A widely distributed diheme enzyme from Burkholderia that displays an atypically stable bis-Fe(IV) state

Nat Commun. 2019 Mar 7;10(1):1101. doi: 10.1038/s41467-019-09020-4.

Abstract

Bacterial diheme peroxidases represent a diverse enzyme family with functions that range from hydrogen peroxide (H2O2) reduction to post-translational modifications. By implementing a sequence similarity network (SSN) of the bCCP_MauG superfamily, we present the discovery of a unique diheme peroxidase BthA conserved in all Burkholderia. Using a combination of magnetic resonance, near-IR and Mössbauer spectroscopies and electrochemical methods, we report that BthA is capable of generating a bis-Fe(IV) species previously thought to be a unique feature of the diheme enzyme MauG. However, BthA is not MauG-like in that it catalytically converts H2O2 to water, and a 1.54-Å resolution crystal structure reveals striking differences between BthA and other superfamily members, including the essential residues for both bis-Fe(IV) formation and H2O2 turnover. Taken together, we find that BthA represents a previously undiscovered class of diheme enzymes, one that stabilizes a bis-Fe(IV) state and catalyzes H2O2 turnover in a mechanistically distinct manner.

Publication types

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

MeSH terms

  • Bacterial Proteins / chemistry
  • Bacterial Proteins / genetics
  • Bacterial Proteins / metabolism*
  • Burkholderia / enzymology*
  • Burkholderia / genetics
  • Catalytic Domain
  • Crystallography, X-Ray
  • Enzyme Stability
  • Hemeproteins / chemistry
  • Hemeproteins / genetics
  • Hemeproteins / metabolism*
  • Iron / chemistry
  • Kinetics
  • Models, Molecular
  • Oxidation-Reduction
  • Peroxidases / chemistry
  • Peroxidases / genetics
  • Peroxidases / metabolism*
  • Protein Conformation

Substances

  • Bacterial Proteins
  • Hemeproteins
  • Iron
  • Peroxidases