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• W3200675527 startingPage "26072" @default.
• W3200675527 abstract "A bis(pyridyl)amine-bipyridine-iron(II) framework (Fe(BPAbipy)) of complexes 1–3 is reported to shed light on the multistep nature of CO2 reduction. Herein, photocatalytic conversion of CO2 to CO even at low CO2 concentration (1 %), together with detailed mechanistic study and DFT calculations, reveal that 1 first undergoes two sequential one-electron transfer affording an intermediate with electron density on both Fe and ligand for CO2 binding over proton. The following 2 H+-assisted Fe-CO formation is rate-determining for selective CO2-to-CO reduction. A pendant, proton-shuttling α-OH group (2) initiates PCET for predominant H2 evolution, while an α-OMe group (3) cancels the selectivity control for either CO or H2. The near-unity selectivity of 1 and 2 enables self-sorting syngas production at flexible CO/H2 ratios. The unprecedented results from one kind of molecular catalyst skeleton encourage insight into the beauty of advanced multi-electron and multi-proton transfer processes for robust CO2RR by photocatalysis." @default.
• W3200675527 created "2021-09-27" @default.
• W3200675527 creator A5001548891 @default.
• W3200675527 creator A5004129270 @default.
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• W3200675527 creator A5033833264 @default.
• W3200675527 creator A5052474997 @default.
• W3200675527 creator A5064078598 @default.
• W3200675527 creator A5071014155 @default.
• W3200675527 date "2021-11-09" @default.
• W3200675527 modified "2023-10-14" @default.
• W3200675527 title "Mechanistic Insights Into Iron(II) Bis(pyridyl)amine‐Bipyridine Skeleton for Selective CO ₂ Photoreduction" @default.
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