Chemical and computational methods for the characterization of covalent reactive groups for the prospective design of irreversible inhibitors

J Med Chem. 2014 Dec 11;57(23):10072-9. doi: 10.1021/jm501412a. Epub 2014 Nov 26.

Abstract

Interest in drugs that covalently modify their target is driven by the desire for enhanced efficacy that can result from the silencing of enzymatic activity until protein resynthesis can occur, along with the potential for increased selectivity by targeting uniquely positioned nucleophilic residues in the protein. However, covalent approaches carry additional risk for toxicities or hypersensitivity reactions that can result from covalent modification of unintended targets. Here we describe methods for measuring the reactivity of covalent reactive groups (CRGs) with a biologically relevant nucleophile, glutathione (GSH), along with kinetic data for a broad array of electrophiles. We also describe a computational method for predicting electrophilic reactivity, which taken together can be applied to the prospective design of thiol-reactive covalent inhibitors.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Drug Design
  • Enzyme Inhibitors / chemistry*
  • Glutathione / chemistry*
  • Glutathione / metabolism
  • Humans
  • Kinetics
  • Mass Spectrometry
  • Nuclear Magnetic Resonance, Biomolecular
  • Pharmaceutical Preparations / chemistry

Substances

  • Enzyme Inhibitors
  • Pharmaceutical Preparations
  • Glutathione