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• W2005159076 abstract "Heme−Cu/O2 adducts are of interest in the elucidation of the fundamental metal−O2 chemistry occurring in heme−Cu enzymes which effect reductive O−O cleavage of dioxygen to water. In this report, the chemistry of four heme−peroxo−copper [FeIII−(O22-)−CuII]+ complexes (1−4), varying in their ligand architecture, copper-ligand denticity, or both and thus their structures and physical properties are compared in their reactivity toward CO, PPh3, acids, cobaltocene, and phenols. In 1 and 2, the copper(II) ligand is N4-tetradentate, and the peroxo unit is bound side-on to iron(III) and end-on to the copper(II). In contrast, 3 and 4 contain a N3-tridentate copper(II) ligand, and the peroxo unit is bound side-on to both metal ions. CO “displaces” the peroxo ligand from 2−4 to form reduced CO−FeII and CO−CuI species. PPh3 reacts with 3 and 4 displacing the peroxide ligand from copper, forming (porphyrinate)FeIII-superoxide plus CuI-PPh3 species. Complex 2 does not react with PPh3, and surprisingly, 1 reacts neither with PPh3 nor CO, exhibiting remarkable stability toward these reagents. The behavior of 1 and 2 compared to that of 3 and 4 correlates with the different denticity of the copper ligand (tetra vs tridentate). Complexes 1−4 react with HCl releasing H2O2, demonstrating the basic character of the peroxide ligand. Cobaltocene causes the two-electron reduction of 1−4 giving the corresponding μ-oxo [FeIII−(O2-)−CuII]+ complexes, in contrast to the findings for other heme-peroxo-copper species of different design. With t-butyl-substituted phenols, no reaction occurs with 1−4. The results described here emphasize how ligand design and variations influence and control not only the structure and physical properties but also the reactivity patterns for heme−Cu/O2 adducts. Implications for future investigations of protonated heme/Cu−peroxo complexes, low-spin analogues, and ultimately O−O cleavage chemistry are discussed." @default.
• W2005159076 created "2016-06-24" @default.
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• W2005159076 date "2007-07-06" @default.
• W2005159076 modified "2023-10-10" @default.
• W2005159076 title "Reactivity Studies on Fe^III−(O₂^2-)−Cu^II Compounds: Influence of the Ligand Architecture and Copper Ligand Denticity" @default.
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• W2005159076 doi "https://doi.org/10.1021/ic700363k" @default.
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