Zurhelle, Alexander F. ; Tong, Xiaorui ; Klein, Andreas ; Mebane, David S. ; De Souza, Roger A. (2017)
A Space-Charge Treatment of the Increased Concentration of Reactive Species at the Surface of a Ceria Solid Solution.
In: Angewandte Chemie International Edition, 56 (46)
doi: 10.1002/anie.201708118
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
A space‐charge theory applicable to concentrated solid solutions (Poisson–Cahn theory) was applied to describe quantitatively as a function of temperature and oxygen partial pressure published data obtained by in situ X‐ray photoelectron spectroscopy (XPS) for the concentration of Ce3+ (the reactive species) at the surface of the oxide catalyst Ce0.8Sm0.2O1.9. In contrast to previous theoretical treatments, these calculations clearly indicate that the surface is positively charged and compensated by an attendant negative space‐charge zone. The high space‐charge potential that develops at the surface (>0.8 V) is demonstrated to be hardly detectable by XPS measurements because of the short extent of the space‐charge layer. This approach emphasizes the need to take into account defect interactions and to allow deviations from local charge neutrality when considering the surfaces of oxide catalysts.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2017 |
| Autor(en): | Zurhelle, Alexander F. ; Tong, Xiaorui ; Klein, Andreas ; Mebane, David S. ; De Souza, Roger A. |
| Art des Eintrags: | Bibliographie |
| Titel: | A Space-Charge Treatment of the Increased Concentration of Reactive Species at the Surface of a Ceria Solid Solution |
| Sprache: | Englisch |
| Publikationsjahr: | 13 November 2017 |
| Verlag: | Wiley-VCH Verlag GmbH, Weinheim |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Angewandte Chemie International Edition |
| Jahrgang/Volume einer Zeitschrift: | 56 |
| (Heft-)Nummer: | 46 |
| DOI: | 10.1002/anie.201708118 |
| URL / URN: | https://doi.org/10.1002/anie.201708118 |
| Kurzbeschreibung (Abstract): | A space‐charge theory applicable to concentrated solid solutions (Poisson–Cahn theory) was applied to describe quantitatively as a function of temperature and oxygen partial pressure published data obtained by in situ X‐ray photoelectron spectroscopy (XPS) for the concentration of Ce3+ (the reactive species) at the surface of the oxide catalyst Ce0.8Sm0.2O1.9. In contrast to previous theoretical treatments, these calculations clearly indicate that the surface is positively charged and compensated by an attendant negative space‐charge zone. The high space‐charge potential that develops at the surface (>0.8 V) is demonstrated to be hardly detectable by XPS measurements because of the short extent of the space‐charge layer. This approach emphasizes the need to take into account defect interactions and to allow deviations from local charge neutrality when considering the surfaces of oxide catalysts. |
| Freie Schlagworte: | ceramics, ceria, space–charge theory, surface chemistry, thermodynamics |
| Fachbereich(e)/-gebiet(e): | 11 Fachbereich Material- und Geowissenschaften 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft 11 Fachbereich Material- und Geowissenschaften > Materialwissenschaft > Fachgebiet Oberflächenforschung |
| Hinterlegungsdatum: | 27 Okt 2017 10:54 |
| Letzte Änderung: | 26 Jun 2018 11:10 |
| PPN: | |
| Sponsoren: | he authors acknowledge funding from the Deutsche Forschungsgemeinschaft (DFG): from the collaborative research center SFB 917 “Nanoswitches”; from project SO499/7‐1; and from project KL1225/7‐1. |
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