extent that we can directly observe the partial oxidation product, styrene oxide, under UHV conditions. We note that partial oxidation exclusively occurs at high oxygen coverages, which we attribute to the reaction of styrene with electrophilic oxygen formed specifically at elevated coverages.
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- Award ID(s):
- 2155068
- PAR ID:
- 10509493
- Publisher / Repository:
- Wiley Blackwell (John Wiley & Sons)
- Date Published:
- Journal Name:
- ChemCatChem
- Volume:
- 16
- Issue:
- 17
- ISSN:
- 1867-3880
- Format(s):
- Medium: X
- Sponsoring Org:
- National Science Foundation
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