Synthesis and evaluation of colletoic acid core derivatives

Eur J Med Chem. 2016 Mar 3:110:126-32. doi: 10.1016/j.ejmech.2016.01.027. Epub 2016 Jan 20.

Abstract

Cortisol homeostasis has been linked to the pathogenesis of metabolic syndrome (MetS), since it stimulates hepatic gluconeogenesis and adipogenesis. MetS is classified as a constellation of health conditions that increase the risk of type 2 diabetes and cardiovascular disease. Intracellular cortisol levels are regulated by 11β-hydroxysteroid dehydrogenase (type 1 and type 2) in a tissue dependent manner. The type 1 enzyme (11β-HSD1) is widely expressed in glucocorticoid targeted tissues and is responsible for the conversion of cortisone to the active cortisol. Local reduction of cortisol regeneration presents a potential strategy for MetS treatment. Recently we disclosed the total synthesis of (+)-colletoic acid as a potent 11β-HSD1 inhibitor. Herein, we describe our improved processing chemistry for the synthesis of the colletoic acid core to access a diverse number of derivatives for evaluation against 11β-HSD1. The Evan's chiral auxiliary was utilized to construct the acyclic precursor 12 to afford the acorane core 9 using a modified Heck reaction in excellent chemical yields. The colletoic acid core derivatives showed modest activity against 11β-HSD1 and will serve for further biological evaluation.

Keywords: (+)-colletoic acid; 11β-HSD1; 11β-HSD2; Metabolic syndrome.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • 11-beta-Hydroxysteroid Dehydrogenase Type 1 / antagonists & inhibitors*
  • 11-beta-Hydroxysteroid Dehydrogenase Type 1 / metabolism
  • Enzyme Inhibitors / chemical synthesis
  • Enzyme Inhibitors / chemistry*
  • Enzyme Inhibitors / pharmacology*
  • Humans
  • Hydrocortisone / metabolism*
  • Metabolic Syndrome / drug therapy
  • Metabolic Syndrome / enzymology
  • Metabolic Syndrome / metabolism
  • Models, Molecular
  • Sesquiterpenes / chemical synthesis
  • Sesquiterpenes / chemistry*
  • Sesquiterpenes / pharmacology*

Substances

  • Enzyme Inhibitors
  • Sesquiterpenes
  • colletoic acid
  • 11-beta-Hydroxysteroid Dehydrogenase Type 1
  • Hydrocortisone