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• W3134422447 endingPage "3778" @default.
• W3134422447 startingPage "3764" @default.
• W3134422447 abstract "The electrocatalytic activity for CO2 reduction is greatly enhanced for Co complexes with pyridyldiimine-based ligands through the stepwise integration of three synergistic substituent effects: extended conjugation, electron-withdrawing ability, and intramolecular electrostatic effects. The stepwise incorporation of these effects into the catalyst structures results in a series of complexes that show an atypical inverse scaling relationship for CO2 reduction-the maximum activity of the resulting catalysts increases as the onset potentials are driven positive due to the ligand electronic substituent effects. Incorporating all three effects simultaneously into the catalyst structure results in a Co complex [Co(PDI-PyCH3+I-)] with dramatically enhanced activity for CO2 reduction, operating with over an order of magnitude higher activity (TOFcat = 4.1 × 104 s-1) and ∼0.2 V more positive catalytic onset (Eonset = -1.52 V vs Fc+/0) compared to the parent complex, an intrinsic activity parameter TOF0 = 6.3 × 10-3 s-1, and >95% Faradaic efficiency for CO production in acetonitrile with 11 M water. This makes [Co(PDI-PyCH3+I-)] among the most active molecular catalysts reported for the CO2 reduction reaction. Our work highlights a promising catalyst design strategy for molecular CO2RR catalysts in which catalytic ability is enhanced by tuning three synergistic substituent effects simultaneously in a single catalyst structure." @default.
• W3134422447 created "2021-03-15" @default.
• W3134422447 creator A5010115051 @default.
• W3134422447 creator A5049208393 @default.
• W3134422447 creator A5050798251 @default.
• W3134422447 date "2021-03-08" @default.
• W3134422447 modified "2023-10-01" @default.
• W3134422447 title "Enhancing a Molecular Electrocatalyst’s Activity for CO₂Reduction by Simultaneously Modulating Three Substituent Effects" @default.
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• W3134422447 doi "https://doi.org/10.1021/jacs.0c09357" @default.
• W3134422447 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/33683865" @default.
• W3134422447 hasPublicationYear "2021" @default.
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