A manganese(IV)/iron(III) cofactor in Chlamydia trachomatis ribonucleotide reductase

Science. 2007 May 25;316(5828):1188-91. doi: 10.1126/science.1141179.

Abstract

In a conventional class I ribonucleotide reductase (RNR), a diiron(II/II) cofactor in the R2 subunit reacts with oxygen to produce a diiron(III/IV) intermediate, which generates a stable tyrosyl radical (Y*). The Y* reversibly oxidizes a cysteine residue in the R1 subunit to a cysteinyl radical (C*), which abstracts the 3'-hydrogen of the substrate to initiate its reduction. The RNR from Chlamydia trachomatis lacks the Y*, and it had been proposed that the diiron(III/IV) complex in R2 directly generates the C* in R1. By enzyme activity measurements and spectroscopic methods, we show that this RNR actually uses a previously unknown stable manganese(IV)/iron(III) cofactor for radical initiation.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Chlamydia trachomatis / enzymology*
  • Coenzymes / metabolism*
  • Electron Spin Resonance Spectroscopy
  • Enzyme Activation
  • Ferric Compounds / metabolism
  • Iron / metabolism*
  • Manganese / metabolism*
  • Ribonucleotide Reductases / metabolism*
  • Tyrosine / metabolism

Substances

  • Coenzymes
  • Ferric Compounds
  • Tyrosine
  • Manganese
  • Iron
  • Ribonucleotide Reductases