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Elucidating CO₂ Hydrogenation over In₂O₃ Nanoparticles using Operando UV/Vis and Impedance Spectroscopies

Ziemba, Marc ; Radtke, Mariusz ; Schumacher, Leon ; Hess, Christian (2022)
Elucidating CO₂ Hydrogenation over In₂O₃ Nanoparticles using Operando UV/Vis and Impedance Spectroscopies.
In: Angewandte Chemie International Edition, 2022, 61 (39)
doi: 10.26083/tuprints-00022886
Article, Secondary publication, Publisher's Version

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Item Type: Article
Type of entry: Secondary publication
Title: Elucidating CO₂ Hydrogenation over In₂O₃ Nanoparticles using Operando UV/Vis and Impedance Spectroscopies
Language: English
Date: 2022
Place of Publication: Darmstadt
Year of primary publication: 2022
Publisher: Wiley-VCH
Journal or Publication Title: Angewandte Chemie International Edition
Volume of the journal: 61
Issue Number: 39
Collation: 8 Seiten
DOI: 10.26083/tuprints-00022886
Corresponding Links:
Origin: Secondary publication DeepGreen
Abstract:

In₂O₃ has emerged as a promising catalyst for CO₂ activation, but a fundamental understanding of its mode of operation in CO₂ hydrogenation is still missing, as the application of operando vibrational spectroscopy is challenging due to absorption effects. In this mechanistic study, we systematically address the redox processes related to the reverse water‐gas shift reaction (rWGSR) over In₂O₃ nanoparticles, both at the surface and in the bulk. Based on temperature‐dependent operando UV/Vis spectra and a novel operando impedance approach for thermal powder catalysts, we propose oxidation by CO₂ as the rate‐determining step for the rWGSR. The results are consistent with redox processes, whereby hydrogen‐containing surface species are shown to exhibit a promoting effect. Our findings demonstrate that oxygen/hydrogen dynamics, in addition to surface processes, are important for the activity, which is expected to be of relevance not only for In₂O₃ but also for other reducible oxide catalysts.

Uncontrolled Keywords: CO₂ Activation, In₂O₃, Operando Spectroscopy, Reaction Mechanism, Reverse Water-Gas Shift
Status: Publisher's Version
URN: urn:nbn:de:tuda-tuprints-228869
Additional Information:

International Version

Classification DDC: 500 Science and mathematics > 540 Chemistry
Divisions: 07 Department of Chemistry > Eduard Zintl-Institut > Physical Chemistry
Date Deposited: 23 Dec 2022 14:05
Last Modified: 05 Jan 2023 07:23
SWORD Depositor: Deep Green
URI: https://tuprints.ulb.tu-darmstadt.de/id/eprint/22886
PPN: 503275042
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