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• W2079032566 abstract "The chemical interplay of nitrogen oxides (NO's) with hemoglobin (Hb) has attracted considerable recent attention because of its potential significance in the mechanism of NO-related vasoactivity regulated by Hb. An important theme of this interplay—redox coupling in adducts of heme iron and NO's—has sparked renewed interest in fundamental studies of FeNOx coordination complexes. In this Article, we report combined UV−vis and comprehensive electron paramagnetic resonance (EPR) spectroscopic studies that address intriguing questions raised in recent studies of the structure and affinity of the nitrite ligand in complexes with FeIII in methemoglobin (metHb). EPR spectra of metHb/NO2− are found to exhibit a characteristic doubling in their sharper spectral features. Comparative EPR measurements at X- and S-band frequencies, and in D2O versus H2O, argue against the assignment of this splitting as hyperfine structure. Correlated changes in the EPR spectra with pH enable complete assignment of the spectrum as deriving from the overlap of two low-spin species with g values of 3.018, 2.122, 1.45 and 2.870, 2.304, 1.45 (values for samples at 20 K and pH 7.4 in phosphate-buffered saline). These g values are typical of g values found for other heme proteins with N-coordinated ligands in the binding pocket and are thus suggestive of N-nitro versus O-nitrito coordination. The positions and shapes of the spectral lines vary only slightly with temperature until motional averaging ensues at ∼150 K. The pattern of motional averaging in the variable-temperature EPR spectra and EPR studies of FeIIINO2−/FeIINO hybrids suggest that one of two species is present in both of the α and β subunits, while the other is exclusive to the β subunit. Our results also reconfirm that the affinity of nitrite for metHb is of millimolar magnitude, thereby making a direct role for nitrite in physiological hypoxic vasodilation difficult to justify." @default.
• W2079032566 created "2016-06-24" @default.
• W2079032566 creator A5017461914 @default.
• W2079032566 creator A5048720198 @default.
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• W2079032566 date "2010-07-12" @default.
• W2079032566 modified "2023-10-11" @default.
• W2079032566 title "EPR Spectroscopy of Nitrite Complexes of Methemoglobin" @default.
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• W2079032566 doi "https://doi.org/10.1021/ic902085s" @default.
• W2079032566 hasPubMedCentralId "https://www.ncbi.nlm.nih.gov/pmc/articles/4498954" @default.
• W2079032566 hasPubMedId "https://pubmed.ncbi.nlm.nih.gov/20666390" @default.
• W2079032566 hasPublicationYear "2010" @default.
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