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  Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and their Selectivity for the Electrochemical CO2 Reduction

Jeon, H., Timoshenko, J., Scholten, F., Sinev, I., Herzog, A., Haase, F., et al. (2019). Operando Insight into the Correlation between the Structure and Composition of CuZn Nanoparticles and their Selectivity for the Electrochemical CO2 Reduction. Journal of the American Chemical Society, 141(50), 19879-19887. doi:10.1021/jacs.9b10709.

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 Urheber:
Jeon, Hyosang1, Autor           
Timoshenko, Janis1, Autor           
Scholten, Fabian1, Autor           
Sinev, Ilya2, Autor
Herzog, Antonia1, Autor           
Haase, Felix1, Autor           
Roldan Cuenya, Beatriz1, Autor           
Affiliations:
1Interface Science, Fritz Haber Institute, Max Planck Society, ou_2461712              
2Department of Physics, Ruhr-University Bochum, 44780 Bochum, Germany, ou_persistent22              

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 Zusammenfassung: Bimetallic CuZn catalysts have been recently proposed as alternative in order to achieve selectivity control during the electrochemical reduction of CO2 (CO2RR). However, fundamental understanding of the underlying reaction mechanism and parameters determining the CO2RR performance is still missing. In this study we have employed size-controlled (~5 nm) Cu100-xZnx nanoparticles (NPs) supported on carbon to investigate the correlation between their structure and composition and catalytic performance. By tuning the concentration of Zn, a drastic increase in CH4 selectivity (~70% Faradaic efficiency (F.E.)) could be achieved for Zn contents from 10-50, which was accompanied by a suppression of the H2 production. Samples containing a higher Zn concentration displayed significantly lower CH4 production and an abrupt switch in the selectivity to CO. Lack of metal leaching was observed based on quasi in situ X-ray photoelectron spectroscopy (XPS). Operando X-ray absorption fine structure (XAFS) spectroscopy measurements revealed that the alloying of Cu atoms with Zn atoms takes place under reaction conditions and plays a determining role in the product selectivity. Time-dependent XAFS analysis showed that the local structure and chemical environment around the Cu atoms continuously evolve during CO2RR for several hours. In particular, cationic Zn species initially present were found to get reduced as the reaction proceeded, leading to the formation of a CuZn alloy (brass). The evolution of the Cu-Zn interaction with time during CO2RR was found to be responsible for the change in the selectivity from CH4 over Cu-ZnO NPs to CO over CuZn alloy NPs. This study highlights the importance of having access to in depth information on the interplay between the different atomic species in bimetallic NP electrocatalysts under operando reaction conditions in order to understand and ultimately tune their reactivity.

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Sprache(n): eng - English
 Datum: 2019-10-042019-11-242019-12-18
 Publikationsstatus: Erschienen
 Seiten: 9
 Ort, Verlag, Ausgabe: -
 Inhaltsverzeichnis: -
 Art der Begutachtung: Expertenbegutachtung
 Identifikatoren: DOI: 10.1021/jacs.9b10709
 Art des Abschluß: -

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Projektname : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Förderprogramm : Horizon 2020 (H2020)
Förderorganisation : European Commission (EC)

Quelle 1

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Titel: Journal of the American Chemical Society
  Andere : J. Am. Chem. Soc.
  Kurztitel : JACS
Genre der Quelle: Zeitschrift
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Affiliations:
Ort, Verlag, Ausgabe: Washington, DC : American Chemical Society
Seiten: 9 Band / Heft: 141 (50) Artikelnummer: - Start- / Endseite: 19879 - 19887 Identifikator: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870