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• W2004441489 abstract "Cuprous and cupric complexes with the new imidazolyl containing tripodal tetradentate ligands {LMIm, (1H-imidazol-4-yl)-N,N-bis((pyridin-2-yl)methyl)methanamine, and LEIm, 2-(1H-imidazol-4-yl)-N,N-bis((pyridin-2-yl)methyl)ethanamine}, have been investigated to probe differences in their chemistry, especially in copper(I)−dioxygen chemistry, compared to that already known for the pyridyl analogue TMPA, tris(2-pyridyl)methyl)amine. Infrared (IR) stretching frequencies obtained from carbon monoxide adducts of [(LMIm)CuI]+ (1a) and [(LEIm)CuI]+ (2a) show that the imidazolyl donor is stronger than its pyridyl analogue. Electrochemical data suggest differences in the binding constant of CuII to LEIm compared to TMPA and LMIm, reflecting geometric changes. Oxygenation of [(LMIm)CuI]+ (1a) in 2-methyltetrahydrofuran (MeTHF) solvent at −128 °C leads to an intensely purple colored species with a UV−vis spectrum characteristic of an end-on bound peroxodicopper(II) complex [{(LMIm)CuII}2(μ-1,2-O22−)]2+ (1bP) {λmax = 528 nm}, very similar to the previously well characterized complex [{(TMPA)CuII}2(μ-1,2-O22−)]2+ {λmax = 520 nm (ε = 12 000 M−1 cm−1), in MeTHF; resonance Raman (rR) spectroscopy: ν(O−O) = 832 (Δ(18O2) = −44) cm−1}. In the low-temperature oxygenation of 2a, benchtop (−128 °C) and stopped-flow (−90 °C) experiments reveal the formation of an initial superoxo-Cu(II) species [(LEIm)CuII(O2•−)]+ (2bS), λmax = 431 nm in THF) . This converts to the low-temperature stable peroxo complex [{(LEIm)CuII}2(μ-1,2-O22−)]2+ (2bP) {rR spectroscopy: ν(O−O) = 822 (Δ(18O2) = −46) cm−1}. Complex 2bP possess distinctly reduced Cu−O and O−O stretching frequencies and a red-shifted UV−vis feature {to λmax = 535 nm (ε = 11 000 M−1 cm−1)} compared to the TMPA analogue due to a distortion from trigonal bipyramidal (TBP) to a square pyramidal ligand field. This distortion is supported by the structural characterization of related ligand−copper(II) complexes: A stable tetramer cluster complex [(μ2-LEIm−)4(CuII)4]4+, obtained from thermal decomposition of 2bP (with formation of H2O2), also exhibits a distorted square pyramidal Cu(II) ion geometry as does the copper(II) complex [(LEIm)CuII(CH3CN)]2+ (2c), characterized by X-ray crystallography and solution electron paramagnetic resonance (EPR) spectroscopy." @default.
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• W2004441489 date "2009-11-03" @default.
• W2004441489 modified "2023-10-18" @default.
• W2004441489 title "Copper(I)/O₂ Chemistry with Imidazole Containing Tripodal Tetradentate Ligands Leading to μ-1,2-Peroxo−Dicopper(II) Species" @default.
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• W2004441489 doi "https://doi.org/10.1021/ic9017695" @default.
• W2004441489 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/2787896" @default.
• W2004441489 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/19886646" @default.
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