Design, synthesis, and evaluation of substrate - analogue inhibitors of Trypanosoma cruzi ribose 5-phosphate isomerase type B

Bioorg Med Chem Lett. 2021 Jan 15:32:127723. doi: 10.1016/j.bmcl.2020.127723. Epub 2020 Nov 26.

Abstract

Ribose 5-phosphate isomerase type B (RPI-B) is a key enzyme of the pentose phosphate pathway that catalyzes the isomerization of ribose 5-phosphate (R5P) and ribulose 5-phosphate (Ru5P). Trypanosoma cruzi RPI-B (TcRPI-B) appears to be a suitable drug-target mainly due to: (i) its essentiality (as previously shown in other trypanosomatids), (ii) it does not present a homologue in mammalian genomes sequenced thus far, and (iii) it participates in the production of NADPH and nucleotide/nucleic acid synthesis that are critical for parasite cell survival. In this survey, we report on the competitive inhibition of TcRPI-B by a substrate - analogue inhibitor, Compound B (Ki = 5.5 ± 0.1 μM), by the Dixon method. This compound has an iodoacetamide moiety that is susceptible to nucleophilic attack, particularly by the cysteine thiol group. Compound B was conceived to specifically target Cys-69, an important active site residue. By incubating TcRPI-B with Compound B, a trypsin digestion LC-MS/MS analysis revealed the identification of Compound B covalently bound to Cys-69. This inhibitor also exhibited notable in vitro trypanocidal activity against T. cruzi infective life-stages co-cultured in NIH-3T3 murine host cells (IC50 = 17.40 ± 1.055 μM). The study of Compound B served as a proof-of-concept so that next generation inhibitors can potentially be developed with a focus on using a prodrug group in replacement of the iodoacetamide moiety, thus representing an attractive starting point for the future treatment of Chagas' disease.

Keywords: Amastigote; Chagas’ disease; Competitive inhibition; Isomerase; Neglected tropical diseases; Substrate-analogue inhibitors; Trypanosoma cruzi; Trypomastigote; Trypsin digestion LC-MS/MS.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • 3T3 Cells
  • Aldose-Ketose Isomerases / antagonists & inhibitors*
  • Aldose-Ketose Isomerases / metabolism
  • Animals
  • Binding Sites
  • Catalytic Domain
  • Drug Design*
  • Enzyme Inhibitors / chemistry*
  • Enzyme Inhibitors / metabolism
  • Enzyme Inhibitors / pharmacology
  • Kinetics
  • Mice
  • Molecular Dynamics Simulation
  • Protozoan Proteins / antagonists & inhibitors*
  • Protozoan Proteins / metabolism
  • Substrate Specificity
  • Trypanocidal Agents / chemical synthesis*
  • Trypanocidal Agents / metabolism
  • Trypanocidal Agents / pharmacology
  • Trypanosoma cruzi / drug effects
  • Trypanosoma cruzi / enzymology*

Substances

  • Enzyme Inhibitors
  • Protozoan Proteins
  • Trypanocidal Agents
  • Aldose-Ketose Isomerases
  • ribosephosphate isomerase