Short Total Synthesis of Δ12-Prostaglandin J2 and Related Prostaglandins. Design, Synthesis, and Biological Evaluation of Macrocyclic Δ12-Prostaglandin J2 Analogues

J Org Chem. 2019 Jan 4;84(1):365-378. doi: 10.1021/acs.joc.8b03057. Epub 2018 Dec 20.

Abstract

Comprised of a large collection of structurally diverse molecules, the prostaglandins exhibit a wide range of biological properties. Among them are Δ12-prostaglandin J212-PGJ2) and Δ12-prostaglandin J312-PGJ3), whose unusual structural motifs and potent cytotoxicities present unique opportunities for chemical and biological investigations. Herein, we report a short olefin-metathesis-based total synthesis of Δ12-PGJ2 and its application to the construction of a series of designed analogues possessing monomeric, dimeric, trimeric, and tetrameric macrocyclic lactones consisting of units of this prostaglandin. Biological evaluation of these analogues led to interesting structure-activity relationships and trends and the discovery of a number of more potent antitumor agents than their parent naturally occurring molecules.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Antineoplastic Agents / chemical synthesis*
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology*
  • Cell Line, Tumor
  • Chemistry Techniques, Synthetic
  • Drug Design*
  • Humans
  • Prostaglandin D2 / chemical synthesis*
  • Prostaglandin D2 / chemistry
  • Prostaglandin D2 / pharmacology*
  • Structure-Activity Relationship

Substances

  • Antineoplastic Agents
  • delta(12)-prostaglandin J(2)
  • Prostaglandin D2