Intracellular metabolism of the nucleotide prodrug GS-9131, a potent anti-human immunodeficiency virus agent

Antimicrob Agents Chemother. 2008 Feb;52(2):648-54. doi: 10.1128/AAC.01209-07. Epub 2007 Dec 3.

Abstract

GS-9131 is a phosphonoamidate prodrug of the novel ribose-modified phosphonate nucleotide analog GS-9148 that demonstrates potent anti-human immunodeficiency virus type 1 (HIV-1) activity and an excellent resistance profile in vitro. Prodrug moieties were optimized for the efficient delivery of GS-9148 and its active diphosphate (DP) metabolite to lymphoid cells following oral administration. To understand the intracellular pharmacology of GS-9131, incubations were performed with various types of lymphoid cells in vitro. The intracellular accumulation and antiviral activity levels of GS-9148 were limited by its lack of cellular permeation, and GS-9131 increased the delivery of GS-9148-DP by 76- to 290-fold relative to that of GS-9148. GS-9131 activation was saturable at high extracellular concentrations, potentially due to a high-affinity promoiety cleavage step. Once inside the cells, GS-9148 was efficiently phosphorylated, forming similar amounts of anabolites in primary lymphoid cells. The levels of GS-9148-DP formed in peripheral blood mononuclear cells infected with HIV-1 were similar to that in uninfected PBMCs, and approximately equivalent intracellular concentrations of GS-9148-DP and tenofovir (TVF)-DP were required to inhibit viral replication by 90%. Once it was formed, GS-9148-DP was efficiently retained in activated CD4(+) cells, with a half-life of 19 h. In addition, GS-9131 showed a low potential for drug interactions with other adenine nucleoside/nucleotide reverse transcriptase inhibitors, based on the lack of competition for anabolism between suprapharmacologic concentrations of GS-9148 and TVF and the lack of activity of GS-9131 metabolites against purine nucleoside phosphorylase, an enzyme involved in the clearance of 2',3'-dideoxyinosine. Together, these observations elucidate the cellular pharmacology of GS-9131 and illustrate its efficient loading of lymphoid cells, resulting in a prolonged intracellular exposure to the active metabolite GS-9148-DP.

MeSH terms

  • Adenine / analogs & derivatives*
  • Adenine / chemistry
  • Adenine / metabolism
  • Anti-HIV Agents / metabolism*
  • Diphosphates / chemistry
  • Diphosphates / metabolism
  • Guanosine / analogs & derivatives
  • Guanosine / chemistry
  • Guanosine / metabolism
  • HIV Infections / virology
  • HIV-1 / drug effects*
  • Humans
  • Leukocytes, Mononuclear / metabolism*
  • Leukocytes, Mononuclear / virology
  • Lymphocyte Activation
  • Organophosphonates / chemistry
  • Organophosphonates / metabolism
  • Prodrugs / chemistry
  • Prodrugs / metabolism*
  • Reverse Transcriptase Inhibitors / chemistry
  • Reverse Transcriptase Inhibitors / metabolism
  • Tenofovir

Substances

  • Anti-HIV Agents
  • Diphosphates
  • GS-9131
  • Organophosphonates
  • Prodrugs
  • Reverse Transcriptase Inhibitors
  • Guanosine
  • Tenofovir
  • GS-9148
  • Adenine