Ruff, Philip ; Schumacher, Leon ; Rogg, Simone ; Hess, Christian (2024)
Atomic Layer Deposition-Assisted Synthesis of Embedded Vanadia Catalysts.
In: ACS Catalysis, 2019, 9 (7)
doi: 10.26083/tuprints-00028250
Artikel, Zweitveröffentlichung, Postprint
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Kurzbeschreibung (Abstract)
Catalyst–support interactions are known to be of great importance for the performance of supported oxide catalysts such as supported vanadia. With the aim of enhancing the oxide–support interactions, we propose a strategy for the controlled synthesis of embedded oxide catalysts using atomic layer deposition (ALD). As demonstrated for vanadia (VOₓ), the synthesis is based on the sequential deposition of VOₓ and the “support” material (Al₂O₃, SiO₂, TiO₂) onto graphene oxide, which serves as a sacrificial carrier matrix facilitating the embedding of VOₓ, followed by template removal by calcination or ozone treatment. Detailed characterization of the synthesis process and the final catalysts is carried out using multiple spectroscopic (Raman, UV–vis, XPS), thermogravimetric, and electron-microscopic (TEM, EELS) analyses. The successful formation of a VOₓ–support interphase is confirmed by UV Raman spectroscopy. Despite the high loadings (Lᵥ > monolayer coverage) of accessible sites, the embedded VOₓ is present in a dispersed state in the case of the ozonolyzed samples. Structural models are proposed to account for the observed behavior. The activity of the embedded VOₓ catalysts is verified in the oxidative dehydrogenation (ODH) of ethanol and compares favorably with reported data on conventional supported catalysts. Compared to the literature, the ozonolyzed VOₓ/Al₂O₃ catalysts show a significantly improved performance, whereas the VOₓ/SiO₂ catalysts define a benchmark. Our results demonstrate the feasibility of rational catalyst engineering of supported oxide catalysts.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Ruff, Philip ; Schumacher, Leon ; Rogg, Simone ; Hess, Christian |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | Atomic Layer Deposition-Assisted Synthesis of Embedded Vanadia Catalysts |
| Sprache: | Englisch |
| Publikationsjahr: | 29 Oktober 2024 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 3 Juni 2019 |
| Ort der Erstveröffentlichung: | Washington, DC |
| Verlag: | American Chemical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | ACS Catalysis |
| Jahrgang/Volume einer Zeitschrift: | 9 |
| (Heft-)Nummer: | 7 |
| Kollation: | 40 Seiten |
| DOI: | 10.26083/tuprints-00028250 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/28250 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| Kurzbeschreibung (Abstract): | Catalyst–support interactions are known to be of great importance for the performance of supported oxide catalysts such as supported vanadia. With the aim of enhancing the oxide–support interactions, we propose a strategy for the controlled synthesis of embedded oxide catalysts using atomic layer deposition (ALD). As demonstrated for vanadia (VOₓ), the synthesis is based on the sequential deposition of VOₓ and the “support” material (Al₂O₃, SiO₂, TiO₂) onto graphene oxide, which serves as a sacrificial carrier matrix facilitating the embedding of VOₓ, followed by template removal by calcination or ozone treatment. Detailed characterization of the synthesis process and the final catalysts is carried out using multiple spectroscopic (Raman, UV–vis, XPS), thermogravimetric, and electron-microscopic (TEM, EELS) analyses. The successful formation of a VOₓ–support interphase is confirmed by UV Raman spectroscopy. Despite the high loadings (Lᵥ > monolayer coverage) of accessible sites, the embedded VOₓ is present in a dispersed state in the case of the ozonolyzed samples. Structural models are proposed to account for the observed behavior. The activity of the embedded VOₓ catalysts is verified in the oxidative dehydrogenation (ODH) of ethanol and compares favorably with reported data on conventional supported catalysts. Compared to the literature, the ozonolyzed VOₓ/Al₂O₃ catalysts show a significantly improved performance, whereas the VOₓ/SiO₂ catalysts define a benchmark. Our results demonstrate the feasibility of rational catalyst engineering of supported oxide catalysts. |
| Freie Schlagworte: | atomic layer deposition, vanadia, embedded catalyst, oxidative dehydrogenation, sacrificial template, graphene oxide |
| Status: | Postprint |
| URN: | urn:nbn:de:tuda-tuprints-282508 |
| 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: | 29 Okt 2024 13:37 |
| Letzte Änderung: | 30 Okt 2024 09:06 |
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- Atomic Layer Deposition-Assisted Synthesis of Embedded Vanadia Catalysts. (deposited 29 Okt 2024 13:37) [Gegenwärtig angezeigt]
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