Rate of Intramolecular Reduction of Oxyferryl Iron in Horse Heart Myoglobin

Craig Fenwick, Stephen Marmor, K. Govindaraju, Ann M. English, James F. Wishart and Ji Sun

J. Am. Chem. Soc. 116, 3169-3170 (1994)

Abstract:

The observed rate constant (kobs), as determined by pulse radiolysis, for intramolecular electron transfer (ET) from a5RuII bound at His48 to the ferric heme of horse heart myoglobin was 0.059 ± 0.003 s-1 at 25 °C, pH 7.0. This value is essentially identical to that previously reported in the literature for sperm whale myoglobin. Following oxidation by H2O2 of the ferric heme to oxyferryl heme (FeIV=O), kobs for intramolecular ET from a5RuII(His48) to heme increased to 0.19 ± 0.02 s-1 at a driving force of 0.96 eV. However, at the same driving force, a rate constant of 105 s-1 has been reported for intramolecular ET to the Zn porphyrin cation in the a5Ru(His48) derivative of Zn-substituted myoglobin. The ~106-fold slower rate of reduction of the FeIV=O heme compared to the Zn porphyrin cation suggests different rate-determing steps for intramolecular ET in the two myoglobin derivatives.