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• W2982447624 endingPage "15432" @default.
• W2982447624 startingPage "15423" @default.
• W2982447624 abstract "The focus of this study is in the description of synthetic heme/copper/O2 chemistry employing a heme-containing binucleating ligand which provides a tridentate chelate for copper ion binding. The addition of O2 (−80 °C, tetrahydrofuran (THF) solvent) to the reduced heme compound (PImH)FeII (1), gives the oxy-heme adduct, formally a heme–superoxide complex FeIII–(O2•–) (2) (resonance Raman spectroscopy (rR): νO–O, 1171 cm–1 (Δ18O2, −61 cm–1); νFe–O, 575 cm–1 (Δ18O2, −24 cm–1)). Simple warming of 2 to room temperature regenerates reduced complex 1; this reaction is reversible, as followed by UV–vis spectroscopy. Complex 2 is electron paramagnetic resonance (EPR)-silent and exhibits upfield-shifted pyrrole resonances (δ 9.12 ppm) in 2H NMR spectroscopy, indicative of a six-coordinate low-spin heme. The coordination of the tethered imidazolyl arm to the heme–superoxide complex as an axial base ligand is suggested. We also report the new fully reduced heme–copper complex [(PImH)FeIICuI]+ (3), where the copper ion is bound to the tethered tridentate portion of PImH. This reacts with O2 to give a distinctive low-temperature-stable, high-spin (S = 2, overall) peroxo-bridged complex [(PImH)FeIII–(O22–)–CuII]+ (3a): λmax, 420 (Soret), 545, 565 nm; δpyrr, 93 ppm; νO–O, 799 cm–1 (Δ18O2, −48 cm–1); νFe–O, 524 cm–1 (Δ18O2, −23 cm–1). To 3a, the addition of dicyclohexylimidazole (DCHIm), which serves as a heme axial base, leads to low-spin (S = 0 overall) species complex [(DCHIm)(PImH)FeIII–(O22–)–CuII]+ (3b): λmax, 425 (Soret), 538 nm; δpyrr, 10.2 ppm; νO–O, 817 cm–1 (Δ18O2, −55 cm–1); νFe–O, 610 cm–1 (Δ18O2, −26 cm–1). These investigations into the characterization of the O2-adducts from (PImH)FeII (1) with/without additional copper chelation advance our understanding of the dioxygen reactivity of heme-only and heme/Cu-ligand heterobinuclear system, thus potentially relevant to O2 reduction in heme–copper oxidases or fuel-cell chemistry." @default.
• W2982447624 created "2019-11-08" @default.
• W2982447624 creator A5022958181 @default.
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• W2982447624 date "2019-10-28" @default.
• W2982447624 modified "2023-09-23" @default.
• W2982447624 title "Heme–Cu Binucleating Ligand Supports Heme/O₂ and Fe^II–Cu^I/O₂ Reactivity Providing High- and Low-Spin Fe^III–Peroxo–Cu^II Complexes" @default.
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• W2982447624 doi "https://doi.org/10.1021/acs.inorgchem.9b02521" @default.
• W2982447624 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/6916717" @default.
• W2982447624 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/31657921" @default.
• W2982447624 hasPublicationYear "2019" @default.
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