Construction of a Shape-Diverse Fragment Set: Design, Synthesis and Screen against Aurora-A Kinase

Chemistry. 2019 May 10;25(27):6831-6839. doi: 10.1002/chem.201900815. Epub 2019 Apr 26.

Abstract

Historically, chemists have explored chemical space in a highly uneven and unsystematic manner. As an example, the shape diversity of existing fragment sets does not generally reflect that of all theoretically possible fragments. To assess experimentally the added value of increased three dimensionality, a shape-diverse fragment set was designed and collated. The set was assembled by both using commercially available fragments and harnessing unified synthetic approaches to sp3 -rich molecular scaffolds. The resulting set of 80 fragments was highly three-dimensional, and its shape diversity was significantly enriched by twenty synthesised fragments. The fragment set was screened by high-throughput protein crystallography against Aurora-A kinase, revealing four hits that targeted the binding site of allosteric regulators. In the longer term, it is envisaged that the fragment set could be screened against a range of functionally diverse proteins, allowing the added value of more shape-diverse screening collections to be more fully assessed.

Keywords: diversity-oriented synthesis; fragments; molecular shape.

MeSH terms

  • Allosteric Regulation
  • Aurora Kinase A / antagonists & inhibitors
  • Aurora Kinase A / metabolism*
  • Binding Sites
  • Crystallography, X-Ray
  • Databases, Chemical
  • Drug Design*
  • Molecular Docking Simulation
  • Protein Binding
  • Protein Kinase Inhibitors / chemical synthesis*
  • Protein Kinase Inhibitors / chemistry
  • Protein Kinase Inhibitors / metabolism
  • Protein Structure, Tertiary

Substances

  • Protein Kinase Inhibitors
  • Aurora Kinase A