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• W3203278317 abstract "Depressing the competitive hydrogen evolution reaction (HER) to promote current efficiency toward carbon-based chemicals in the electrocatalytic CO2 reduction reaction (CO2RR) is desirable. A strategy is to apply the hydrophobically molecular-modified electrodes. However, the molecular-scale catalytic process remains poorly understood. Using alkanethiol-modified hydrophobic Cu as an electrode and CO2-saturated KHCO3 as an electrolyte, we reveal that H2O, rather than HCO3–, is the major H+ source for the HER, determined by differential electrochemical mass spectrometry with isotopic labeling. As a result, using in situ Raman, we find that the hydrophobic molecules screen the cathodic electric field effect on the reorientation of interfacial H2O to a “H-down” configuration toward Cu surfaces that corresponds to the decreased content of H-bonding-free water, leading to unfavorable H2O dissociation and thus decreased H+ source for the HER. Further, density functional theory calculations suggest that the absorbed alkanethiol molecules alter the electronic structure of Cu sites, thus decreasing the formation energy barrier of CO2RR intermediates, which consequently increases the CO2RR selectivity. This work provides a molecular-level understanding of improved CO2RR on hydrophobically molecule-modified catalysts and presents general references for catalytic systems having H2O-involved competitive HER." @default.
• W3203278317 created "2021-10-11" @default.
• W3203278317 creator A5025557587 @default.
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• W3203278317 date "2021-09-28" @default.
• W3203278317 modified "2023-10-10" @default.
• W3203278317 title "Molecular-Scale Insights into Electrochemical Reduction of CO₂ on Hydrophobically Modified Cu Surfaces" @default.
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• W3203278317 doi "https://doi.org/10.1021/acsami.1c13529" @default.
• W3203278317 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/34582170" @default.
• W3203278317 hasPublicationYear "2021" @default.
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