Synthesis and biological evaluation of 6-substituted-5-fluorouridine ProTides

Bioorg Med Chem. 2018 Feb 1;26(3):551-565. doi: 10.1016/j.bmc.2017.11.037. Epub 2017 Dec 2.

Abstract

A new family of thirteen phosphoramidate prodrugs (ProTides) of different 6-substituted-5-fluorouridine nucleoside analogues were synthesized and evaluated as potential anticancer agents. In addition, antiviral activity against Chikungunya (CHIKV) virus was evaluated using a cytopathic effect inhibition assay. Although a carboxypeptidase Y assay supported a putative mechanism of activation of ProTides built on 5-fluorouridine with such C6-modifications, the Hint docking studies revealed a compromised substrate-activity for the Hint phosphoramidase-type enzyme that is likely responsible for phosphoramidate bioactivation through P-N bond cleavage and free nucleoside 5'-monophosphate delivery. Our observations may support and explain to some extent the poor in vitro biological activity generally demonstrated by the series of 6-substituted-5-fluorouridine phosphoramidates (ProTides) and will be of guidance for the design of novel phosphoramidate prodrugs.

Keywords: Anticancer; Human Hint enzyme; Nucleoside analogue (NA); Orotidine-5′-monophosphate decarboxylase (ODCase); Phosphoramidate (ProTide) approach.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Antineoplastic Agents / chemical synthesis
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / toxicity
  • Antiviral Agents / chemical synthesis
  • Antiviral Agents / chemistry
  • Antiviral Agents / pharmacology
  • Binding Sites
  • Cell Line, Tumor
  • Cell Survival / drug effects
  • Chikungunya virus / physiology
  • Drug Screening Assays, Antitumor
  • Humans
  • Molecular Docking Simulation
  • Nerve Tissue Proteins / chemistry
  • Nerve Tissue Proteins / metabolism
  • Phosphoramides / chemical synthesis*
  • Phosphoramides / chemistry
  • Phosphoramides / pharmacology
  • Prodrugs / chemical synthesis*
  • Prodrugs / chemistry
  • Prodrugs / pharmacology
  • Protein Structure, Tertiary
  • Structure-Activity Relationship
  • Uridine / analogs & derivatives*
  • Uridine / chemical synthesis
  • Uridine / chemistry
  • Uridine / pharmacology
  • Virus Internalization / drug effects

Substances

  • Antineoplastic Agents
  • Antiviral Agents
  • HINT1 protein, human
  • Nerve Tissue Proteins
  • Phosphoramides
  • Prodrugs
  • 5-fluorouridine
  • Uridine