Computationally-guided optimization of a docking hit to yield catechol diethers as potent anti-HIV agents

J Med Chem. 2011 Dec 22;54(24):8582-91. doi: 10.1021/jm201134m. Epub 2011 Nov 29.

Abstract

A 5-μM docking hit has been optimized to an extraordinarily potent (55 pM) non-nucleoside inhibitor of HIV reverse transcriptase. Use of free energy perturbation (FEP) calculations to predict relative free energies of binding aided the optimizations by identifying optimal substitution patterns for phenyl rings and a linker. The most potent resultant catechol diethers feature terminal uracil and cyanovinylphenyl groups. A halogen bond with Pro95 likely contributes to the extreme potency of compound 42. In addition, several examples are provided illustrating failures of attempted grafting of a substructure from a very active compound onto a seemingly related scaffold to improve its activity.

Publication types

  • Research Support, N.I.H., Extramural

MeSH terms

  • Anti-HIV Agents / chemical synthesis
  • Anti-HIV Agents / chemistry*
  • Anti-HIV Agents / pharmacology
  • Catechols / chemical synthesis
  • Catechols / chemistry*
  • Catechols / pharmacology
  • Computer Simulation*
  • Ethers / chemical synthesis
  • Ethers / chemistry
  • Ethers / pharmacology
  • HIV Reverse Transcriptase / chemistry
  • HIV Reverse Transcriptase / metabolism
  • HIV-1 / drug effects
  • HIV-1 / enzymology
  • Humans
  • Models, Molecular*
  • Molecular Structure
  • Protein Binding
  • Quantitative Structure-Activity Relationship
  • Reverse Transcriptase Inhibitors / chemical synthesis
  • Reverse Transcriptase Inhibitors / chemistry
  • Reverse Transcriptase Inhibitors / pharmacology
  • Stereoisomerism
  • T-Lymphocytes / drug effects
  • T-Lymphocytes / virology

Substances

  • Anti-HIV Agents
  • Catechols
  • Ethers
  • Reverse Transcriptase Inhibitors
  • HIV Reverse Transcriptase