Synthesis and Biological Activity of Tetracyclic Dispiro Core Derivatives of Natural Products Dispirocochlearoids A-C

Org Lett. 2024 Nov 15;26(45):9654-9658. doi: 10.1021/acs.orglett.4c03358. Epub 2024 Nov 1.

Abstract

Natural products dispirocochlearoids A-C, which are meroterpenoids derived from Ganoderma fungi, feature a 6/6/5/6/6/6 ring system and exhibit selective COX-2 inhibitory activity. Herein, the concise total synthesis of the tetracyclic core structure of dispirocochlearoids A-C was achieved through an aldol reaction/cyclization/deprotection/cyclization cascade sequence. A series of simplified tetracyclic analogues was successfully constructed and their anti-inflammatory activity was further explored, with several tetracyclic analogues (such as compound 8ab) exhibiting strong inhibitory activity against IL-1β expression in lipopolysaccharide-stimulated bone marrow-derived macrophage cells (IC50 = 2.8 μM).

MeSH terms

  • Animals
  • Anti-Inflammatory Agents / chemical synthesis
  • Anti-Inflammatory Agents / chemistry
  • Anti-Inflammatory Agents / pharmacology
  • Biological Products* / chemical synthesis
  • Biological Products* / chemistry
  • Biological Products* / pharmacology
  • Cyclization
  • Cyclooxygenase 2 Inhibitors / chemical synthesis
  • Cyclooxygenase 2 Inhibitors / chemistry
  • Cyclooxygenase 2 Inhibitors / pharmacology
  • Ganoderma / chemistry
  • Interleukin-1beta / antagonists & inhibitors
  • Interleukin-1beta / metabolism
  • Lipopolysaccharides* / antagonists & inhibitors
  • Lipopolysaccharides* / pharmacology
  • Macrophages* / drug effects
  • Mice
  • Molecular Structure
  • Structure-Activity Relationship
  • Terpenes / chemical synthesis
  • Terpenes / chemistry
  • Terpenes / pharmacology

Substances

  • Biological Products
  • Lipopolysaccharides
  • Interleukin-1beta
  • Anti-Inflammatory Agents
  • Terpenes
  • Cyclooxygenase 2 Inhibitors