Discovery of a Distinct Chemical and Mechanistic Class of Allosteric HIV-1 Integrase Inhibitors with Antiretroviral Activity

ACS Chem Biol. 2017 Nov 17;12(11):2858-2865. doi: 10.1021/acschembio.7b00550. Epub 2017 Oct 19.

Abstract

Allosteric integrase inhibitors (ALLINIs) bind to the lens epithelial-derived growth factor (LEDGF) pocket on HIV-1 integrase (IN) and possess potent antiviral effects. Rather than blocking proviral integration, ALLINIs trigger IN conformational changes that have catastrophic effects on viral maturation, rendering the virions assembled in the presence of ALLINIs noninfectious. A high-throughput screen for compounds that disrupt the IN·LEDGF interaction was executed, and extensive triage led to the identification of a t-butylsulfonamide series, as exemplified by 1. The chemical, biochemical, and virological characterization of this series revealed that 1 and its analogs produce an ALLINI-like phenotype through engagement of IN sites distinct from the LEDGF pocket. Key to demonstrating target engagement and differentiating this new series from the existing ALLINIs was the development of a fluorescence polarization probe of IN (FLIPPIN) based on the t-butylsulfonamide series. These findings further solidify the late antiviral mechanism of ALLINIs and point toward opportunities to develop structurally and mechanistically novel antiretroviral agents with unique resistance patterns.

MeSH terms

  • Allosteric Regulation / drug effects*
  • Cell Line
  • Drug Discovery
  • HIV Infections / drug therapy*
  • HIV Infections / metabolism
  • HIV Infections / virology
  • HIV Integrase / metabolism*
  • HIV Integrase Inhibitors / chemistry*
  • HIV Integrase Inhibitors / pharmacology*
  • HIV-1 / drug effects*
  • HIV-1 / metabolism
  • Humans
  • Intercellular Signaling Peptides and Proteins / metabolism
  • Protein Interaction Maps / drug effects
  • Sulfonamides / chemistry
  • Sulfonamides / pharmacology

Substances

  • HIV Integrase Inhibitors
  • Intercellular Signaling Peptides and Proteins
  • Sulfonamides
  • lens epithelium-derived growth factor
  • HIV Integrase
  • p31 integrase protein, Human immunodeficiency virus 1