The electrochemical conversion of CO_(2) into value‐added chemicals represents a critical strategy for sustainable energy utilization and environmental remediation.In this work,we develop a supramolecular engineering...The electrochemical conversion of CO_(2) into value‐added chemicals represents a critical strategy for sustainable energy utilization and environmental remediation.In this work,we develop a supramolecular engineering approach by constructing cucurbit[6]uril(CB[6])‐modified copper‐based electrocatalysts that create dynamic metal‐organic interfaces,which couple the captured CO_(2) with a hydrophobic surface microenvironment for efficient CO_(2) electroreduction to CO.Systematic investigations reveal that the functionalization with CB[6]simultaneously modulates the oxidation state of Cu sites,enriches local CO_(2) concentration via host‐vip interactions,and optimizes interfacial hydrophobicity.These synergistic effects lead to a significant enhancement in CO selectivity,achieving a faradaic efficiency of up to 98.3%for CO.The modified interfaces also demonstrate superior operational stability,maintaining catalytic activity for extended durations of up to 12 h.This study provides both fundamental insights into supramolecular interface engineering and a practical strategy for advancing CO_(2) conversion technologies.展开更多
基金L.P.acknowledges funding support from the National Natural Science Foundation of China(Grant 22373080)Fujian Provincial Natural Science Foundation of China(Grant 2024J08008)+2 种基金J.L.acknowledges funding support from the National Natural Science Foundation of China(Grant 22078274)S.Y.acknowledges funding support from the Fundamental Research Funds for the Central Universities(Grant 20720240054)the Nan‐qiang Youth Scholar Program of Xiamen University and Xiaomi Young Talents Program/Xiaomi Foundation.
文摘The electrochemical conversion of CO_(2) into value‐added chemicals represents a critical strategy for sustainable energy utilization and environmental remediation.In this work,we develop a supramolecular engineering approach by constructing cucurbit[6]uril(CB[6])‐modified copper‐based electrocatalysts that create dynamic metal‐organic interfaces,which couple the captured CO_(2) with a hydrophobic surface microenvironment for efficient CO_(2) electroreduction to CO.Systematic investigations reveal that the functionalization with CB[6]simultaneously modulates the oxidation state of Cu sites,enriches local CO_(2) concentration via host‐vip interactions,and optimizes interfacial hydrophobicity.These synergistic effects lead to a significant enhancement in CO selectivity,achieving a faradaic efficiency of up to 98.3%for CO.The modified interfaces also demonstrate superior operational stability,maintaining catalytic activity for extended durations of up to 12 h.This study provides both fundamental insights into supramolecular interface engineering and a practical strategy for advancing CO_(2) conversion technologies.
