Design, Synthesis, and SAR of C-3 Benzoic Acid, C-17 Triterpenoid Derivatives. Identification of the HIV-1 Maturation Inhibitor 4-((1 R,3a S,5a R,5b R,7a R,11a S,11b R,13a R,13b R)-3a-((2-(1,1-Dioxidothiomorpholino)ethyl)amino)-5a,5b,8,8,11a-pentamethyl-1-(prop-1-en-2-yl)-2,3,3a,4,5,5a,5b,6,7,7a,8,11,11a,11b,12,13,13a,13b-octadecahydro-1 H-cyclopenta[ a]chrysen-9-yl)benzoic Acid (GSK3532795, BMS-955176)

J Med Chem. 2018 Aug 23;61(16):7289-7313. doi: 10.1021/acs.jmedchem.8b00854. Epub 2018 Aug 1.

Abstract

GSK3532795, formerly known as BMS-955176 (1), is a potent, orally active, second-generation HIV-1 maturation inhibitor (MI) that advanced through phase IIb clinical trials. The careful design, selection, and evaluation of substituents appended to the C-3 and C-17 positions of the natural product betulinic acid (3) was critical in attaining a molecule with the desired virological and pharmacokinetic profile. Herein, we highlight the key insights made in the discovery program and detail the evolution of the structure-activity relationships (SARs) that led to the design of the specific C-17 amine moiety in 1. These modifications ultimately enabled the discovery of 1 as a second-generation MI that combines broad coverage of polymorphic viruses (EC50 <15 nM toward a panel of common polymorphisms representative of 96.5% HIV-1 subtype B virus) with a favorable pharmacokinetic profile in preclinical species.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • ATP Binding Cassette Transporter, Subfamily B, Member 1 / genetics
  • Administration, Oral
  • Animals
  • Anti-HIV Agents / chemistry*
  • Anti-HIV Agents / pharmacokinetics
  • Anti-HIV Agents / pharmacology*
  • Benzoic Acid / chemistry
  • Biological Availability
  • Chemistry Techniques, Synthetic
  • Chrysenes / chemistry*
  • Chrysenes / pharmacology
  • Dogs
  • Drug Design
  • Drug Stability
  • HIV-1 / drug effects
  • HIV-1 / genetics
  • Humans
  • Macaca fascicularis
  • Male
  • Mice, Inbred Strains
  • Mice, Knockout
  • Microsomes, Liver / drug effects
  • Morpholines / chemistry*
  • Morpholines / pharmacology
  • Polymorphism, Genetic
  • Rats, Sprague-Dawley
  • Structure-Activity Relationship*
  • Triterpenes / chemistry*
  • Triterpenes / pharmacology

Substances

  • ATP Binding Cassette Transporter, Subfamily B, Member 1
  • Anti-HIV Agents
  • Chrysenes
  • Morpholines
  • Triterpenes
  • BMS-955176
  • Benzoic Acid