Discovery of 2,4-pyrimidinediamine derivatives as potent dual inhibitors of ALK and HDAC

Eur J Med Chem. 2021 Nov 15:224:113672. doi: 10.1016/j.ejmech.2021.113672. Epub 2021 Jun 29.

Abstract

Combination of anaplastic lymphoma kinase (ALK) inhibitor with histone deacetylases (HDAC) inhibitor could exert synergistically anti-proliferative effects on ALK positive non-small cell lung cancer (NSCLC) naïve or resistant cells. In this work, we designed and synthesized a series of 2,4-pyrimidinediamine derivatives as dual ALK and HDAC inhibitors based on pharmacophore merged strategy. Among which, compound 10f displayed the most potent and balanced inhibitory activity against ALK (IC50 = 2.1 nM) and HDAC1 (IC50 = 7.9 nM), respectively. In particular, 10f was also potent against the frequently observed Crizotinib-resistant ALKL1196M (IC50 = 1.7 nM) as well as the Ceritinib-resistant ALKG1202R (IC50 = 0.4 nM) mutants. In antiproliferative activity assay, 10f exhibited impressive activity on ALK-addicted cancer cell lines at low micromole concentrations, which was comparable to that of Crizotinib and Ceritinib. Further flow cytometric analysis indicated that 10f could effectively induce cell death via cell apoptosis and cell cycle arrest. Taken together, these results suggested 10f would be a promising lead compound for the ALK-positive NSCLC treatment, especially the Ceritinib- or Crizotinib-resistant NSCLC.

Keywords: 2,4-Pyrimidinediamine; ALK/HDAC dual Inhibitors; NSCLC; Pharmacophore merged strategy.

MeSH terms

  • Anaplastic Lymphoma Kinase / antagonists & inhibitors*
  • Anaplastic Lymphoma Kinase / metabolism
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / metabolism
  • Antineoplastic Agents / pharmacology
  • Apoptosis / drug effects
  • Binding Sites
  • Cell Cycle Checkpoints / drug effects
  • Cell Line, Tumor
  • Cell Movement / drug effects
  • Cell Proliferation / drug effects
  • Diamines / chemistry*
  • Diamines / metabolism
  • Diamines / pharmacology
  • Drug Design
  • Drug Resistance, Neoplasm / drug effects
  • Drug Screening Assays, Antitumor
  • Histone Deacetylase Inhibitors / chemistry*
  • Histone Deacetylase Inhibitors / metabolism
  • Histone Deacetylase Inhibitors / pharmacology
  • Histone Deacetylases / chemistry*
  • Histone Deacetylases / metabolism
  • Humans
  • Molecular Dynamics Simulation
  • Protein Kinase Inhibitors / chemistry*
  • Protein Kinase Inhibitors / metabolism
  • Protein Kinase Inhibitors / pharmacology
  • Pyrimidines / chemistry
  • Structure-Activity Relationship

Substances

  • Antineoplastic Agents
  • Diamines
  • Histone Deacetylase Inhibitors
  • Protein Kinase Inhibitors
  • Pyrimidines
  • Anaplastic Lymphoma Kinase
  • Histone Deacetylases
  • pyrimidine