Ionic strength and pH effect on the Fe(III)-imidazolate bond in the heme pocket of horseradish peroxidase: an EPR and UV-visible combined approach

J Inorg Biochem. 2000 Oct 1;81(4):259-66. doi: 10.1016/s0162-0134(00)00124-0.

Abstract

The effects of chloride, dihydrogenphosphate and ionic strength on the spectroscopic properties of horseradish peroxidase in aqueous solution at pH=3.0 were investigated. A red-shift (lambda=408 nm) of the Soret band was observed in the presence of 40 mM chloride; 500 mM dihydrogenphosphate or chloride brought about a blue shift of the same band (lambda=370 nm). The EPR spectrum of the native enzyme at pH 3.0 was characterized by the presence of two additional absorption bands in the region around g=6, with respect to pH 6.5. Chloride addition resulted in the loss of these features and in a lower rhombicity of the signal. A unique EPR band at g=6.0 was obtained as a result of the interaction between HRP and dihydrogenphosphate, both in the absence and presence of 40 mM Cl-. We suggest that a synergistic effect of low pH, Cl- and ionic strength is responsible for dramatic modifications of the enzyme conformation consistent with the Fe(II)-His170 bond cleavage. Dihydrogenphosphate as well as high chloride concentrations are shown to display an unspecific effect, related to ionic strength. A mechanistic explanation for the acid transition of HRP, previously observed by Smulevich et al. [Biochemistry 36 (1997) 640] and interpreted as a pure pH effect, is proposed.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Chlorides / chemistry
  • Chlorides / metabolism
  • Chlorides / pharmacology
  • Electron Spin Resonance Spectroscopy
  • Heme / metabolism*
  • Horseradish Peroxidase / chemistry*
  • Horseradish Peroxidase / drug effects
  • Horseradish Peroxidase / metabolism
  • Hydrogen-Ion Concentration
  • Imidazoles / chemistry*
  • Iron / chemistry*
  • Osmolar Concentration
  • Protein Conformation
  • Spectrophotometry, Ultraviolet

Substances

  • Chlorides
  • Imidazoles
  • Heme
  • imidazole
  • Iron
  • Horseradish Peroxidase