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• W4386522925 endingPage "20213" @default.
• W4386522925 startingPage "20208" @default.
• W4386522925 abstract "Advances in electrocatalysis research rely heavily on building a thorough mechanistic understanding of catalyst active sites under realistic operating conditions. Only recently have techniques emerged that enable sensitive spectroscopic data collection to distinguish catalytically relevant surface sites from the underlying bulk material under applied potential in the presence of an electrolyte layer. Here, we demonstrate that operando high-energy-resolution fluorescence detected X-ray absorption spectroscopy (HERFD-XAS) is a powerful spectroscopic method which offers critical surface chemistry insights in CO2 electroreduction with sub-electronvolt energy resolution using hard X-rays. Combined with the high surface area-to-volume ratio of 5 nm copper nanoparticles, operando HERFD-XAS allows us to observe with clear evidence the breaking of chemical bonds between the ligands and the Cu surface as part of the ligand desorption process occurring under electrochemical potentials relevant for the CO2 reduction reaction (CO2RR). In addition, the dynamic evolution of oxidation state and coordination number throughout the operation of the nanocatalyst was continuously tracked. With these results in hand, undercoordinated metallic copper nanograins are proposed to be the real active sites in the CO2RR. This work emphasizes the importance of HERFD-XAS compared to routine XAS in catalyst characterization and mechanism exploration, especially in the complicated electrochemical CO2RR." @default.
• W4386522925 created "2023-09-08" @default.
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• W4386522925 date "2023-09-07" @default.
• W4386522925 modified "2023-10-15" @default.
• W4386522925 title "<i>Operando</i> High-Energy-Resolution X-ray Spectroscopy of Evolving Cu Nanoparticle Electrocatalysts for CO₂ Reduction" @default.
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• W4386522925 doi "https://doi.org/10.1021/jacs.3c08182" @default.
• W4386522925 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/37677089" @default.
• W4386522925 hasPublicationYear "2023" @default.
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