Literature DB >> 22290292

The naphthol selective estrogen receptor modulator (SERM), LY2066948, is oxidized to an o-quinone analogous to the naphthol equine estrogen, equilenin.

Teshome B Gherezghiher1, Bradley Michalsen, R Esala P Chandrasena, Zhihui Qin, Johann Sohn, Gregory R J Thatcher, Judy L Bolton.   

Abstract

o-Quinone forming estrogens and selective estrogen receptor modulators (SERMs) have been associated with carcinogenesis. LY2066948, a novel SERM in development by Eli Lilly for the treatment of uterine fibroids and myomas, has structural similarity to the equine estrogen equilenin present in hormone replacement formulations; both contain a naphthol group susceptible to oxidative metabolism to o-quinones. LY2066948 was synthesized and assayed for antiestrogenic activity, and in cell culture was confirmed to be a more potent antiestrogen than the prototypical SERM, 4-hydroxytamoxifen. Oxidation of LY2066948 with 2-iodoxybenzoic acid gave an o-quinone (t(1/2)=3.9 ± 0.1h) which like 4-hydroxyequilenin-o-quinone (t(1/2)=2.5 ± 0.2 h) was observed to be exceptionally long-lived with the potential to cause cytotoxicity and/or genotoxicity. In model reactions with tyrosinase, the catechol metabolites of LY2066948 and equilenin were products; interestingly, in the presence of ascorbate to inhibit autoxidation, these catechols were formed quantitatively. Tyrosinase incubations in the presence of GSH gave the expected GSH conjugates resulting from trapping of the o-quinones, which were characterized by LC-MS/MS. Incubations of LY2066948 or equilenin with rat liver microsomes also gave detectable o-quinone trapped GSH conjugates; however, as observed with other SERMs, oxidative metabolism of LY2066948 mainly occurred on the amino side chain to yield the N-dealkylated metabolite. CYP1B1 is believed to be responsible for extra-hepatic generation of genotoxic estrogen quinones and o-quinone GSH conjugates were detected in equilenin incubations. However, in corresponding incubations with CYP1B1 supersomes, no o-quinone GSH conjugates of LY2066948 were detected. These studies suggest that although the naphthol group is susceptible to oxidative metabolism to long-lived o-quinones, the formation of these quinones by cytochrome P450 can be attenuated by the chemistry of the remainder of the molecule as in the case of LY2066948.
Copyright © 2012 Elsevier Ireland Ltd. All rights reserved.

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Year:  2012        PMID: 22290292      PMCID: PMC3319273          DOI: 10.1016/j.cbi.2012.01.004

Source DB:  PubMed          Journal:  Chem Biol Interact        ISSN: 0009-2797            Impact factor:   5.192


  55 in total

1.  Bioactivation of tamoxifen to metabolite E quinone methide: reaction with glutathione and DNA.

Authors:  P W Fan; J L Bolton
Journal:  Drug Metab Dispos       Date:  2001-06       Impact factor: 3.922

2.  Estrogen induces apoptosis in estrogen deprivation-resistant breast cancer through stress responses as identified by global gene expression across time.

Authors:  Eric A Ariazi; Heather E Cunliffe; Joan S Lewis-Wambi; Michael J Slifker; Amanda L Willis; Pilar Ramos; Coya Tapia; Helen R Kim; Smitha Yerrum; Catherine G N Sharma; Emmanuelle Nicolas; Yoganand Balagurunathan; Eric A Ross; V Craig Jordan
Journal:  Proc Natl Acad Sci U S A       Date:  2011-10-19       Impact factor: 11.205

3.  4-Hydroxylated metabolites of the antiestrogens tamoxifen and toremifene are metabolized to unusually stable quinone methides.

Authors:  P W Fan; F Zhang; J L Bolton
Journal:  Chem Res Toxicol       Date:  2000-01       Impact factor: 3.739

4.  Equine estrogen metabolite 4-hydroxyequilenin induces DNA damage in the rat mammary tissues: formation of single-strand breaks, apurinic sites, stable adducts, and oxidized bases.

