N-Substituted Quinolinonyl Diketo Acid Derivatives as HIV Integrase Strand Transfer Inhibitors and Their Activity against RNase H Function of Reverse Transcriptase

J Med Chem. 2015 Jun 11;58(11):4610-23. doi: 10.1021/acs.jmedchem.5b00159. Epub 2015 May 26.

Abstract

Bifunctional quinolinonyl DKA derivatives were first described as nonselective inhibitors of 3'-processing (3'-P) and strand transfer (ST) functions of HIV-1 integrase (IN), while 7-aminosubstituted quinolinonyl derivatives were proven IN strand transfer inhibitors (INSTIs) that also displayed activity against ribonuclease H (RNase H). In this study, we describe the design, synthesis, and biological evaluation of new quinolinonyl diketo acid (DKA) derivatives characterized by variously substituted alkylating groups on the nitrogen atom of the quinolinone ring. Removal of the second DKA branch of bifunctional DKAs, and the amino group in position 7 of quinolinone ring combined with a fine-tuning of the substituents on the benzyl group in position 1 of the quinolinone, increased selectivity for IN ST activity. In vitro, the most potent compound was 11j (IC50 = 10 nM), while the most active compounds against HIV infected cells were ester derivatives 10j and 10l. In general, the activity against RNase H was negligible, with only a few compounds active at concentrations higher than 10 μM. The binding mode of the most potent IN inhibitor 11j within the IN catalytic core domain (CCD) is described as well as its binding mode within the RNase H catalytic site to rationalize its selectivity.

Publication types

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

MeSH terms

  • Catalytic Domain
  • HIV Infections / drug therapy
  • HIV Infections / virology
  • HIV Integrase / chemistry*
  • HIV Integrase Inhibitors / chemistry
  • HIV Integrase Inhibitors / pharmacology*
  • HIV-1 / drug effects
  • HeLa Cells
  • Humans
  • Keto Acids / chemistry
  • Keto Acids / pharmacology*
  • Models, Molecular
  • Molecular Structure
  • Quinolones / chemistry
  • Quinolones / pharmacology*
  • RNA-Directed DNA Polymerase / chemistry*
  • Ribonuclease H / antagonists & inhibitors*
  • Structure-Activity Relationship
  • Virus Replication / drug effects

Substances

  • 4-(1-(2,4-difluorophenyl)methyl-4(1H)-quinolinon-3-yl)-2-hydroxy-4-oxo-2-butenoic acid
  • HIV Integrase Inhibitors
  • Keto Acids
  • Quinolones
  • HIV Integrase
  • RNA-Directed DNA Polymerase
  • Ribonuclease H
  • p31 integrase protein, Human immunodeficiency virus 1