Tight-binding inhibitors efficiently inactivate both reaction centers of monomeric Plasmodium falciparum glyoxalase 1

FEBS J. 2012 Jul;279(14):2568-78. doi: 10.1111/j.1742-4658.2012.08640.x. Epub 2012 Jun 18.

Abstract

Glucose consumption and therefore methylglyoxal production of human erythrocytes increase significantly upon infection with malaria parasites. The glyoxalase systems of the host-parasite unit cope with this metabolic challenge by catalyzing the removal of harmful methylglyoxal. Thus, glyoxalase 1 from the malaria parasite Plasmodium falciparum (PfGlo1) could be a promising drug target. However, the enzyme has two different active sites and their simultaneous inactivation is considered challenging. Here, we describe the inactivation of PfGlo1 by two glyoxalase-specific tight-binding inhibitors with nanomolar K(i)(app) values and noncompetitive inhibition patterns. The inhibitors do not discriminate between the high-affinity and the high-activity conformations of PfGlo1, but seem to stabilize or trigger a conformational change in analogy with the substrate. In summary, we have characterized the most potent inhibitors of PfGlo1 known to date.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Binding Sites
  • Catalytic Domain
  • Dose-Response Relationship, Drug
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / metabolism*
  • Enzyme Inhibitors / pharmacology
  • Erythrocytes / drug effects
  • Erythrocytes / metabolism
  • Erythrocytes / parasitology
  • Host-Parasite Interactions
  • Humans
  • Kinetics
  • Lactoylglutathione Lyase / antagonists & inhibitors
  • Lactoylglutathione Lyase / genetics
  • Lactoylglutathione Lyase / metabolism*
  • Models, Molecular
  • Molecular Structure
  • Plasmodium falciparum / enzymology*
  • Plasmodium falciparum / physiology
  • Protein Binding
  • Protein Conformation
  • Protozoan Proteins / antagonists & inhibitors
  • Protozoan Proteins / genetics
  • Protozoan Proteins / metabolism*
  • Pyruvaldehyde / metabolism
  • Recombinant Proteins / antagonists & inhibitors
  • Recombinant Proteins / chemistry
  • Recombinant Proteins / metabolism

Substances

  • Enzyme Inhibitors
  • Protozoan Proteins
  • Recombinant Proteins
  • Pyruvaldehyde
  • Lactoylglutathione Lyase