Authors:  F Zhang; S M Swanson; R B van Breemen; X Liu; Y Yang; C Gu; J L Bolton
Journal:  Chem Res Toxicol       Date:  2001-12       Impact factor: 3.739

5.  Regioselective oxidation of phenols to o-quinones with o-iodoxybenzoic acid (IBX).

Authors:  Derek Magdziak; Andy A Rodriguez; Ryan W Van De Water; Thomas R R Pettus
Journal:  Org Lett       Date:  2002-01-24       Impact factor: 6.005

6.  Metabolism of equilenin in MCF-7 and MDA-MB-231 human breast cancer cells.

Authors:  D C Spink; F Zhang; M M Hussain; B H Katz; X Liu; D R Hilker; J L Bolton
Journal:  Chem Res Toxicol       Date:  2001-05       Impact factor: 3.739

7.  Catechin metabolism: glutathione conjugate formation catalyzed by tyrosinase, peroxidase, and cytochrome p450.

Authors:  M Y Moridani; H Scobie; P Salehi; P J O'Brien
Journal:  Chem Res Toxicol       Date:  2001-07       Impact factor: 3.739

8.  A metabolite of equine estrogens, 4-hydroxyequilenin, induces DNA damage and apoptosis in breast cancer cell lines.

Authors:  Y Chen; X Liu; E Pisha; A I Constantinou; Y Hua; L Shen; R B van Breemen; E C Elguindi; S Y Blond; F Zhang; J L Bolton
Journal:  Chem Res Toxicol       Date:  2000-05       Impact factor: 3.739

9.  Identification of tamoxifen-DNA adducts in the endometrium of women treated with tamoxifen.

Authors:  S Shibutani; A Ravindernath; N Suzuki; I Terashima; S M Sugarman; A P Grollman; M L Pearl
Journal:  Carcinogenesis       Date:  2000-08       Impact factor: 4.944

10.  Oxidative DNA damage induced by equine estrogen metabolites: role of estrogen receptor alpha.

Authors:  Xuemei Liu; Jiaqin Yao; Emily Pisha; Yanan Yang; Yousheng Hua; Richard B van Breemen; Judy L Bolton
Journal:  Chem Res Toxicol       Date:  2002-04       Impact factor: 3.739

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  5 in total

1.  Selective estrogen receptor modulator (SERM) lasofoxifene forms reactive quinones similar to estradiol.

Authors:  Bradley T Michalsen; Teshome B Gherezghiher; Jaewoo Choi; R Esala P Chandrasena; Zhihui Qin; Gregory R J Thatcher; Judy L Bolton
Journal:  Chem Res Toxicol       Date:  2012-06-14       Impact factor: 3.739

2.  Add-On Selective Estrogen Receptor Modulators for Methadone Maintenance Treatment.

Authors:  Chieh-Liang Huang; Yao-Chang Chiang; Wei-Chun Chang; Yu-Ting Su; Juan-Cheng Yang; Wei-Chung Cheng; Hsien-Yuan Lane; Ing-Kang Ho; Wen-Lung Ma
Journal:  Front Endocrinol (Lausanne)       Date:  2021-08-05       Impact factor: 5.555

3.  Evaluation of estrogenic activity of licorice species in comparison with hops used in botanicals for menopausal symptoms.

Authors:  Atieh Hajirahimkhan; Charlotte Simmler; Yang Yuan; Jeffrey R Anderson; Shao-Nong Chen; Dejan Nikolić; Birgit M Dietz; Guido F Pauli; Richard B van Breemen; Judy L Bolton
Journal:  PLoS One       Date:  2013-07-12       Impact factor: 3.240

Review 4.  Selective estrogen receptor modulators: tissue specificity and clinical utility.

Authors:  Stephen Martinkovich; Darshan Shah; Sonia Lobo Planey; John A Arnott
Journal:  Clin Interv Aging       Date:  2014-08-28       Impact factor: 4.458

5.  Formation and Biological Targets of Quinones: Cytotoxic versus Cytoprotective Effects.

Authors:  Judy L Bolton; Tareisha Dunlap
Journal:  Chem Res Toxicol       Date:  2016-09-29       Impact factor: 3.739

  5 in total

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