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• W2068765668 abstract "Earlier we showed that the shapes of the EPR spectra of cobalt(II) porphyrinate(nitrogen base)(dioxygen) complexes in fluid solution were sensitive to the rate of rotation about the Co−O bond (Walker, F. A.; Bowen, J. H. J. Am. Chem. Soc. 1985, 107, 7632). We have now extended these studies to four metal-substituted hybrid hemoglobins in an attempt to determine whether EPR spectroscopy is sensitive to differences in the mobility of dioxygen in the α and β subunits of the T and R quaternary states. For purposes of this study, [α2(CoO2)β2(FeO2)] and [α2(FeO2)β2(CoO2)] were used as R-state models and [α2(CoO2)β2(Zn)] and [α2(Zn)β2(CoO2)] were used as T-state models. EPR spectra were recorded for samples of each of the above hybrids, equilibrated with 1 atm of O2 gas, as a function of temperature. The “progress toward averaging” of the EPR signals of the Co−O2-containing subunits was measured as the difference in field positions, ΔH, for the midpoint of the low- and high-field extrema of the derivative EPR spectra. A plot of ΔH vs temperature for each hybrid shows that the [α2(Zn)β2(CoO2)] hybrid is unique in averaging more slowly than the other three (all of which behave similarly), indicating more restricted rotation of dioxygen in T-state β-chain pockets than in the heme distal O2-binding pockets of any other form. This finding is consistent with X-ray crystallographic data which show that valine E11 on the distal side of the T-state β-chain pocket partially blocks the dioxygen binding site (Perutz, M. F.; Fermi, G.; Luisi, B.; Shaanan, B.; Liddington, R. C. Acc. Chem. Res. 1987, 20, 309). Simulation of EPR spectra as a function of jump time provides semiquantitative estimates of the rate of dioxygen rotation in these mixed-metal hemoglobin−dioxygen samples; these rates are in the 1 × 108 s-1 range for three of the hybrids at 35−37 °C, and about one-third that value for T-state β(CoO2) centers. These results provide new insight into the highly dynamic nature of dioxygen bound to the metal centers of hemoglobin at physiological temperatures." @default.
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• W2068765668 date "1997-10-01" @default.
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• W2068765668 title "EPR Studies of the Dynamics of Rotation of Dioxygen in Model Cobalt(II) Hemes and Cobalt-Containing Hybrid Hemoglobins" @default.
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• W2068765668 doi "https://doi.org/10.1021/jp9711306" @default.
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