EPR stopped-flow studies of the reaction of the tyrosyl radical of protein R2 from ribonucleotide reductase with hydroxyurea

Biochem Biophys Res Commun. 1992 Oct 30;188(2):879-87. doi: 10.1016/0006-291x(92)91138-g.

Abstract

The reaction of the functional tyrosyl radical in protein R2 of ribonucleotide reductase from E. coli and mouse with the enzyme inhibitor hydroxyurea has been studied by EPR stopped-flow techniques at room temperature. The rate of disappearance of the tyrosyl radical in E. coli protein R2 is k2 = 0.43 M-1 s-1 at 25 degrees C. The reaction follows pseudo-first-order kinetics up to 450 mM hydroxyurea indicating that no saturation by hydroxyurea takes place even at this high concentration. Transient nitroxide-like radicals from hydroxyurea have been detected for the first time in the reaction of hydroxyurea with protein R2 from E. coli and mouse, indicating that 1-electron transfer from hydroxyurea to the tyrosyl radical is the dominating mechanism in the inhibitor reaction. The hydroxyurea radicals appear in low steady-state concentrations during 2-3 half-decay times of the tyrosyl radical and disappear thereafter.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Electron Spin Resonance Spectroscopy / methods
  • Escherichia coli / enzymology
  • Free Radicals
  • Hydroxyurea / metabolism*
  • Hydroxyurea / pharmacology
  • Kinetics
  • Macromolecular Substances
  • Mice
  • Oxidation-Reduction
  • Ribonucleotide Reductases / metabolism*

Substances

  • Free Radicals
  • Macromolecular Substances
  • Ribonucleotide Reductases
  • Hydroxyurea