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• W2791036277 abstract "Herein, we report the exploration of understanding the reactivity and structure of atomically dispersed M–N4 (M = Fe and Co) sites for the CO2 reduction reaction (CO2RR). Nitrogen coordinated Fe or Co site atomically dispersed into carbons (M–N–C) containing bulk- and edge-hosted M–N4 coordination were prepared by using Fe- or Co-doped metal–organic framework precursors, respectively, which were further studied as ideal model catalysts. Fe is intrinsically more active than Co in M–N4 for the reduction of CO2 to CO, in terms of a larger current density and a higher CO Faradaic efficiency (FE) (93% vs. 45%). First principle computations elucidated that the edge-hosted M–N2+2–C8 moieties bridging two adjacent armchair-like graphitic layers is the active sites for the CO2RR. They are much more active than previously proposed bulk-hosted M–N4–C10 moieties embedded compactly in a graphitic layer. During the CO2RR, when the dissociation of *COOH occurs on the M–N2+2–C8, the metal atom is the site for the adsorption of *CO and the carbon atom with a dangling bond next to an adjacent N is the other active center to bond *OH. In particular, on the Fe–N2+2–C8 sites, the CO2RR is more favorable over the hydrogen evolution reaction, thus resulting in a remarkable FE." @default.
• W2791036277 created "2018-03-29" @default.
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• W2791036277 date "2018-03-08" @default.
• W2791036277 modified "2023-10-14" @default.
• W2791036277 title "Unveiling Active Sites of CO₂ Reduction on Nitrogen-Coordinated and Atomically Dispersed Iron and Cobalt Catalysts" @default.
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• W2791036277 doi "https://doi.org/10.1021/acscatal.8b00398" @default.
• W2791036277 hasPublicationYear "2018" @default.
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