Effect of distal cavity mutations on the formation of compound I in catalase-peroxidases

J Biol Chem. 2000 Jul 28;275(30):22854-61. doi: 10.1074/jbc.M002371200.

Abstract

Catalase-peroxidases have a predominant catalase activity but differ from monofunctional catalases in exhibiting a substantial peroxidase activity and in having different residues in the heme cavity. We present a kinetic study of the formation of the key intermediate compound I by probing the role of the conserved distal amino acid triad Arg-Trp-His of a recombinant catalase-peroxidase in its reaction with hydrogen peroxide, peroxoacetic acid, and m-chloroperbenzoic acid. Both the wild-type enzyme and six mutants (R119A, R119N, W122F, W122A, H123Q, H123E) have been investigated by steady-state and stopped-flow spectroscopy. The turnover number of catalase activity of R119A is 14.6%, R119N 0.5%, H123E 0.03%, and H123Q 0.02% of wild-type activity. Interestingly, W122F and W122A completely lost their catalase activity but retained their peroxidase activity. Bimolecular rate constants of compound I formation of the wild-type enzyme and the mutants have been determined. The Trp-122 mutants for the first time made it possible to follow the transition of the ferric enzyme to compound I by hydrogen peroxide spectroscopically underlining the important role of Trp-122 in catalase activity. The results demonstrate that the role of the distal His-Arg pair in catalase-peroxidases is important in the heterolytic cleavage of hydrogen peroxide (i.e. compound I formation), whereas the distal tryptophan is essential for compound I reduction by hydrogen peroxide.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Catalase / metabolism*
  • Circular Dichroism
  • Mutagenesis, Site-Directed
  • Peroxidase / metabolism*
  • Recombinant Proteins / metabolism
  • Spectrophotometry, Ultraviolet

Substances

  • Recombinant Proteins
  • Catalase
  • Peroxidase