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Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies

Schumacher, Leon ; Radtke, Mariusz ; Welzenbach, Jan ; Hess, Christian (2023)
Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies.
In: Communications Chemistry, 6
doi: 10.1038/s42004-023-01028-8
Artikel, Bibliographie

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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: 2023
Autor(en): Schumacher, Leon ; Radtke, Mariusz ; Welzenbach, Jan ; Hess, Christian
Art des Eintrags: Bibliographie
Titel: Unraveling surface and bulk dynamics of iron(III) molybdate during oxidative dehydrogenation using operando and transient spectroscopies
Sprache: Englisch
Publikationsjahr: 26 Oktober 2023
Verlag: Springer Nature
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Communications Chemistry
Jahrgang/Volume einer Zeitschrift: 6
DOI: 10.1038/s42004-023-01028-8
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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.

Zusätzliche Informationen:

Artikel-ID: 260

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: 02 Nov 2023 06:05
Letzte Änderung: 25 Apr 2024 07:25
PPN: 512845808
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