Protoflavones in melanoma therapy: Prooxidant and pro-senescence effect of protoapigenone and its synthetic alkyl derivative in A375 cells

Life Sci. 2020 Nov 1:260:118419. doi: 10.1016/j.lfs.2020.118419. Epub 2020 Sep 12.

Abstract

Aims: In our study, the anticancer effects of a semisynthetic p-quinol, protoapigenone 1'-O-butyl ether (PABut), were tested in human melanoma A375 cells also in comparison with natural congener, protoapigenone (PA).

Main methods: The cytotoxic effect of PABut and PA was determined using MTT assay. Flow cytometry analysis was used to evaluate the influence of the compounds tested on ROS generation and cell cycle distribution in A375 cells. Moreover, apoptosis was evaluated by AO/EB dual staining as well as by flow cytometry. Markers of senescence were quantified by spectrofluorimetry and by Western blot analysis.

Key findings: Both PABut and PA showed significant cytotoxicity against melanoma A375 cells at sub-micromolar concentrations. Both protoflavones induced comparable cell cycle arrest in G2/M phase. However, a more profound upregulation of intracellular ROS levels was found following PABut treatment. An increased apoptosis in the cells following 48 h treatment with both protoflavones tested was also confirmed. Both compounds tested remarkably upregulated p21 protein levels in A375 cells. Unlike PA, PABut significantly decreased protein levels of NAD+-dependent deacetylase SirT1 and β-actin accompanied by mild significant upregulation of mitochondrial SOD2 and senescence markers, p16 protein and SA-β-Gal activity. However, a significant upregulation of p53 only following PA treatment was found.

Significance: These results suggest that PABut and PA confer high chemotherapeutic potential in melanoma cells and are suitable for further testing. Furthermore, modification of protoapigenone with 1'-O-butyl ether moiety can be associated with improved senescence-inducing effect and, thus, enhanced chemotherapeutic potency of PABut compared to the unmodified natural protoflavone.

Keywords: Alkyl protoflavone; Flavonoid; Melanoma; Protoapigenone; Semi-synthesis; Senescence.

MeSH terms

  • Antineoplastic Agents, Phytogenic / chemistry
  • Antineoplastic Agents, Phytogenic / pharmacology*
  • Antineoplastic Agents, Phytogenic / therapeutic use
  • Autophagy / drug effects
  • Biomarkers / metabolism
  • Cell Cycle / drug effects
  • Cell Line, Tumor
  • Cellular Senescence / drug effects
  • Cyclohexanones / chemistry
  • Cyclohexanones / pharmacology*
  • Ethers / chemistry
  • Ethers / pharmacology*
  • Ethers / therapeutic use
  • Flavones / chemistry
  • Flavones / pharmacology*
  • Humans
  • Hydroquinones / chemistry
  • Hydroquinones / pharmacology*
  • Hydroquinones / therapeutic use
  • Melanoma / drug therapy*
  • Melanoma / metabolism
  • Melanoma / pathology*
  • Reactive Oxygen Species / metabolism
  • Superoxide Dismutase / metabolism
  • beta-Galactosidase / metabolism

Substances

  • Antineoplastic Agents, Phytogenic
  • Biomarkers
  • Cyclohexanones
  • Ethers
  • Flavones
  • Hydroquinones
  • Reactive Oxygen Species
  • protoapigenone
  • protoapigenone 1'-O-butyl ether
  • Superoxide Dismutase
  • superoxide dismutase 2
  • GLB1 protein, human
  • beta-Galactosidase