Structure and Reactivity of Active Oxygen Species on Silver Surfaces for Ethylene Epoxidation.
ACS Catal
; 14(13): 10234-10244, 2024 Jul 05.
Article
en En
| MEDLINE
| ID: mdl-38988650
ABSTRACT
The epoxidation of ethylene stands as one of the most important industrial catalytic reactions, and silver-based catalysts show superior activity and selectivity. Oxygen is activated on the surface of silver during the reaction and exerts a substantial impact on product selectivity. Notably, the oxygen species residing in the topmost atomic layers profoundly influence the reactivity of a catalyst. However, their characterization under in situ reaction conditions remains a huge challenge, and specific structures have not been identified yet. In this study, we employ in situ X-ray photoelectron spectroscopy and density functional theory calculations to determine the oxygen species formed at the topmost atomic layers of a silver foil and to assign them a structure. Three different groups of oxygen species activated on silver are identified (i) surface lattice oxygen and two oxygen species originating from associatively adsorbed dioxygen and (ii) top and (iii) subsurface oxygen. Transient in situ photoelectron spectroscopy experiments are carried out to reveal the dynamic evolution and thus reactivity of the different oxygen species under ethylene epoxidation reaction environments. The top oxygen atom from the adsorbed associated dioxygen is the most active. Meanwhile, a frequency-selective data analysis method, developed to process time-resolved data, provides insights into the evolving trends of peak intensities for different oxygen species. The versatility of this method suggests its potential application in future time-resolved characterization studies.
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1
Colección:
01-internacional
Base de datos:
MEDLINE
Idioma:
En
Revista:
ACS Catal
Año:
2024
Tipo del documento:
Article
País de afiliación:
Suiza