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• W2077506046 endingPage "13331" @default.
• W2077506046 startingPage "13325" @default.
• W2077506046 abstract "Dioxygen addition to coordinatively unsaturated [Fe(II)(O(Me2)N4(6-Me-DPEN))](PF6) (1) is shown to afford a complex containing a dihydroxo-bridged Fe(III)2(μ-OH)2 diamond core, [Fe(III)(O(Me2)N4(6-Me-DPEN))]2(μ-OH)2(PF6)2·(CH3CH2CN)2 (2). The diamond core of 2 resembles the oxidized methane monooxygenase (MMOox) resting state, as well as the active site product formed following H-atom abstraction from Tyr-OH by ribonucleotide reductase (RNR). The Fe-OH bond lengths of 2 are comparable with those of the MMOHox suggesting that MMOHox contains a Fe(III)2(μ-OH)2 as opposed to Fe(III)2(μ-OH)(μ-OH2) diamond core as had been suggested. Isotopic labeling experiments with (18)O2 and CD3CN indicate that the oxygen and proton of the μ-OH bridges of 2 are derived from dioxygen and acetonitrile. Deuterium incorporation (from CD3CN) suggests that an unobserved intermediate capable of abstracting a H-atom from CH3CN forms en route to 2. Given the high C-H bond dissociation energy (BDE = 97 kcal/mol) of acetonitrile, this indicates that this intermediate is a potent oxidant, possibly a high-valent iron oxo. Consistent with this, iodosylbenzene (PhIO) also reacts with 1 in CD3CN to afford the deuterated Fe(III)2(μ-OD)2 derivative of 2. Intermediates are not spectroscopically observed in either reaction (O2 and PhIO) even at low-temperatures (-80 °C), indicating that this intermediate has a very short lifetime, likely due to its highly reactive nature. Hydroxo-bridged 2 was found to stoichiometrically abstract hydrogen atoms from 9,10-dihydroanthracene (C-H BDE = 76 kcal/mol) at ambient temperatures." @default.
• W2077506046 created "2016-06-24" @default.
• W2077506046 creator A5020214026 @default.
• W2077506046 creator A5058835657 @default.
• W2077506046 creator A5066321625 @default.
• W2077506046 date "2013-11-14" @default.
• W2077506046 modified "2023-09-25" @default.
• W2077506046 title "Isolation and Characterization of a Dihydroxo-Bridged Iron(III,III)(μ-OH)₂ Diamond Core Derived from Dioxygen" @default.
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• W2077506046 doi "https://doi.org/10.1021/ic4010906" @default.
• W2077506046 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/3885352" @default.
• W2077506046 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/24229319" @default.
• W2077506046 hasPublicationYear "2013" @default.
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