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• W2803359626 abstract "Oxygenation of a tricopper(I) cyclophanate (1) affords reactive transients competent for C-H bond activation and O atom transfer to various substrates (including toluene, dihydroanthracene, and ethylmethylsulfide) based on 1H NMR, gas chromatography/mass spectrometry (MS), and electrospray ionization (ESI)/MS data. Low product yields (<1%) are determined for C-H activation substrates (e.g, toluene, ethylbenzene), which we attribute to competitive ligand oxidation. The combined stopped-flow UV/visible, electron paramagnetic resonance, ESI/MS, 1H NMR, and density functional theory (DFT) results for reaction of 1 with O2 are consistent with transient peroxo- and di(oxo)-bridged intermediates. DFT calculations elucidate a concerted proton-coupled electron transfer from toluene to the di(μ-oxo) intermediate and subsequent radical rebound as the C-H activation mechanism. Our results support a multicopper oxidase-like mechanism for O2 activation by 1, traversing species similar to the coplanar Cu3O2 unit in the peroxy and native intermediates." @default.
• W2803359626 created "2018-06-01" @default.
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• W2803359626 date "2018-05-23" @default.
• W2803359626 modified "2023-10-15" @default.
• W2803359626 title "A Tricopper(I) Complex Competent for O Atom Transfer, C–H Bond Activation, and Multiple O₂ Activation Steps" @default.
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• W2803359626 doi "https://doi.org/10.1021/acs.inorgchem.8b00921" @default.
• W2803359626 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/29791149" @default.
• W2803359626 hasPublicationYear "2018" @default.
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