Synthesis of Unsymmetrical Squaramides as Allosteric GSK-3β Inhibitors Promoting β-Catenin-Mediated Transcription of TCF/LEF in Retinal Pigment Epithelial Cells

ChemMedChem. 2022 Dec 16;17(24):e202200456. doi: 10.1002/cmdc.202200456. Epub 2022 Oct 27.

Abstract

The glycogen synthase kinase 3β (GSK-3β) is a ubiquitous enzyme that is a validated target for the development of potential therapeutics useful in several diseases including retinal degeneration. Aiming at developing an innovative class of allosteric inhibitors of GSK-3β potentially useful for retinal degeneration, we explored the class of squaramides. The developed compounds (6 a-l) were obtained through a nontoxic one-pot synthetic protocol, which employs low-cost goods and avoids any purification step. Ethanol was used as the reaction solvent, simultaneously allowing the pure reaction products' recovery (by precipitation). Out of this set of squaramides, 6 j stood out, from computational and enzymatic converging data, as an ATP non-competitive inhibitor of GSK-3β of micromolar potency. When engaged in cellular studies using retinal pigment epithelial cells (ARPE-19) transfected with a luciferase reporter gene under the control of T-cell factor/lymphoid enhancer factor (TCF/LEF) binding sites, 6 j was able to dose-dependently induce β-catenin nuclear accumulation, as shown by the increased luciferase activity at a concentration of 2.5 μM.

Keywords: The authors thank MIUR-PRIN no. 20175SA5JJ..

MeSH terms

  • Epithelial Cells* / metabolism
  • Glycogen Synthase Kinase 3 beta* / antagonists & inhibitors
  • Humans
  • Luciferases / metabolism
  • Quinine* / analogs & derivatives
  • Quinine* / chemical synthesis
  • Retinal Degeneration*
  • Retinal Pigment Epithelium
  • Signal Transduction
  • TCF Transcription Factors* / genetics
  • TCF Transcription Factors* / metabolism
  • beta Catenin / metabolism

Substances

  • beta Catenin
  • Glycogen Synthase Kinase 3 beta
  • Luciferases
  • squaramide
  • TCF Transcription Factors
  • Quinine