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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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jacs.9b10709.pdf (Publisher version), 6MB
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 Creators:
Jeon, Hyosang1, Author              
Timoshenko, Janis1, Author              
Scholten, Fabian1, Author              
Sinev, Ilya2, Author
Herzog, Antonia1, Author              
Haase, Felix1, Author              
Roldan Cuenya, Beatriz1, Author              
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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 Abstract: 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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Language(s): eng - English
 Dates: 2019-10-042019-11-242019-12-18
 Publication Status: Published in print
 Pages: 9
 Publishing info: -
 Table of Contents: -
 Rev. Type: Peer
 Identifiers: DOI: 10.1021/jacs.9b10709
 Degree: -

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Project name : OPERANDOCAT - In situ and Operando Nanocatalysis: Size, Shape and Chemical State Effects
Grant ID : 725915
Funding program : Horizon 2020 (H2020)
Funding organization : European Commission (EC)

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Title: Journal of the American Chemical Society
  Other : J. Am. Chem. Soc.
  Abbreviation : JACS
Source Genre: Journal
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Publ. Info: Washington, DC : American Chemical Society
Pages: 9 Volume / Issue: 141 (50) Sequence Number: - Start / End Page: 19879 - 19887 Identifier: ISSN: 0002-7863
CoNE: https://pure.mpg.de/cone/journals/resource/954925376870