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• W3201958423 endingPage "16864" @default.
• W3201958423 startingPage "16849" @default.
• W3201958423 abstract "We report the design, synthesis, and characterization of four N-annulated perylene diimide (NPDI) functionalized rhenium bipyridine [Re(bpy)] supramolecular dyads. The Re(bpy) scaffold was connected to the NPDI chromophore either directly [Re(py-C0-NPDI)] or via an ethyl [Re(bpy-C2-NPDI)], butyl [Re(bpy-C4-NPDI)], or hexyl [Re(bpy-C6-NPDI)] alkyl-chain spacer. Upon electrochemical reduction in the presence of CO2 and a proton source, Re(bpy-C2/4/6-NPDI) all exhibited significant current enhancement effects, while Re(py-C0-NPDI) did not. During controlled potential electrolysis (CPE) experiments at Eappl = −1.8 V vs Fc+/0, Re(bpy-C2/4/6-NPDI) all achieved comparable activity (TONco ∼ 25) and Faradaic efficiency (FEco ∼ 94%). Under identical CPE conditions, the standard catalyst Re(dmbpy) was inactive for electrocatalytic CO2 reduction; only at Eappl = −2.1 V vs Fc+/0 could Re(dmbpy) achieve the same catalytic performance, representing a 300 mV lowering in overpotential for Re(bpy-C2/4/6-NPDI). At higher overpotentials, Re(bpy-C4/6-NPDI) both outperformed Re(bpy-C2-NPDI), indicating the possibility of coinciding electrocatalytic CO2 reduction mechanisms that are dictated by tether-length and overpotential. Using UV-vis-nearIR spectroelectrochemistry (SEC), FTIR SEC, and chemical reduction experiments, it was shown that the NPDI-moiety served as an electron-reservoir for Re(bpy), thereby allowing catalytic activity at lower overpotentials. Density functional theory studies probing the optimized geometries and frontier molecular orbitals of various catalytic intermediates revealed that the geometric configuration of NPDI relative to the Re(bpy)-moiety plays a critical role in accessing electrons from the electron-reservoir. The improved performance of Re(bpy-C2/4/6-NPDI)dyads at lower overpotentials, relative to Re(dmbpy), highlights the utility of chromophore electron-reservoirs as a method for lowering the overpotential for CO2 conversion." @default.
• W3201958423 created "2021-10-11" @default.
• W3201958423 creator A5011826172 @default.
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• W3201958423 creator A5056847387 @default.
• W3201958423 creator A5060208186 @default.
• W3201958423 creator A5071985889 @default.
• W3201958423 creator A5079664532 @default.
• W3201958423 creator A5082332881 @default.
• W3201958423 date "2021-10-01" @default.
• W3201958423 modified "2023-09-25" @default.
• W3201958423 title "Lowering Electrocatalytic CO₂ Reduction Overpotential Using N-Annulated Perylene Diimide Rhenium Bipyridine Dyads with Variable Tether Length" @default.
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