A Stable Ferryl Porphyrin at the Active Site of Y463M BthA

J Am Chem Soc. 2020 Jul 15;142(28):11978-11982. doi: 10.1021/jacs.0c04023. Epub 2020 Jul 1.

Abstract

BthA is a diheme enzyme that is a member of the bacterial cytochrome c peroxidase superfamily, capable of generating a highly unusual Fe(IV)Fe(IV)═O oxidation state, known to be responsible for long-range oxidative chemistry in the enzyme MauG. Here, we show that installing a canonical Met ligand in lieu of the Tyr found at the heme of MauG associated with electron transfer, results in a construct that yields an unusually stable Fe(IV)═O porphyrin at the peroxidatic heme. This state is spontaneously formed at ambient conditions using either molecular O2 or H2O2. The resulting data illustrate how a ferryl iron, with unforeseen stability, may be achieved in biology.

Publication types

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

MeSH terms

  • Bacterial Proteins / chemistry
  • Bacterial Proteins / genetics
  • Bacterial Proteins / metabolism*
  • Binding Sites
  • Cytochrome-c Peroxidase / chemistry
  • Cytochrome-c Peroxidase / genetics
  • Cytochrome-c Peroxidase / metabolism*
  • Iron / chemistry
  • Iron / metabolism*
  • Models, Molecular
  • Mutation
  • Porphyrins / chemistry
  • Porphyrins / metabolism*

Substances

  • Bacterial Proteins
  • Porphyrins
  • ferryl iron
  • Iron
  • Cytochrome-c Peroxidase