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• W2897324430 endingPage "14160" @default.
• W2897324430 startingPage "14150" @default.
• W2897324430 abstract "The iron(III) complex [Fe(tpena)]2+ (tpena = N,N,N′-tris(2-pyridylmethyl)ethylendiamine-N′-acetate) undergoes irreversible O2-dependent N-demethylcarboxylation to afford [FeII(SBPy3)(MeCN)]2+ (SBPy3 = N,N-bis(2-pyridylmethyl)amine-N-ethyl-2-pyridine-2-aldimine), when irradiated with near-UV light. The loss of a mass equivalent to the glycyl group in a process involving consecutive C–C and C–N cleavages is documented by the measurement of the sequential production of CO2 and formaldehyde, respectively. Time-resolved UV–vis absorption, Mössbauer, EPR, and Raman spectroscopy have allowed the spectroscopic characterization of two iron-based intermediates along the pathway. The first of these, proposed to be a low-spin iron(II)-radical ligand complex, reacts with O2 in the rate-determining step to produce a putative alkylperoxide complex. DFT calculations suggest that this evolves into an Fe(IV)-oxo species, which can abstract a hydrogen atom from a cis methylene group of the ligand to give the second spectroscopically identified intermediate, a high-spin iron(III)-hydroxide of the product oxidized ligand, [FeIII(OH)(SBPy3)]2+. Reduction and exchange of the cohydroxo/water ligand produces the crystallographically characterized products [FeII(SBPy3)(X)]2+/3+, X = MeCN, [Zn(tpena)]+." @default.
• W2897324430 created "2018-10-26" @default.
• W2897324430 creator A5002648736 @default.
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• W2897324430 date "2018-10-22" @default.
• W2897324430 modified "2023-10-17" @default.
• W2897324430 title "Photoinduced O₂-Dependent Stepwise Oxidative Deglycination of a Nonheme Iron(III) Complex" @default.
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• W2897324430 doi "https://doi.org/10.1021/jacs.8b07455" @default.
• W2897324430 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/30347152" @default.
• W2897324430 hasPublicationYear "2018" @default.
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