Tamoxifen-DNA adducts formed by alpha-acetoxytamoxifen N-oxide

Chem Res Toxicol. 1999 Nov;12(11):1083-9. doi: 10.1021/tx990132+.

Abstract

DNA adduct formation is assumed to be a major carcinogenic event, leading to the development of endometrial cancer in breast cancer patients taking tamoxifen and healthy women enrolled in a tamoxifen chemopreventive trial. To determine whether DNA adducts were formed by tamoxifen, trans- and cis-alpha-acetoxytamoxifen N-oxides were synthesized as model-activated forms via major tamoxifen metabolites, tamoxifen N-oxide and alpha-hydroxytamoxifen N-oxide. When alpha-acetoxytamoxifen N-oxide was reacted with human DNA, at least three DNA adducts were detected by (32)P-postlabeling coupled with HPLC. The total amount of DNA adducts formed by trans-alpha-hydroxytamoxifen N-oxide was 1.5-fold higher than that formed by the cis form. Both trans- and cis-alpha-acetoxytamoxifen N-oxide reacted with 2'-deoxyguanosine, resulting in the formation of three adducts (fr-1, fr-2-1, and fr-2-2). These products were studied using mass spectroscopy and proton magnetic resonance spectroscopy. fr-1 was identified as a mixture of the epimers of trans-alpha-(N(2)-deoxyguanosinyl)tamoxifen N-oxide. fr-2-1 and fr-2-2 were determined to be epimers of cis-alpha-(N(2)-deoxyguanosinyl)tamoxifen N-oxide.

Publication types

  • Research Support, Non-U.S. Gov't
  • Research Support, U.S. Gov't, P.H.S.

MeSH terms

  • Acetylation
  • Antineoplastic Agents, Hormonal / chemistry*
  • Chromatography, High Pressure Liquid
  • DNA Adducts / chemistry*
  • Spectrometry, Mass, Fast Atom Bombardment
  • Sulfates / chemistry
  • Tamoxifen / analogs & derivatives*
  • Tamoxifen / chemistry*

Substances

  • Antineoplastic Agents, Hormonal
  • DNA Adducts
  • Sulfates
  • alpha-acetoxytamoxifen
  • Tamoxifen