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- W4280520900 abstract "Although biological iron-sulfur (Fe-S) clusters perform some of the most difficult redox reactions in nature, they are thought to be composed exclusively of Fe2+ and Fe3+ ions, as well as mixed-valent pairs with average oxidation states of Fe2.5+. We herein show that Fe-S clusters formally composed of these valences can access a wider range of electronic configurations─in particular, those featuring low-valent Fe1+ centers. We demonstrate that CO binding to a synthetic [Fe4S4]0 cluster supported by N-heterocyclic carbene ligands induces the generation of Fe1+ centers via intracluster electron transfer, wherein a neighboring pair of Fe2+ sites reduces the CO-bound site to a low-valent Fe1+ state. Similarly, CO binding to an [Fe4S4]+ cluster induces electron delocalization with a neighboring Fe site to form a mixed-valent Fe1.5+Fe2.5+ pair in which the CO-bound site adopts partial low-valent character. These low-valent configurations engender remarkable C-O bond activation without having to traverse highly negative and physiologically inaccessible [Fe4S4]0/[Fe4S4]- redox couples." @default.
- W4280520900 created "2022-05-22" @default.
- W4280520900 creator A5031634252 @default.
- W4280520900 creator A5048476786 @default.
- W4280520900 creator A5080827187 @default.
- W4280520900 date "2022-05-16" @default.
- W4280520900 modified "2023-10-03" @default.
- W4280520900 title "Evidence for Low-Valent Electronic Configurations in Iron–Sulfur Clusters" @default.
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- W4280520900 doi "https://doi.org/10.1021/jacs.2c01872" @default.
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