Ziemba, Marc ; Weyel, Jakob ; Hess, Christian (2025)
Elucidating the Mechanism of the Reverse Water–Gas Shift Reaction over Au/CeO₂ Catalysts Using Operando and Transient Spectroscopies.
In: Applied Catalysis B: Environment and Energy, 2021, 301
doi: 10.26083/tuprints-00028223
Artikel, Zweitveröffentlichung, Postprint
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Kurzbeschreibung (Abstract)
The reaction mechanism of the reverse water–gas shift reaction (rWGSR) over Au/ceria catalysts was investigated by monitoring the catalyst dynamics and reaction intermediates using operando and transient spectroscopies, as well as by DFT calculations. Combined operando Raman and UV-Vis spectroscopic analysis allows establishing a correlation between subsurface oxygen vacancies and catalytic activity. Comparison of different ceria support materials, i.e., polyhedra and polycrystalline sheets, reveals that the defect concentration is not rate-determinant. Using transient DRIFTS, we are able to identify individual steps of hydrogen dissociation on supported gold and to gain detailed insight into the reduction of CO₂ via formate and carbonate formation. It is demonstrated that CO₂ reduction is influenced by the surface pretreatment. Considering all spectroscopic findings, we propose an associative mechanism via carbonate and formate intermediates as the main route for the rWGSR over Au/ceria(111) catalysts, while a redox mechanism plays only a minor role.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2025 |
| Autor(en): | Ziemba, Marc ; Weyel, Jakob ; Hess, Christian |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | Elucidating the Mechanism of the Reverse Water–Gas Shift Reaction over Au/CeO₂ Catalysts Using Operando and Transient Spectroscopies |
| Sprache: | Englisch |
| Publikationsjahr: | 13 Januar 2025 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 18 Oktober 2021 |
| Ort der Erstveröffentlichung: | Amsterdam |
| Verlag: | Elsevier |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Applied Catalysis B: Environment and Energy |
| Jahrgang/Volume einer Zeitschrift: | 301 |
| Kollation: | 33 Seiten |
| DOI: | 10.26083/tuprints-00028223 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/28223 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| Kurzbeschreibung (Abstract): | The reaction mechanism of the reverse water–gas shift reaction (rWGSR) over Au/ceria catalysts was investigated by monitoring the catalyst dynamics and reaction intermediates using operando and transient spectroscopies, as well as by DFT calculations. Combined operando Raman and UV-Vis spectroscopic analysis allows establishing a correlation between subsurface oxygen vacancies and catalytic activity. Comparison of different ceria support materials, i.e., polyhedra and polycrystalline sheets, reveals that the defect concentration is not rate-determinant. Using transient DRIFTS, we are able to identify individual steps of hydrogen dissociation on supported gold and to gain detailed insight into the reduction of CO₂ via formate and carbonate formation. It is demonstrated that CO₂ reduction is influenced by the surface pretreatment. Considering all spectroscopic findings, we propose an associative mechanism via carbonate and formate intermediates as the main route for the rWGSR over Au/ceria(111) catalysts, while a redox mechanism plays only a minor role. |
| Freie Schlagworte: | Gold-based catalyst, CeO₂, Reverse water–gas shift, CO₂ activation, Operando spectroscopy |
| Status: | Postprint |
| URN: | urn:nbn:de:tuda-tuprints-282237 |
| 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: | 13 Jan 2025 12:26 |
| Letzte Änderung: | 14 Jan 2025 06:17 |
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| Suche nach Titel in: | TUfind oder in Google |
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- Elucidating the Mechanism of the Reverse Water–Gas Shift Reaction over Au/CeO₂ Catalysts Using Operando and Transient Spectroscopies. (deposited 13 Jan 2025 12:26) [Gegenwärtig angezeigt]
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