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Understanding the Reduction Behavior of VOₓ/CeO₂ on a Molecular Level: Combining Temperature-Programmed Reduction with Multiple In Situ Spectroscopies and X-Ray Diffraction

Schumacher, Leon ; Ziemba, Marc ; Brunnengräber, Kai ; Totzauer, Lea ; Hofmann, Kathrin ; Etzold, Bastian J. M. ; Albert, Barbara ; Hess, Christian (2024)
Understanding the Reduction Behavior of VOₓ/CeO₂ on a Molecular Level: Combining Temperature-Programmed Reduction with Multiple In Situ Spectroscopies and X-Ray Diffraction.
In: The Journal of Physical Chemistry C, 2023, 127 (12)
doi: 10.26083/tuprints-00028238
Artikel, Zweitveröffentlichung, Postprint

WarnungEs ist eine neuere Version dieses Eintrags verfügbar.

Kurzbeschreibung (Abstract)

As catalytic processes become more important in academic and industrial applications, an intimate understanding is highly desirable to improve their efficiency on a rational basis. Because thorough mechanistic investigations require an elaborate and expensive spectroscopic and theoretical analysis, it is a major goal to link mechanistic insights to simple descriptors, such as the reducibility, that are accessible by temperature-programmed reduction (TPR) experiments, to bridge the gap between fundamental understanding and application of catalysts. In this work, we present a detailed in-situ spectroscopic analysis of TPR results from loading-dependent VOₓ/CeO₂ catalysts, using in-situ multiwavelength Raman, IR, UV–vis, and quasi-in-situ X-ray photoelectron spectroscopy as well as in-situ X-ray diffraction. The catalyst reduction shows a complex network of different processes, contributing to the overall reducibility, which are controlled by the unique interaction at the vanadia–ceria interface. The temperatures at which they occur depend significantly on the nuclearity of the surface vanadia species. By elucidating the temperature- and vanadia loading-dependent behavior, we provide a fundamental understanding of the underlying molecular processes, thus developing an important basis for interpretation of the reduction behavior of other oxide catalysts.

Typ des Eintrags: Artikel
Erschienen: 2024
Autor(en): Schumacher, Leon ; Ziemba, Marc ; Brunnengräber, Kai ; Totzauer, Lea ; Hofmann, Kathrin ; Etzold, Bastian J. M. ; Albert, Barbara ; Hess, Christian
Art des Eintrags: Zweitveröffentlichung
Titel: Understanding the Reduction Behavior of VOₓ/CeO₂ on a Molecular Level: Combining Temperature-Programmed Reduction with Multiple In Situ Spectroscopies and X-Ray Diffraction
Sprache: Englisch
Publikationsjahr: 6 Dezember 2024
Ort: Darmstadt
Publikationsdatum der Erstveröffentlichung: 20 März 2023
Ort der Erstveröffentlichung: Washington, DC
Verlag: American Chemical Society
Titel der Zeitschrift, Zeitung oder Schriftenreihe: The Journal of Physical Chemistry C
Jahrgang/Volume einer Zeitschrift: 127
(Heft-)Nummer: 12
Kollation: 41 Seiten
DOI: 10.26083/tuprints-00028238
URL / URN: https://tuprints.ulb.tu-darmstadt.de/28238
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Herkunft: Zweitveröffentlichungsservice
Kurzbeschreibung (Abstract):

As catalytic processes become more important in academic and industrial applications, an intimate understanding is highly desirable to improve their efficiency on a rational basis. Because thorough mechanistic investigations require an elaborate and expensive spectroscopic and theoretical analysis, it is a major goal to link mechanistic insights to simple descriptors, such as the reducibility, that are accessible by temperature-programmed reduction (TPR) experiments, to bridge the gap between fundamental understanding and application of catalysts. In this work, we present a detailed in-situ spectroscopic analysis of TPR results from loading-dependent VOₓ/CeO₂ catalysts, using in-situ multiwavelength Raman, IR, UV–vis, and quasi-in-situ X-ray photoelectron spectroscopy as well as in-situ X-ray diffraction. The catalyst reduction shows a complex network of different processes, contributing to the overall reducibility, which are controlled by the unique interaction at the vanadia–ceria interface. The temperatures at which they occur depend significantly on the nuclearity of the surface vanadia species. By elucidating the temperature- and vanadia loading-dependent behavior, we provide a fundamental understanding of the underlying molecular processes, thus developing an important basis for interpretation of the reduction behavior of other oxide catalysts.

Freie Schlagworte: Catalysts, Hydrogen, Oxides, Oxygen, Redox reactions
Status: Postprint
URN: urn:nbn:de:tuda-tuprints-282386
Sachgruppe der Dewey Dezimalklassifikatin (DDC): 500 Naturwissenschaften und Mathematik > 540 Chemie
Fachbereich(e)/-gebiet(e): 07 Fachbereich Chemie
07 Fachbereich Chemie > Ernst-Berl-Institut
07 Fachbereich Chemie > Eduard Zintl-Institut
07 Fachbereich Chemie > Eduard Zintl-Institut > Fachgebiet Physikalische Chemie
07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie
07 Fachbereich Chemie > Ernst-Berl-Institut > Fachgebiet Technische Chemie > Technische Chemie I
Hinterlegungsdatum: 06 Dez 2024 13:30
Letzte Änderung: 09 Dez 2024 12:44
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