Weyel, Jakob ; Hess, Christian (2024)
Refining the mechanism of CO₂ and H₂ activation over gold-ceria catalysts by IR modulation excitation spectroscopy.
In: Physical Chemistry Chemical Physics, 26 (8)
doi: 10.1039/D3CP05102A
Artikel, Bibliographie
Kurzbeschreibung (Abstract)
The activation and utilization of the greenhouse gas CO₂ is of great interest to the energy transition as a fossil-free carbon source mitigating the climate change. CO₂ hydrogenation via the reverse water-gas shift reaction (RWGSR) converts CO₂ to CO, a crucial component of syngas, enabling further transformation by means of the Fischer-Tropsch process. In this study, we unravel the detailed mechanism of the RWGSR on low-loaded Au/CeO₂ catalysts using IR modulation excitation spectroscopy (MES), by periodically modulating the concentration of the reactants, followed by phase-sensitive detection (PSD). Applying such an MES-PSD approach to Au/CeO₂ catalysts during RWGSR gives direct spectroscopic evidence for the active role of gold hydride, bidentate carbonate and hydroxyl species in the reaction mechanism, while disproving the participation of other species such as formate. Our results highlight the potential of modulation-excitation spectroscopy combined with phase-sensitive detection to provide new mechanistic insight into catalytic reactions not accessible by steady-state techniques, including a profound understanding of the sequence of reaction steps.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Weyel, Jakob ; Hess, Christian |
| Art des Eintrags: | Bibliographie |
| Titel: | Refining the mechanism of CO₂ and H₂ activation over gold-ceria catalysts by IR modulation excitation spectroscopy |
| Sprache: | Englisch |
| Publikationsjahr: | 2024 |
| Verlag: | Royal Society of Chemistry |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Physical Chemistry Chemical Physics |
| Jahrgang/Volume einer Zeitschrift: | 26 |
| (Heft-)Nummer: | 8 |
| Kollation: | 20 Seiten |
| DOI: | 10.1039/D3CP05102A |
| URL / URN: | https://pubs.rsc.org/en/content/articlelanding/2024/cp/d3cp0... |
| Kurzbeschreibung (Abstract): | The activation and utilization of the greenhouse gas CO₂ is of great interest to the energy transition as a fossil-free carbon source mitigating the climate change. CO₂ hydrogenation via the reverse water-gas shift reaction (RWGSR) converts CO₂ to CO, a crucial component of syngas, enabling further transformation by means of the Fischer-Tropsch process. In this study, we unravel the detailed mechanism of the RWGSR on low-loaded Au/CeO₂ catalysts using IR modulation excitation spectroscopy (MES), by periodically modulating the concentration of the reactants, followed by phase-sensitive detection (PSD). Applying such an MES-PSD approach to Au/CeO₂ catalysts during RWGSR gives direct spectroscopic evidence for the active role of gold hydride, bidentate carbonate and hydroxyl species in the reaction mechanism, while disproving the participation of other species such as formate. Our results highlight the potential of modulation-excitation spectroscopy combined with phase-sensitive detection to provide new mechanistic insight into catalytic reactions not accessible by steady-state techniques, including a profound understanding of the sequence of reaction steps. |
| Freie Schlagworte: | 2024 HOT PCCP article |
| Zusätzliche Informationen: | Award: Part of the 2024 HOT articles collection. |
| Fachbereich(e)/-gebiet(e): | 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie |
| Hinterlegungsdatum: | 02 Feb 2024 09:53 |
| Letzte Änderung: | 13 Mär 2024 09:54 |
| PPN: | 515222100 |
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