Biotransformation of geldanamycin and 17-allylamino-17-demethoxygeldanamycin by human liver microsomes: reductive versus oxidative metabolism and implications

Drug Metab Dispos. 2007 Jan;35(1):21-9. doi: 10.1124/dmd.106.009639. Epub 2006 Sep 29.

Abstract

Comparative metabolite profiling of geldanamycin and 17-allylamino-17-demethoxygeldanamycin (17AAG) using human liver microsomes in normoxia and hypoxia was conducted to understand their differential metabolic fates. Geldanamycin bearing a 17-methoxy group primarily underwent reductive metabolism, generating the corresponding hydroquinone under both conditions. The formed hydroquinone resists further metabolism and serves as a reservoir. On exposure to oxygen, this hydroquinone slowly reverts to geldanamycin. In the presence of glutathione, geldanamycin was rapidly converted to 19-glutathionyl geldanamycin hydroquinone, suggesting its reactive nature. In contrast, the counterpart (17AAG) preferentially remained as its quinone form, which underwent extensive oxidative metabolism on both the 17-allylamino sidechain and the ansa ring. Only a small amount (<1%) of 19-glutathione conjugate of 17AAG was detected in the incubation of 17AAG with glutathione at 37 degrees C for 60 min. To confirm the differential nature of quinone-hydroquinone conversion between the two compounds, hypoxic incubations with human cytochrome P450 reductase at 37 degrees C and direct injection analysis were performed. Approximately 89% of hydroquinone, 5% of quinone, and 6% of 17-O-demethylgeldanamycin were observed after 1-min incubation of geldanamycin, whereas about 1% of hydroquinone and 99% of quinone were found in the 60-min incubation of 17AAG. The results provide direct evidence for understanding the 17-substituent effects of these benzoquinone ansamycins on their phase I metabolism, reactivity with glutathione, and acute hepatotoxicity.

Publication types

  • Comparative Study

MeSH terms

  • Antibiotics, Antineoplastic / metabolism*
  • Benzoquinones / metabolism*
  • Biotransformation
  • Cell Hypoxia
  • HSP90 Heat-Shock Proteins / antagonists & inhibitors
  • Humans
  • Lactams, Macrocyclic / metabolism*
  • Microsomes, Liver / metabolism*
  • NADPH-Ferrihemoprotein Reductase / metabolism
  • Oxidation-Reduction

Substances

  • Antibiotics, Antineoplastic
  • Benzoquinones
  • HSP90 Heat-Shock Proteins
  • Lactams, Macrocyclic
  • tanespimycin
  • NADPH-Ferrihemoprotein Reductase
  • geldanamycin