Ziemba, Marc ; Schumacher, Leon ; Hess, Christian (2024)
The Reduction Behavior of Cubic In₂O₃ Nanoparticles by Combined Multi-In Situ Spectroscopy and DFT.
In: The Journal of Physical Chemistry Letters, 2021, 12 (15)
doi: 10.26083/tuprints-00028247
Artikel, Zweitveröffentlichung, Postprint
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Kurzbeschreibung (Abstract)
Indium oxide (In₂O₃) has emerged as a highly active catalyst for methanol synthesis by CO₂ hydrogenation. In this work we elucidate the reduction behavior and oxygen dynamics of cubic In₂O₃ nanoparticles by in situ Raman and UV–vis spectra in combination with density functional theory (DFT) calculations. We demonstrate that application of UV and visible Raman spectroscopy enables, first, a complete description of the In₂O₃ vibrational structure fully consistent with theory and, second, the first theoretical identification of the nature of defect-related bands in reduced In₂O₃. Combining these findings with quasi in situ XPS and in situ UV–vis measurements allows the temperature-dependent structural dynamics of In₂O₃ to be unraveled. While the surface of a particle is not in equilibrium with its bulk at room temperature, oxygen exchange between the bulk and the surface occurs at elevated temperatures, leading to an oxidation of the surface and an increase in oxygen defects in the bulk. Our results demonstrate the potential of combining different in situ spectroscopic methods with DFT to elucidate the complex redox behavior of In₂O₃ nanoparticles.
| Typ des Eintrags: | Artikel |
|---|---|
| Erschienen: | 2024 |
| Autor(en): | Ziemba, Marc ; Schumacher, Leon ; Hess, Christian |
| Art des Eintrags: | Zweitveröffentlichung |
| Titel: | The Reduction Behavior of Cubic In₂O₃ Nanoparticles by Combined Multi-In Situ Spectroscopy and DFT |
| Sprache: | Englisch |
| Publikationsjahr: | 6 Dezember 2024 |
| Ort: | Darmstadt |
| Publikationsdatum der Erstveröffentlichung: | 12 April 2021 |
| Ort der Erstveröffentlichung: | Washington, DC |
| Verlag: | American Chemical Society |
| Titel der Zeitschrift, Zeitung oder Schriftenreihe: | The Journal of Physical Chemistry Letters |
| Jahrgang/Volume einer Zeitschrift: | 12 |
| (Heft-)Nummer: | 15 |
| Kollation: | 19 Seiten |
| DOI: | 10.26083/tuprints-00028247 |
| URL / URN: | https://tuprints.ulb.tu-darmstadt.de/28247 |
| Zugehörige Links: | |
| Herkunft: | Zweitveröffentlichungsservice |
| Kurzbeschreibung (Abstract): | Indium oxide (In₂O₃) has emerged as a highly active catalyst for methanol synthesis by CO₂ hydrogenation. In this work we elucidate the reduction behavior and oxygen dynamics of cubic In₂O₃ nanoparticles by in situ Raman and UV–vis spectra in combination with density functional theory (DFT) calculations. We demonstrate that application of UV and visible Raman spectroscopy enables, first, a complete description of the In₂O₃ vibrational structure fully consistent with theory and, second, the first theoretical identification of the nature of defect-related bands in reduced In₂O₃. Combining these findings with quasi in situ XPS and in situ UV–vis measurements allows the temperature-dependent structural dynamics of In₂O₃ to be unraveled. While the surface of a particle is not in equilibrium with its bulk at room temperature, oxygen exchange between the bulk and the surface occurs at elevated temperatures, leading to an oxidation of the surface and an increase in oxygen defects in the bulk. Our results demonstrate the potential of combining different in situ spectroscopic methods with DFT to elucidate the complex redox behavior of In₂O₃ nanoparticles. |
| Freie Schlagworte: | Defects, Nanoparticles, Oxygen, Raman spectroscopy, Redox reactions |
| Status: | Postprint |
| URN: | urn:nbn:de:tuda-tuprints-282474 |
| 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: | 06 Dez 2024 13:13 |
| Letzte Änderung: | 09 Dez 2024 12:53 |
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- The Reduction Behavior of Cubic In₂O₃ Nanoparticles by Combined Multi-In Situ Spectroscopy and DFT. (deposited 06 Dez 2024 13:13) [Gegenwärtig angezeigt]
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