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  The Mechanism of Interfacial CO2 Activation on Al Doped Cu/ZnO

Heenemann, M., Millet, M.-M., Girgsdies, F., Eichelbaum, M., Risse, T., Schlögl, R., et al. (2020). The Mechanism of Interfacial CO2 Activation on Al Doped Cu/ZnO. ACS Catalysis, 10, 5672-5680. doi:10.1021/acscatal.0c00574.

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 Creators:
Heenemann, Maria1, Author              
Millet, Marie-Mathilde1, Author              
Girgsdies, Frank1, Author              
Eichelbaum, Maik2, Author
Risse, Thomas3, Author
Schlögl, Robert1, 4, Author              
Jones, Travis1, Author              
Frei, Elias1, Author              
Affiliations:
1Inorganic Chemistry, Fritz Haber Institute, Max Planck Society, ou_24023              
2Technische Hochschule Nürnberg, Institute of Analytical Chemistry, Kefllerplatz 12, 90489 Nürnberg (Germany), ou_persistent22              
3Freie Universität Berlin, Institute of Chemistry and Biochemistry, Takustrafle 3, 14195 Berlin (Germany), ou_persistent22              
4Max Planck Institute for Chemical Energy Conversion, Max Planck Society, Mülheim an der Ruhr, DE, ou_3023867              

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 Abstract: We report on a combined quantitative charge carrier and catalytic activity analysis of Cu/ZnO model catalysts. The promoting effect of Al3+ on the ZnO support for CO2 activation via the reverse water-gas-shift reaction has been investigated. To the best of our knowledge, this is the first time that contact-free and operando microwave Hall Effect technique is applied to measure charge carriers in Cu/ZnO based model catalysts under reverse water-gas shift reaction conditions. This method allows us to monitor the electrical conductivity, charge carrier mobility, and absolute number of charge carriers. An increase in charge carrier concentration with increasing Al3+ content and its direct correlation with the catalytic activity for CO formation is found. We conclude that the increased availability of charge carriers plays a key role in CO2 activation and CO formation, which finds additional support in a concurrent decrease of the apparent activation energy and increase in the reaction order of CO2. In combination with comprehensive DFT calculations, the impact of the interfacial charge transfer, coupled to oxygen defect sites in ZnO and CO2 adsorption properties, is elucidated and highlighted. In conclusion, the results from this operando investigation combined with DFT calculations demonstrate the importance of charge transfer processes as decisive descriptors for understanding and explaining catalytic properties.

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Language(s): eng - English
 Dates: 2020-04-182020-02-032020-04-20
 Publication Status: Published online
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/acscatal.0c00574
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Title: ACS Catalysis
  Abbreviation : ACS Catal.
Source Genre: Journal
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Publ. Info: Washington, DC : ACS
Pages: 9 Volume / Issue: 10 Sequence Number: - Start / End Page: 5672 - 5680 Identifier: ISSN: 2155-5435
CoNE: https://pure.mpg.de/cone/journals/resource/2155-5435