Discovery of Novel Inhibitors of the Tautomerase Activity of Macrophage Migration Inhibitory Factor (MIF)

J Biomol Screen. 2016 Jun;21(5):446-58. doi: 10.1177/1087057116633997. Epub 2016 Mar 1.

Abstract

Macrophage migration inhibitory factor (MIF) is a proinflammatory cytokine associated with multiple diseases, including neurodegenerative disorders. With the ultimate goal of providing novel chemotypes as starting points for development of disease-modifying therapeutics for neurodegeneration, we endeavored to screen the GSK compound collection for MIF inhibitors using a miniaturized, activity-based kinetic assay. The assay monitors the increase in absorbance at 320 nm resulting from keto-to-enol tautomerization of 4-hydroxyphenylpyruvate, a reaction catalyzed by MIF. We ran a full-diversity screen evaluating the inhibitory activity of 1.6 million compounds. Primary hits were confirmed and retested in an orthogonal assay measuring tautomerization of l-dopachrome methyl ester by the decrease in absorbance at 475 nm in kinetic mode. Selected compounds were progressed to medium-throughput mode-of-inhibition studies, which included time dependence, enzyme concentration dependence, and reversibility of their inhibitory effect. With these results and after inspection of the physicochemical properties of compounds, 17 chemotypes were prioritized and progressed to further stages of validation and characterization to better assess their therapeutic potential.

Keywords: 4-hydroxyphenylpyruvic acid; MIF; high-throughput screening; l-dopachrome methyl ester; macrophage migration inhibitory factor; tautomerase.

MeSH terms

  • Drug Discovery / methods*
  • Humans
  • Intramolecular Oxidoreductases / antagonists & inhibitors*
  • Intramolecular Oxidoreductases / chemistry
  • Intramolecular Oxidoreductases / genetics
  • Kinetics
  • Macrophage Migration-Inhibitory Factors / antagonists & inhibitors*
  • Macrophage Migration-Inhibitory Factors / chemistry
  • Macrophage Migration-Inhibitory Factors / genetics
  • Macrophages / enzymology
  • Neurodegenerative Diseases / drug therapy*
  • Neurodegenerative Diseases / genetics
  • Phenylpyruvic Acids / metabolism
  • Small Molecule Libraries / isolation & purification*
  • Small Molecule Libraries / therapeutic use
  • Structure-Activity Relationship

Substances

  • Macrophage Migration-Inhibitory Factors
  • Phenylpyruvic Acids
  • Small Molecule Libraries
  • 4-hydroxyphenylpyruvic acid
  • Intramolecular Oxidoreductases
  • MIF protein, human