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• W4380086722 abstract "Electrochemical CO2 reduction reaction (eCO2RR) is of great significance to energy and environmental engineering, while fundamental questions remain regarding its mechanisms. Herein, we formulate a fundamental understanding of the interplay between the applied potential (U) and kinetics of CO2 activation in eCO2RR on Cu surfaces. We find that the nature of the CO2 activation mechanism in eCO2RR varies with U, and it is the sequential electron-proton transfer (SEPT) mechanism dominant at the working U but switched to the concerted proton-electron transfer (CPET) mechanism at highly negative U. We then identify that the barrier of the electron-transfer step in the SEPT mechanism exhibits an inverted region as U decreases, which originates from the rapidly rising Pauli repulsion in the physisorption of CO2 with decreasing U. We further demonstrate catalyst designs that effectively suppress the adverse effect of Pauli repulsion. This fundamental understanding may be general for the electrochemical reduction reactions of closed-shell molecules." @default.
• W4380086722 created "2023-06-10" @default.
• W4380086722 creator A5023546157 @default.
• W4380086722 creator A5056828341 @default.
• W4380086722 date "2023-06-09" @default.
• W4380086722 modified "2023-10-06" @default.
• W4380086722 title "Inverted Region in Electrochemical Reduction of CO₂ Induced by Potential-Dependent Pauli Repulsion" @default.
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• W4380086722 doi "https://doi.org/10.1021/jacs.3c02447" @default.
• W4380086722 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/37294851" @default.
• W4380086722 hasPublicationYear "2023" @default.
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