Schumacher, Leon ; Weyel, Jakob ; Hess, Christian (2022)
Unraveling the Active Vanadium Sites and Adsorbate Dynamics in VOₓ/CeO₂ Oxidation Catalysts Using Transient IR Spectroscopy.
In: Journal of the American Chemical Society, 144 (32)
doi: 10.1021/jacs.2c06303
Artikel, Bibliographie
Dies ist die neueste Version dieses Eintrags.
Kurzbeschreibung (Abstract)
The oxidative dehydrogenation (ODH) of propane over supported vanadia catalysts is an attractive route toward propene (propylene) with the potential of industrial application and has been extensively studied over decades. Despite numerous mechanistic studies, the active vanadyl site of the reaction has not been elucidated. In this work, we unravel the ODH reaction mechanism, including the nuclearity-dependent vanadyl and surface dynamics, over ceria-supported vanadia (VOₓ/CeO₂) catalysts by applying (isotopic) modulation excitation IR spectroscopy supported by operando Raman and UV–vis spectroscopies. Based on our loading-dependent analysis, we were able to identify two different mechanisms leading to propylene, which are characterized by isopropyl- and acrylate-like intermediates. The modulation excitation IR approach also allows for the determination of the time evolution of the vanadia, hydroxyl, and adsorbate dynamics, underlining the intimate interplay between the surface vanadia species and the ceria support. Our results highlight the potential of transient IR spectroscopy to provide a detailed understanding of reaction mechanisms in oxidation catalysis and the dynamics of surface catalytic processes in general.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2022 |
| Autor(en): | Schumacher, Leon ; Weyel, Jakob ; Hess, Christian |
| Art des Eintrags: | Bibliographie |
| Titel: | Unraveling the Active Vanadium Sites and Adsorbate Dynamics in VOₓ/CeO₂ Oxidation Catalysts Using Transient IR Spectroscopy |
| Sprache: | Englisch |
| Publikationsjahr: | 2 August 2022 |
| Ort: | Washington, DC |
| Verlag: | American Chemical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Journal of the American Chemical Society |
| Jahrgang/Volume einer Zeitschrift: | 144 |
| (Heft-)Nummer: | 32 |
| Kollation: | 40 Seiten |
| DOI: | 10.1021/jacs.2c06303 |
| Zugehörige Links: | |
| Kurzbeschreibung (Abstract): | The oxidative dehydrogenation (ODH) of propane over supported vanadia catalysts is an attractive route toward propene (propylene) with the potential of industrial application and has been extensively studied over decades. Despite numerous mechanistic studies, the active vanadyl site of the reaction has not been elucidated. In this work, we unravel the ODH reaction mechanism, including the nuclearity-dependent vanadyl and surface dynamics, over ceria-supported vanadia (VOₓ/CeO₂) catalysts by applying (isotopic) modulation excitation IR spectroscopy supported by operando Raman and UV–vis spectroscopies. Based on our loading-dependent analysis, we were able to identify two different mechanisms leading to propylene, which are characterized by isopropyl- and acrylate-like intermediates. The modulation excitation IR approach also allows for the determination of the time evolution of the vanadia, hydroxyl, and adsorbate dynamics, underlining the intimate interplay between the surface vanadia species and the ceria support. Our results highlight the potential of transient IR spectroscopy to provide a detailed understanding of reaction mechanisms in oxidation catalysis and the dynamics of surface catalytic processes in general. |
| Freie Schlagworte: | Alkyls, Anions, Catalysts, Oxides, Oxygen |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie |
| Hinterlegungsdatum: | 20 Dez 2024 08:49 |
| Letzte Änderung: | 20 Dez 2024 08:49 |
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Verfügbare Versionen dieses Eintrags
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Unraveling the Active Vanadium Sites and Adsorbate Dynamics in VOₓ/CeO₂ Oxidation Catalysts Using Transient IR Spectroscopy. (deposited 05 Dez 2024 13:50)
- Unraveling the Active Vanadium Sites and Adsorbate Dynamics in VOₓ/CeO₂ Oxidation Catalysts Using Transient IR Spectroscopy. (deposited 20 Dez 2024 08:49) [Gegenwärtig angezeigt]
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