Theory-Guided Modification of Ionic Liquid on Cu2O Promotes Asymmetric C–C Coupling for CO2 Conversion

Le résumé fourni par la source

The electrocatalytic reduction of carbon dioxide (CO 2 RR) by copper oxide-based materials is conducive to the formation of high value-added products, but their activities and selectivities remain unsatisfactory. Organic ligand modification is a promising strategy to achieve a high CO 2 RR activity. Here, the modification of Cu 2 O with 1-butyl-3-methylimidazolium chloride (Bmim-Cu 2 O) enhanced the adsorption of reaction intermediates and improved the stability of the catalyst in the CO 2 RR, which displays a high Faradaic efficiency of ≈85% to C 2+ products with a current density as large as ≈352.5 mA cm –2 . In situ characterization reveals a stronger *CO signal with bridge configuration and a stronger *OCCHO signal over Bmim-Cu 2 O than unmodified Cu 2 O and can improve the stability during electrochemical CO 2 reduction. Density functional theory calculations show that local molecular modulation can effectively regulate the electronic structure of Cu 2 O and enhance the adsorption of *CO and *CHO intermediates through the stabilization of a noncovalent interaction, which can greatly promote the asymmetric *CO–*CHO coupling in the electrochemical reaction process.

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