Quaternary ammonium-linked glucuronidation of trans-4-hydroxytamoxifen, an active metabolite of tamoxifen, by human liver microsomes and UDP-glucuronosyltransferase 1A4

Biochem Pharmacol. 2006 Apr 28;71(9):1358-69. doi: 10.1016/j.bcp.2006.01.004. Epub 2006 Feb 14.

Abstract

Tamoxifen (TAM), a nonsteroidal antiestrogen, is the most widely used drug for chemotherapy of hormone-dependent breast cancer in women. Trans-4-hydroxy-TAM (trans-4-HO-TAM), one of the TAM metabolites in humans, has been considered to be an active metabolite of TAM because of its higher affinity toward estrogen receptors (ERs) than the parent drug and other side-chain metabolites. In the present study, we found a new potential metabolic pathway of trans-4-HO-TAM and its geometrical isomer, cis-4-HO-TAM, via N-linked glucuronic acid conjugation for excretion in humans. N+-Glucuronides of 4-HO-TAM isomers were isolated along with O-glucuronides from a reaction mixture consisting of trans- or cis-4-HO-TAM and human liver microsomes fortified with UDP-glucuronic acid and identified with their respective synthetic specimens by high performance liquid chromatography-electrospray ionization time-of-flight mass spectrometry. Although N- and O-glucuronidating activities of human liver microsomes toward trans-4-HO-TAM were nearly comparable, O-glucuronidation was predominant for cis-4-HO-TAM conjugation. Only UGT1A4 catalyzed the N-linked glucuronidation of 4-HO-TAM among recombinant human UGT isoforms (UGT1A1, UGT1A3, UGT1A4, UGT1A6, UGT1A7, UGT1A8, UGT1A9, UGT1A10, UGT2B4, UGT2B7, UGT2B15, and UGT2B17) expressed in insect cells. In contrast, all UGT isoforms, except for UGT1A3 and UGT1A4, catalyzed O-glucuronidation of 4-HO-TAM. Although O-glucuronidation of 4-HO-TAM greatly decreased binding affinity for human ERs, 4-HO-TAM N+-glucuronide still had binding affinity similar to 4-HO-TAM itself, suggesting that N+-glucuronide might contribute to the biological activity of TAM in vivo.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Animals
  • Dogs
  • Female
  • Glucuronides / metabolism*
  • Glucuronosyltransferase / metabolism*
  • Guinea Pigs
  • Humans
  • In Vitro Techniques
  • Insecta
  • Macaca fascicularis
  • Male
  • Mice
  • Mice, Inbred Strains
  • Microsomes, Liver / metabolism
  • Protein Isoforms / metabolism
  • Quaternary Ammonium Compounds
  • Rabbits
  • Rats
  • Rats, Sprague-Dawley
  • Recombinant Proteins / metabolism
  • Species Specificity
  • Tamoxifen / analogs & derivatives*
  • Tamoxifen / metabolism

Substances

  • Glucuronides
  • Protein Isoforms
  • Quaternary Ammonium Compounds
  • Recombinant Proteins
  • bilirubin glucuronoside glucuronosyltransferase
  • Tamoxifen
  • afimoxifene
  • Glucuronosyltransferase