Bifunctional inhibition of human immunodeficiency virus type 1 reverse transcriptase: mechanism and proof-of-concept as a novel therapeutic design strategy

J Med Chem. 2013 May 23;56(10):3959-68. doi: 10.1021/jm400160s. Epub 2013 May 9.

Abstract

Human immunodeficiency virus type 1 reverse transcriptase (HIV-1 RT) is a major target for currently approved anti-HIV drugs. These drugs are divided into two classes: nucleoside and non-nucleoside reverse transcriptase inhibitors (NRTIs and NNRTIs). This study illustrates the synthesis and biochemical evaluation of a novel bifunctional RT inhibitor utilizing d4T (NRTI) and a TMC-derivative (a diarylpyrimidine NNRTI) linked via a poly(ethylene glycol) (PEG) linker. HIV-1 RT successfully incorporates the triphosphate of d4T-4PEG-TMC bifunctional inhibitor in a base-specific manner. Moreover, this inhibitor demonstrates low nanomolar potency that has 4.3-fold and 4300-fold enhancement of polymerization inhibition in vitro relative to the parent TMC-derivative and d4T, respectively. This study serves as a proof-of-concept for the development and optimization of bifunctional RT inhibitors as potent inhibitors of HIV-1 viral replication.

Publication types

  • Research Support, N.I.H., Extramural
  • Research Support, Non-U.S. Gov't

MeSH terms

  • Anti-HIV Agents / chemical synthesis*
  • Anti-HIV Agents / pharmacology*
  • DNA Primers
  • Dinucleoside Phosphates / chemistry
  • Dinucleoside Phosphates / isolation & purification
  • Drug Design
  • HIV Reverse Transcriptase / chemistry
  • HIV Reverse Transcriptase / isolation & purification
  • HIV Reverse Transcriptase / metabolism
  • HIV-1 / drug effects
  • Humans
  • Indicators and Reagents
  • Mass Spectrometry
  • Models, Molecular
  • Oligonucleotides / chemistry
  • Oligonucleotides / isolation & purification
  • Polyethylene Glycols / pharmacology
  • Reverse Transcriptase Inhibitors / chemical synthesis*
  • Reverse Transcriptase Inhibitors / pharmacology*
  • Structure-Activity Relationship
  • Virus Replication / drug effects
  • X-Ray Diffraction

Substances

  • Anti-HIV Agents
  • DNA Primers
  • Dinucleoside Phosphates
  • Indicators and Reagents
  • Oligonucleotides
  • Reverse Transcriptase Inhibitors
  • Polyethylene Glycols
  • HIV Reverse Transcriptase