Nature of electrophilic oxygen: insights from periodic density functional theory investigations
Title | Nature of electrophilic oxygen: insights from periodic density functional theory investigations |
Publication Type | Journal Article |
Year of Publication | 2019 |
Authors | Kenge, N, Pitale, S, Joshi, K |
Journal | Surface Science |
Volume | 679 |
Pagination | 188-195 |
Date Published | JAN |
Type of Article | Article |
ISSN | 0039-6028 |
Keywords | Ag(100), DFT, Electrophilic, epoxidation, Nucleophilic oxygen |
Abstract | Increasing demand of ethylene oxide and the cost of versatile chemical ethene has been a driving force for understanding mechanism of epoxidation to develop highly selective catalytic process. Direct epoxidation is a proposed mechanism which in theory provides 100% selectivity. A key aspect of this mechanism is an electrophilic oxygen (O-ele) species forming on the Ag surface. In the past two and half decades, large number of theoretical and experimental investigations have tried to elucidate formation of O-ele, on Ag surface with little success. Equipped with this rich literature on Ag-O interactions, we investigate the same using periodic DFT calculations to further understand how silver surface and oxygen interact with each other from a chemical standpoint. Based on energetics, Lowdin charges, topologies and pdos data described in this study, we scrutinize the established notions of O-ele. Our study provides no evidence in support of O-ele, being an atomic species nor a diatomic molecular species. In fact, a triatomic molecular species described in this work bears multiple signatures which are very convincing evidence for considering it as the most sought for electrophilic entity. |
DOI | 10.1016/j.susc.2018.09.009 |
Type of Journal (Indian or Foreign) | Foreign |
Impact Factor (IF) | 1.997 |
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