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Facile synthesis of 1,2-dione-containing abietane analogues for the generation of human carboxylesterase inhibitors.
Binder, Randall J; Hatfield, M Jason; Chi, Liying; Potter, Philip M.
Afiliación
  • Binder RJ; Department of Chemical Biology and Therapeutics, 262 Danny Thomas Place, St. Jude Children's Research Hospital, Memphis, TN 38105, United States. Electronic address: Randall.binder@stjude.org.
  • Hatfield MJ; Department of Chemical Biology and Therapeutics, 262 Danny Thomas Place, St. Jude Children's Research Hospital, Memphis, TN 38105, United States. Electronic address: Jason.hatfield@stjude.org.
  • Chi L; Department of Chemical Biology and Therapeutics, 262 Danny Thomas Place, St. Jude Children's Research Hospital, Memphis, TN 38105, United States. Electronic address: Liying.chi@stjude.org.
  • Potter PM; Department of Chemical Biology and Therapeutics, 262 Danny Thomas Place, St. Jude Children's Research Hospital, Memphis, TN 38105, United States. Electronic address: Phil.potter@stjude.org.
Eur J Med Chem ; 149: 79-89, 2018 Apr 10.
Article en En | MEDLINE | ID: mdl-29499489
Recently, a series of selective human carboxylesterase inhibitors have been identified based upon the tanshinones, with biologically active molecules containing a 1,2-dione group as part of a naphthoquinone core. Unfortunately, the synthesis of such compounds is complex. Here we describe a novel method for the generation of 1,2-dione containing diterpenoids using a unified approach, by which boronic acids are joined to vinyl bromo-cyclohexene derivatives via Suzuki coupling, followed by electrocyclization and oxidation to the o-phenanthroquinones. This has allowed the construction of a panel of miltirone analogues containing an array of substituents (methyl, isopropyl, fluorine, methoxy) which have been used to develop preliminary SAR with the two human carboxylesterase isoforms. As a consequence, we have synthesized highly potent inhibitors of these enzymes (Ki < 15 nM), that maintain the core tanshinone scaffold. Hence, we have developed a facile and reproducible method for the synthesis of abietane analogues that have resulted in a panel of miltirone derivatives that will be useful tool compounds to assess carboxylesterase biology.
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Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Fenantrenos / Abietanos / Carboxilesterasa / Técnicas de Química Sintética Límite: Humans Idioma: En Revista: Eur J Med Chem Año: 2018 Tipo del documento: Article Pais de publicación: Francia

Texto completo: 1 Colección: 01-internacional Base de datos: MEDLINE Asunto principal: Fenantrenos / Abietanos / Carboxilesterasa / Técnicas de Química Sintética Límite: Humans Idioma: En Revista: Eur J Med Chem Año: 2018 Tipo del documento: Article Pais de publicación: Francia