Structure-based design, synthesis, and biological evaluation of withaferin A-analogues as potent apoptotic inducers

Eur J Med Chem. 2017 Nov 10:140:52-64. doi: 10.1016/j.ejmech.2017.09.004. Epub 2017 Sep 6.

Abstract

Apoptosis inducers represent an attractive approach for the discovery and development of anticancer agents. Herein, we report on the development by molecular fine tuning of a withaferin A-based library of 63 compounds (2-64), 53 of them reported for the first time. Their antiproliferative evaluation on HeLa, A-549 and MCF-7 human tumor cell lines identified fifteen analogues displaying higher activity (IC50 values ranging 0.3-4.8 μM) than the lead (IC50 values ranging 1.3-10.1 μM) either in lag or log growth phases. SAR analysis revealed that acylation enhances cytotoxicity, suggesting the hydrophobic moiety contributes to the activity, presumably by increasing affinity and/or cell membrane permeability. Further investigation clearly indicated that compounds 3, 11, 12, and 18 induce apoptosis evidenced by chromatin condensation, phosphatidylserine externalization, and caspase-3 activation effects on HeLa cells. The potent capacity to induce apoptosis with concomitant cell loss in G2/M highlights the potential of 27-benzyl analogue (18) as an apoptotic inducer drug candidate.

Keywords: Apoptosis; Compound library; Cytotoxicity; Structure-activity relationship; Withaferin A.

MeSH terms

  • Animals
  • Antineoplastic Agents, Phytogenic / chemical synthesis
  • Antineoplastic Agents, Phytogenic / chemistry
  • Antineoplastic Agents, Phytogenic / pharmacology*
  • Apoptosis / drug effects*
  • Cell Proliferation / drug effects
  • Cell Survival / drug effects
  • Cells, Cultured
  • Chlorocebus aethiops
  • Dose-Response Relationship, Drug
  • Drug Design*
  • Drug Screening Assays, Antitumor
  • Humans
  • Molecular Structure
  • Plant Leaves / chemistry
  • Structure-Activity Relationship
  • Vero Cells
  • Withania / chemistry
  • Withanolides / chemical synthesis
  • Withanolides / chemistry
  • Withanolides / pharmacology*

Substances

  • Antineoplastic Agents, Phytogenic
  • Withanolides
  • withaferin A