Operando insights into correlating CO coverage and Cu-Au alloying with the selectivity of Au NP-decorated Cu 2 O nanocubes during the electrocatalytic CO 2 reduction.

Autor:	Rettenmaier C; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Herzog A; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Casari D; Electron Spectrometry and Microscopy Laboratory (LSME), Institute of Physics (IPHYS), École Polytechnique Fédérale de Lausanne (EPFL) Lausanne CH-1015 Switzerland., Rüscher M; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Jeon HS; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Kordus D; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Luna ML; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Kühl S; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Hejral U; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Davis EM; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Chee SW; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Timoshenko J; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Alexander DTL; Electron Spectrometry and Microscopy Laboratory (LSME), Institute of Physics (IPHYS), École Polytechnique Fédérale de Lausanne (EPFL) Lausanne CH-1015 Switzerland., Bergmann A; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de., Cuenya BR; Department of Interface Science, Fritz-Haber-Institute of the Max-Planck Society Faradayweg 4-6 14195 Berlin Germany roldan@fhi-berlin.mpg.de.
Jazyk:	angličtina
Zdroj:	EES catalysis [EES Catal] 2023 Oct 25; Vol. 2 (1), pp. 311-323. Date of Electronic Publication: 2023 Oct 25 (Print Publication: 2024).
DOI:	10.1039/d3ey00162h
Abstrakt:	Electrochemical reduction of CO 2 (CO 2 RR) is an attractive technology to reintegrate the anthropogenic CO 2 back into the carbon cycle driven by a suitable catalyst. This study employs highly efficient multi-carbon (C 2+ ) producing Cu 2 O nanocubes (NCs) decorated with CO-selective Au nanoparticles (NPs) to investigate the correlation between a high CO surface concentration microenvironment and the catalytic performance. Structure, morphology and near-surface composition are studied via operando X-ray absorption spectroscopy and surface-enhanced Raman spectroscopy, operando high-energy X-ray diffraction as well as quasi in situ X-ray photoelectron spectroscopy. These operando studies show the continuous evolution of the local structure and chemical environment of our catalysts during reaction conditions. Along with its alloy formation, a CO-rich microenvironment as well as weakened average CO binding on the catalyst surface during CO 2 RR is detected. Linking these findings to the catalytic function, a complex compositional interplay between Au and Cu is revealed in which higher Au loadings primarily facilitate CO formation. Nonetheless, the strongest improvement in C 2+ formation appears for the lowest Au loadings, suggesting a beneficial role of the Au-Cu atomic interaction for the catalytic function in CO 2 RR. This study highlights the importance of site engineering and operando investigations to unveil the electrocatalyst's adaptations to the reaction conditions, which is a prerequisite to understand its catalytic behavior. Competing Interests: There are no conflicts to declare. (This journal is © The Royal Society of Chemistry.)
Databáze:	MEDLINE
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