C1'-Branched acyclic nucleoside phosphonates mimicking adenosine monophosphate: Potent inhibitors of Trypanosoma brucei adenine phosphoribosyltransferase

Eur J Med Chem. 2021 Dec 5:225:113798. doi: 10.1016/j.ejmech.2021.113798. Epub 2021 Aug 25.

Abstract

Some pathogens, including parasites of the genus Trypanosoma causing Human and Animal African Trypanosomiases, cannot synthesize purines de novo and they entirely rely on the purine salvage pathway (PSP) for their nucleotide generation. Thus, their PSP enzymes are considered as promising drug targets, sparsely explored so far. Recently, a significant role of acyclic nucleoside phosphonates (ANPs) as inhibitors of key enzymes of PSP, namely of 6-oxopurine phosphoribosyltransferases (PRTs), has been discovered. Herein, we designed and synthesized two series of new ANPs branched at the C1' position as mimics of adenosine monophosphate. The novel ANPs efficaciously inhibited Trypanosoma brucei adenine PRT (TbrAPRT1) activity in vitro and it was shown that the configuration on the C1' chiral centre strongly influenced their activity: the (R)-enantiomers proved to be more potent compared to the (S)-enantiomers. Two ANPs, with Ki values of 0.39 μM and 0.57 μM, represent the most potent TbrAPRT1 inhibitors reported to date and they are an important tool to further study purine metabolism in various parasites.

Keywords: APRT; Enzyme inhibitors; Nucleotide analogues; Phosphonates; Purine salvage pathway; Trypanosomiasis.

MeSH terms

  • Adenine Phosphoribosyltransferase / antagonists & inhibitors*
  • Adenine Phosphoribosyltransferase / metabolism
  • Adenosine Monophosphate / chemical synthesis
  • Adenosine Monophosphate / chemistry
  • Adenosine Monophosphate / pharmacology*
  • Antiprotozoal Agents / chemical synthesis
  • Antiprotozoal Agents / chemistry
  • Antiprotozoal Agents / pharmacology*
  • Dose-Response Relationship, Drug
  • Enzyme Inhibitors / chemical synthesis
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / pharmacology*
  • Molecular Structure
  • Nucleosides / chemical synthesis
  • Nucleosides / chemistry
  • Nucleosides / pharmacology*
  • Parasitic Sensitivity Tests
  • Structure-Activity Relationship
  • Trypanosoma brucei brucei / drug effects*
  • Trypanosoma brucei brucei / enzymology

Substances

  • Antiprotozoal Agents
  • Enzyme Inhibitors
  • Nucleosides
  • Adenosine Monophosphate
  • Adenine Phosphoribosyltransferase