Schumacher, Leon ; Radtke, Mariusz ; Welzenbach, Jan ; Hess, Christian (2024)
Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies.
In: Communications Chemistry, 2023, 6 (1)
doi: 10.26083/tuprints-00026657
Artikel, Zweitveröffentlichung, Verlagsversion
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Kurzbeschreibung (Abstract)
Iron(III) molybdate (Fe₂(MoO₄)₃) is a commercial catalyst for the oxidative dehydrogenation (ODH) of methanol, but it has recently been shown to be relevant for other substrates as well. Despite its commercial use, a detailed mechanistic understanding of Fe₂(MoO₄)₃ catalysts at the surface and in the bulk has been lacking, largely hampered by the lack of suitable spectroscopic methods, directly applicable under reaction conditions. Using propane ODH as an example, we highlight the potential of operando Raman and impedance spectroscopy combined with transient IR spectroscopy, to identify surface active sites and monitor the hydrogen transfer and oxygen dynamics. By comparison with the behavior of reference compounds (MoO₃, MoOₓ/Fe₂O₃) a mechanistic model is proposed. The presence of iron greatly influences the reactivity behavior via oxygen diffusion but is moderated in its oxidative capacity by surface MoOₓ. Our approach directly elucidates fundamental properties of Fe₂(MoO₄)₃ of general importance to selective oxidation catalysis.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Schumacher, Leon ; Radtke, Mariusz ; Welzenbach, Jan ; Hess, Christian |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies |
| Sprache: | Englisch |
| Publikationsjahr: | 24 April 2024 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 26 Oktober 2023 |
| Ort der Erstveröffentlichung: | London |
| Verlag: | Springer Nature |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | Communications Chemistry |
| Jahrgang/Volume einer Zeitschrift: | 6 |
| (Heft-)Nummer: | 1 |
| Kollation: | 9 Seiten |
| DOI: | 10.26083/tuprints-00026657 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/26657 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| Kurzbeschreibung (Abstract): | Iron(III) molybdate (Fe₂(MoO₄)₃) is a commercial catalyst for the oxidative dehydrogenation (ODH) of methanol, but it has recently been shown to be relevant for other substrates as well. Despite its commercial use, a detailed mechanistic understanding of Fe₂(MoO₄)₃ catalysts at the surface and in the bulk has been lacking, largely hampered by the lack of suitable spectroscopic methods, directly applicable under reaction conditions. Using propane ODH as an example, we highlight the potential of operando Raman and impedance spectroscopy combined with transient IR spectroscopy, to identify surface active sites and monitor the hydrogen transfer and oxygen dynamics. By comparison with the behavior of reference compounds (MoO₃, MoOₓ/Fe₂O₃) a mechanistic model is proposed. The presence of iron greatly influences the reactivity behavior via oxygen diffusion but is moderated in its oxidative capacity by surface MoOₓ. Our approach directly elucidates fundamental properties of Fe₂(MoO₄)₃ of general importance to selective oxidation catalysis. |
| Freie Schlagworte: | Catalytic mechanisms, Heterogeneous catalysis, Raman spectroscopy, Surface spectroscopy |
| ID-Nummer: | Artikel-ID: 230 (2023) |
| Status: | Verlagsversion |
| URN: | urn:nbn:de:tuda-tuprints-266575 |
| Sachgruppe der Dewey Dezimalklassifikatin (DDC): | 500 Naturwissenschaften und Mathematik > 540 Chemie |
| Fachbereich(e)/-gebiet(e): | DFG-Sonderforschungsbereiche (inkl. Transregio) DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche 07 Fachbereich Chemie 07 Fachbereich Chemie > Eduard Zintl-Institut 07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie DFG-Sonderforschungsbereiche (inkl. Transregio) > Sonderforschungsbereiche > SFB 1487: Eisen, neu gedacht! |
| Hinterlegungsdatum: | 24 Apr 2024 12:49 |
| Letzte Änderung: | 25 Apr 2024 07:24 |
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| Suche nach Titel in: | TUfind oder in Google |
Verfügbare Versionen dieses Eintrags
- Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies. (deposited 24 Apr 2024 12:49) [Gegenwärtig angezeigt]
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