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CO₂ as a soft oxidant for propane oxidative dehydrogenation: a mechanistic study using operando UV Raman spectroscopy

Rogg, Simone ; Hess, Christian (2025)
CO₂ as a soft oxidant for propane oxidative dehydrogenation: a mechanistic study using operando UV Raman spectroscopy.
In: Journal of CO2 Utilization, 2021, 50
doi: 10.26083/tuprints-00028222
Artikel, Zweitveröffentlichung, Postprint

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Kurzbeschreibung (Abstract)

The utilization of CO₂ as an oxidant has recently attracted increasing attention due to its mild oxidizing properties allowing higher product selectivities to be achieved e.g. in propane oxidative dehydrogenation (ODH). In this communication we address mechanistic aspects of propane ODH over silica supported vanadia (VOₓ/SiO₂) catalysts in the presence of CO₂ as oxidizing agent. The use of operando UV Raman spectroscopy reveals distinct changes in the surface vanadia structure including breakage of V-O-V bonds and a partial reduction of vanadyl, as well as the formation of support hydroxyl groups, while the presence of CO₂ is observed to prevent coke deposition. Our results are fully consistent with the occurrence of two parallel pathways, i.e., direct ODH (one step) and dehydrogenation followed by a reverse water-gas shift reaction (two step), supporting previous literature proposals.

Typ des Eintrags: Artikel
Erschienen: 2025
Autor(en): Rogg, Simone ; Hess, Christian
Art des Eintrags: Zweitveröffentlichung
Titel: CO₂ as a soft oxidant for propane oxidative dehydrogenation: a mechanistic study using operando UV Raman spectroscopy
Sprache: Englisch
Publikationsjahr: 13 Januar 2025
Ort: Darmstadt
Publikationsdatum der Erstveröffentlichung: 5 Juni 2021
Ort der Erstveröffentlichung: Amsterdam [u.a.]
Verlag: Elsevier
Titel der Zeitschrift, Zeitung oder Schriftenreihe: Journal of CO2 Utilization
Jahrgang/Volume einer Zeitschrift: 50
Kollation: 24 Seiten
DOI: 10.26083/tuprints-00028222
URL / URN: https://tuprints.ulb.tu-darmstadt.de/28222
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Herkunft: Zweitveröffentlichungsservice
Kurzbeschreibung (Abstract):

The utilization of CO₂ as an oxidant has recently attracted increasing attention due to its mild oxidizing properties allowing higher product selectivities to be achieved e.g. in propane oxidative dehydrogenation (ODH). In this communication we address mechanistic aspects of propane ODH over silica supported vanadia (VOₓ/SiO₂) catalysts in the presence of CO₂ as oxidizing agent. The use of operando UV Raman spectroscopy reveals distinct changes in the surface vanadia structure including breakage of V-O-V bonds and a partial reduction of vanadyl, as well as the formation of support hydroxyl groups, while the presence of CO₂ is observed to prevent coke deposition. Our results are fully consistent with the occurrence of two parallel pathways, i.e., direct ODH (one step) and dehydrogenation followed by a reverse water-gas shift reaction (two step), supporting previous literature proposals.

Freie Schlagworte: Propylene, Oxidative dehydrogenation (ODH), CO₂, Reverse water-gas shift, Supported metal oxide, Vanadia, Operando Raman, Reaction mechanism
Status: Postprint
URN: urn:nbn:de:tuda-tuprints-282222
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 12:25
Letzte Änderung: 14 Jan 2025 06:14
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