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- W3167667070 abstract "Non-heme-iron (NH-Fe) enzymes activate O2 for an array of biomedically, agriculturally, and environmentally important oxidation reactions. Our past decade's work has characterized iron(IV)-oxo (ferryl) complexes in several such NH-Fe enzymes.1 In all such systems that transform aliphatic carbon centers, the ferryl complexes generate substrate radicals by abstracting hydrogen (H•),2–6 leading to formation of new C–O,2–4 C–Cl/Br,5,6 or C–S bonds.1 Motivated by our success in rationalizing the divergent outcomes of the NH-Fe- and 2- (oxo)glutarate-dependent aliphatic hydroxylases and halogenases,7 we now seek both to exploit the ferryl manifold for novel, unnatural carbon-functionalization reactions8 and to explain the structural and mechanistic bases for several other natural reaction types – including 1,3-dehydrogenation of an alcohol to epoxide,9 stereo-inversion of a chiral carbon,10 and desaturation and cleavage of C–C bonds – that are initiated by ferryl complexes in other NH-Fe enzymes. Insight obtained will inform development of new biocatalytic synthetic routes and combinatorial design of new antibiotic and anticancer drugs. Support or Funding InformationNational Institutes of Health GM118812, GM113106, and GM069657; National Science Foundation CHE-0724084 and MCB-0642058." @default.
- W3167667070 created "2021-06-22" @default.
- W3167667070 creator A5050467129 @default.
- W3167667070 creator A5076704150 @default.
- W3167667070 date "2017-04-01" @default.
- W3167667070 modified "2023-10-17" @default.
- W3167667070 title "Mechanistic pathways to unusual outcomes in reactions of iron‐dependent oxygenases" @default.
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- W3167667070 doi "https://doi.org/10.1096/fasebj.31.1_supplement.258.1" @default.
- W3167667070 hasPublicationYear "2017" @default.
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