Quaternary ammonium-linked glucuronidation of tamoxifen by human liver microsomes and UDP-glucuronosyltransferase 1A4

Biochem Pharmacol. 2004 Jun 1;67(11):2093-102. doi: 10.1016/j.bcp.2004.02.014.

Abstract

Tamoxifen (TAM), a nonsteroidal antiestrogen, is the most widely used drug for chemotherapy of hormone-dependent breast cancer in women. In the present study, we found a new potential metabolic pathway of TAM via N-linked glucuronic acid conjugation for excretion in humans. TAM N(+)-glucuronide was isolated from a reaction mixture consisting of TAM and human liver microsomes fortified with UDP-glucuronic acid (UDPGA) and identified with a synthetic specimen by high-performance liquid chromatography-electrospray ionization-mass spectrometry. However, no TAM-glucuronidating activity was detected in microsomes from rat, mouse, monkey, dog, and guinea pig livers. A strong correlation (r(2) =0.92 ) was observed between N-glucuronidating activities toward TAM and trifluoperazine, a probe substrate for human UDP-glucuronosyltransferase (UGT) 1A4, in human liver microsomes from eight donors (five females, three males). However, no correlation ( (r(2) =0.02 )) was observed in the activities between 7-hydroxy-4-(trifluoromethyl)coumarin and TAM. Only UGT1A4 catalyzed the N-linked glucuronidation of TAM among recombinant UGTs (UGT1A1, UGT1A3, UGT1A4, UGT1A6, UGT1A9, UGT2B4, UGT2B7, UGT2B15, and UGT2B17) expressed in insect cells. Apparent K(m) values for TAM N-glucuronidation by human liver microsomes and recombinant UGT1A4 were 35.8 and 32.4 microM, respectively. These results strongly suggested that UGT1A4 could play a role in metabolism and excretion of TAM without Phase I metabolism in human liver. TAM N(+)-glucuronide still had binding affinity similar to TAM itself for human estrogen receptors, ERalpha and ERbeta, suggesting that TAM N(+)-glucuronide might contribute to the biological activity of TAM in vivo.

MeSH terms

  • Adult
  • Aged
  • Animals
  • Antineoplastic Agents, Hormonal / metabolism
  • Dogs
  • Estrogen Receptor alpha
  • Female
  • Glucuronides / metabolism*
  • Glucuronosyltransferase / metabolism*
  • Guinea Pigs
  • Humans
  • Insecta / cytology
  • Macaca fascicularis
  • Male
  • Mice
  • Microsomes, Liver / metabolism*
  • Middle Aged
  • Rats
  • Rats, Sprague-Dawley
  • Receptors, Estrogen / metabolism
  • Tamoxifen / metabolism*
  • Uridine Diphosphate Glucuronic Acid / pharmacology

Substances

  • Antineoplastic Agents, Hormonal
  • Estrogen Receptor alpha
  • Glucuronides
  • Receptors, Estrogen
  • bilirubin glucuronoside glucuronosyltransferase
  • Tamoxifen
  • Uridine Diphosphate Glucuronic Acid
  • Glucuronosyltransferase