Identification, design and biological evaluation of heterocyclic quinolones targeting Plasmodium falciparum type II NADH:quinone oxidoreductase (PfNDH2)

J Med Chem. 2012 Mar 8;55(5):1844-57. doi: 10.1021/jm201184h. Epub 2012 Feb 24.

Abstract

Following a program undertaken to identify hit compounds against NADH:ubiquinone oxidoreductase (PfNDH2), a novel enzyme target within the malaria parasite Plasmodium falciparum, hit to lead optimization led to identification of CK-2-68, a molecule suitable for further development. In order to reduce ClogP and improve solubility of CK-2-68 incorporation of a variety of heterocycles, within the side chain of the quinolone core, was carried out, and this approach led to a lead compound SL-2-25 (8b). 8b has IC(50)s in the nanomolar range versus both the enzyme and whole cell P. falciparum (IC(50) = 15 nM PfNDH2; IC(50) = 54 nM (3D7 strain of P. falciparum) with notable oral activity of ED(50)/ED(90) of 1.87/4.72 mg/kg versus Plasmodium berghei (NS Strain) in a murine model of malaria when formulated as a phosphate salt. Analogues in this series also demonstrate nanomolar activity against the bc(1) complex of P. falciparum providing the potential added benefit of a dual mechanism of action. The potent oral activity of 2-pyridyl quinolones underlines the potential of this template for further lead optimization studies.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Administration, Oral
  • Animals
  • Antimalarials / chemical synthesis*
  • Antimalarials / chemistry
  • Antimalarials / pharmacology
  • Atovaquone / pharmacology
  • Crystallography, X-Ray
  • Cytochromes b / genetics
  • Drug Design
  • Drug Resistance
  • Humans
  • Malaria / drug therapy
  • Male
  • Mice
  • Microsomes, Liver / metabolism
  • Models, Molecular
  • Parasitic Sensitivity Tests
  • Plasmodium berghei
  • Plasmodium falciparum / drug effects
  • Plasmodium falciparum / enzymology*
  • Plasmodium falciparum / genetics
  • Pyridines / chemical synthesis*
  • Pyridines / chemistry
  • Pyridines / pharmacology
  • Quinolones / chemical synthesis*
  • Quinolones / chemistry
  • Quinolones / pharmacology
  • Quinone Reductases / antagonists & inhibitors*
  • Rats
  • Structure-Activity Relationship

Substances

  • Antimalarials
  • Pyridines
  • Quinolones
  • SL-2-25
  • Cytochromes b
  • NADH dehydrogenase (quinone)
  • Quinone Reductases
  • Atovaquone