Direct detection of oxygen intermediates in the non-heme Fe enzyme taurine/alpha-ketoglutarate dioxygenase

J Am Chem Soc. 2004 Feb 4;126(4):1022-3. doi: 10.1021/ja039113j.

Abstract

The reaction of substrate-bound taurine/alpha-ketoglutarate dioxygenase with O2 has been studied using cryogenic continuous-flow spectroscopy. Transient absorption spectra acquired at -38 degrees C show an exponential decay of a 318-nm chromophore with an apparent rate of 1.3 s-1. The observed optical changes and their kinetics are consistent with the profile of an Fe(IV) species detected recently by Mössbauer spectroscopy (Price et al., Biochemistry 2003, 42, 7497-7508). Resonance Raman measurement upon excitation at 363.7 nm reveal at least two oxygen isotope-sensitive vibrations at 821/787 cm-1 and 583/555 cm-1 for 16O and 18O derivatives, respectively. An additional mode is likely to be obscured by an ethylene glycol vibration at 865 cm-1 and/or 1089 cm-1. The 821 cm-1 vibration is assigned to the stretching mode of Fe(IV)=O species on the basis of its frequency and isotopic shift amplitude. The 583 cm-1 band is likely to originate from an Fe-O2 precursor of the Fe(IV)=O species, although its structural details are unclear at present.

Publication types

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

MeSH terms

  • Mixed Function Oxygenases / chemistry
  • Mixed Function Oxygenases / metabolism*
  • Nonheme Iron Proteins / chemistry
  • Nonheme Iron Proteins / metabolism*
  • Oxygen / chemistry
  • Oxygen / metabolism*
  • Oxygen Isotopes
  • Spectrophotometry, Ultraviolet
  • Spectrum Analysis, Raman

Substances

  • Nonheme Iron Proteins
  • Oxygen Isotopes
  • Mixed Function Oxygenases
  • taurine-alpha-ketoglutarate dioxygenase
  • Oxygen