C-H Activation Enables a Concise Total Synthesis of Quinine and Analogues with Enhanced Antimalarial Activity

Angew Chem Int Ed Engl. 2018 Aug 13;57(33):10737-10741. doi: 10.1002/anie.201804551. Epub 2018 Jun 22.

Abstract

We report a novel approach to the classical natural product quinine that is based on two stereoselective key steps, namely a C-H activation and an aldol reaction, to unite the two heterocyclic moieties of the target molecule. This straightforward and flexible strategy enables a concise synthesis of natural (-)-quinine, the first synthesis of unnatural (+)-quinine, and also provides access to unprecedented C3-aryl analogues, which were prepared in only six steps. We additionally demonstrate that these structural analogues exhibit improved antimalarial activity compared with (-)-quinine both in vitro and in mice infected with Plasmodium berghei.

Keywords: C−H activation; malaria; quinine; total synthesis.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Aldehydes / chemistry
  • Animals
  • Antimalarials / chemical synthesis*
  • Antimalarials / pharmacology
  • Antimalarials / therapeutic use
  • Carbon / chemistry
  • Catalysis
  • Crystallography, X-Ray
  • Hydrogen / chemistry
  • Malaria / drug therapy
  • Malaria / veterinary
  • Mice
  • Molecular Conformation
  • Plasmodium berghei / drug effects
  • Quinine / analogs & derivatives*
  • Quinine / pharmacology
  • Quinine / therapeutic use
  • Ruthenium / chemistry
  • Stereoisomerism

Substances

  • Aldehydes
  • Antimalarials
  • Carbon
  • Ruthenium
  • Hydrogen
  • 3-hydroxybutanal
  • Quinine