Oxygen isotope effects on electron transfer to O2 probed using chemically modified flavins bound to glucose oxidase

J Am Chem Soc. 2004 Nov 24;126(46):15120-31. doi: 10.1021/ja047050e.

Abstract

Apo-glucose oxidase has been reconstituted with flavins modified in the 7 and 8 positions and characterized with regard to the catalytic rate of O(2) reduction and oxygen-18 isotope effects on this process. Kinetic studies as a function of driving force indicate a reorganization energy for electron transfer to O(2) of lambda = 28 kcal mol(-)(1) at optimal pH, which is similar to the value obtained earlier from temperature dependencies of rates (Roth, J. P.; Klinman, J. P. Proc. Natl. Acad. Sci. U.S.A. 2003, 100, 62-67). For the various enzyme-bound flavins, competitive oxygen-18 kinetic isotope effects fall within the narrow range of 1.0266(5) to 1.0279(6), apparently because of the dominant contribution of outer-sphere reorganization to the activation barrier; within the context of semiclassical and quantum mechanical electron transfer theories, the magnitude of the isotope effects reveals the importance of nuclear tunneling.

Publication types

  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Aspergillus niger / enzymology
  • Flavin-Adenine Dinucleotide / analogs & derivatives
  • Flavin-Adenine Dinucleotide / chemistry
  • Flavin-Adenine Dinucleotide / metabolism
  • Flavins / chemistry*
  • Flavins / metabolism
  • Glucose Oxidase / chemistry*
  • Glucose Oxidase / metabolism
  • Kinetics
  • Oxidation-Reduction
  • Oxygen / chemistry*
  • Oxygen / metabolism
  • Oxygen Isotopes
  • Quantum Theory
  • Thermodynamics

Substances

  • Flavins
  • Oxygen Isotopes
  • Flavin-Adenine Dinucleotide
  • Glucose Oxidase
  • Oxygen