Schilling, Christian ; Ganduglia-Pirovano, M. Verónica ; Hess, Christian (2018)
Experimental and theoretical study on the nature of adsorbed oxygen species on shaped ceria nanoparticles.
In: The Journal of Physical Chemistry Letters, 9 (22)
doi: 10.1021/acs.jpclett.8b02728
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
Ceria is widely used in heterogeneous catalysis owing to its redox properties. Engineering the shape of ceria particles offers a powerful tool to develop materials with enhanced catalytic properties. In this study, we provide evidence for the shape-dependent dioxygen adsorption and activation of ceria nanoparticles with (111) and (100) facets by in situ Raman spectroscopy and relate these properties to unique adsorption sites employing density functional theory. Temperature- and gas-phase-dependent experiments demonstrate facilitated formation of peroxide, superoxide, and weakly bound dioxygen species on the (100) facets as rationalized by calculated vibrational frequencies of O₂²⁻, O₂⁻, and O₂ species on CeO₂₋ₓ(100) surfaces. Our results show that localization of the excess charge, driving the Ce⁴⁺ → Ce³⁺ reduction, significantly affects the stretching vibrations. Our approach provides a powerful basis for future developments of ceria-based catalysts by bridging the materials gap between idealized and real catalytic systems.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2018 |
| Autor(en): | Schilling, Christian ; Ganduglia-Pirovano, M. Verónica ; Hess, Christian |
| Art des Eintrags: | Bibliographie |
| Titel: | Experimental and theoretical study on the nature of adsorbed oxygen species on shaped ceria nanoparticles |
| Sprache: | Englisch |
| Publikationsjahr: | 2018 |
| Verlag: | American Chemical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | The Journal of Physical Chemistry Letters |
| Jahrgang/Volume einer Zeitschrift: | 9 |
| (Heft-)Nummer: | 22 |
| DOI: | 10.1021/acs.jpclett.8b02728 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | Ceria is widely used in heterogeneous catalysis owing to its redox properties. Engineering the shape of ceria particles offers a powerful tool to develop materials with enhanced catalytic properties. In this study, we provide evidence for the shape-dependent dioxygen adsorption and activation of ceria nanoparticles with (111) and (100) facets by in situ Raman spectroscopy and relate these properties to unique adsorption sites employing density functional theory. Temperature- and gas-phase-dependent experiments demonstrate facilitated formation of peroxide, superoxide, and weakly bound dioxygen species on the (100) facets as rationalized by calculated vibrational frequencies of O₂²⁻, O₂⁻, and O₂ species on CeO₂₋ₓ(100) surfaces. Our results show that localization of the excess charge, driving the Ce⁴⁺ → Ce³⁺ reduction, significantly affects the stretching vibrations. Our approach provides a powerful basis for future developments of ceria-based catalysts by bridging the materials gap between idealized and real catalytic systems. |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie Zentrale Einrichtungen Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) Zentrale Einrichtungen > Hochschulrechenzentrum (HRZ) > Hochleistungsrechner |
| Hinterlegungsdatum: | 31 Okt 2018 10:32 |
| Letzte Änderung: | 30 Okt 2024 09:14 |
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| Suche nach Titel in: | TUfind oder in Google |
Verfügbare Versionen dieses Eintrags
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Experimental and Theoretical Study on the Nature of Adsorbed Oxygen Species on Shaped Ceria Nanoparticles. (deposited 29 Okt 2024 13:29)
- Experimental and theoretical study on the nature of adsorbed oxygen species on shaped ceria nanoparticles. (deposited 31 Okt 2018 10:32) [Gegenwärtig angezeigt]
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