Selectivity for strand-transfer over 3'-processing and susceptibility to clinical resistance of HIV-1 integrase inhibitors are driven by key enzyme-DNA interactions in the active site

Nucleic Acids Res. 2016 Aug 19;44(14):6896-906. doi: 10.1093/nar/gkw592. Epub 2016 Jul 1.

Abstract

Integrase strand transfer inhibitors (INSTIs) are highly effective against HIV infections. Co-crystal structures of the prototype foamy virus intasome have shown that all three FDA-approved drugs, raltegravir (RAL), elvitegravir and dolutegravir (DTG), act as interfacial inhibitors during the strand transfer (ST) integration step. However, these structures give only a partial sense for the limited inhibition of the 3'-processing reaction by INSTIs and how INSTIs can be modified to overcome drug resistance, notably against the G140S-Q148H double mutation. Based on biochemical experiments with modified oligonucleotides, we demonstrate that both the viral DNA +1 and -1 bases, which flank the 3'-processing site, play a critical role for 3'-processing efficiency and inhibition by RAL and DTG. In addition, the G140S-Q148H (SH) mutant integrase, which has a reduced 3'-processing activity, becomes more active and more resistant to inhibition of 3'-processing by RAL and DTG in the absence of the -1 and +1 bases. Molecular modeling of HIV-1 integrase, together with biochemical data, indicate that the conserved residue Q146 in the flexible loop of HIV-1 integrase is critical for productive viral DNA binding through specific contacts with the virus DNA ends in the 3'-processing and ST reactions. The potency of integrase inhibitors against 3'-processing and their ability to overcome resistance is discussed.

MeSH terms

  • Biocatalysis / drug effects
  • Catalytic Domain*
  • DNA, Viral / metabolism*
  • Drug Resistance, Viral / drug effects*
  • Guanine / metabolism
  • HIV Integrase / chemistry
  • HIV Integrase / metabolism*
  • HIV Integrase Inhibitors / chemistry
  • HIV Integrase Inhibitors / pharmacology*
  • Ions
  • Magnesium / pharmacology
  • Models, Molecular
  • Mutation / genetics
  • Substrate Specificity / drug effects

Substances

  • DNA, Viral
  • HIV Integrase Inhibitors
  • Ions
  • Guanine
  • HIV Integrase
  • Magnesium
  • p31 integrase protein, Human immunodeficiency virus 1