Synthesis, DNA/RNA-interaction and biological activity of benzo[k,l]xanthene lignans

Bioorg Chem. 2020 Nov:104:104190. doi: 10.1016/j.bioorg.2020.104190. Epub 2020 Aug 26.

Abstract

Interactions of two newly synthesized and six previously reported benzoxanthene lignans (BXLs), analogues of rare natural products, with DNA/RNA, G-quadruplex and HSA were evaluated by a set of spectrophotometric methods. Presence/absence of methoxy and hydroxy groups on the benzoxanthene core and minor modifications at C-1/C-2 side pendants - presence/absence of phenyl ring and presence/absence of methoxy and hydroxy groups on phenyl ring - influenced the fluorescence changes and the binding strength to double-stranded (ds-) and G-quadruplex structures. In general, compounds without phenyl ring showed stronger fluorescence changes upon binding than phenyl-substituted BXLs. On the other hand, BXLs with an unsubstituted phenyl ring showed the best stabilization effects of G-quadruplex. Circular dichroism spectroscopy results suggest mixed binding mode, groove binding and partial intercalation, to ds-DNA/RNA and end-stacking to top or bottom G-tetrads as the main binding modes of BXLs to those targets. All compounds exhibited micromolar binding affinities toward HSA and an increased protein thermal stability. Moderate to strong antiradical scavenging activity was observed for all BXLs with hydroxy groups at C-6, C-9 and C-10 positions of the benzoxanthene core, except for derivative bearing methoxy groups at these positions. BXLs with unsubstituted or low-substituted phenyl ring and one derivative without phenyl ring showed strong growth inhibition of Gram-positive Staphylococcus aureus. All compounds showed moderate to strong tumor cell growth-inhibitory activity and cytotoxicity.

Keywords: Antiproliferative effect; Benzo[k,l]xanthene lignans; DNA/RNA recognition; G-quadruplex interaction; HSA interaction.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Antineoplastic Agents / chemical synthesis
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / pharmacology*
  • Cell Proliferation / drug effects
  • Circulating Tumor DNA / chemistry*
  • Dose-Response Relationship, Drug
  • Drug Screening Assays, Antitumor
  • Escherichia coli K12 / cytology
  • Escherichia coli K12 / drug effects
  • Humans
  • Lignans / chemical synthesis
  • Lignans / chemistry
  • Lignans / pharmacology*
  • Molecular Structure
  • RNA, Neoplasm / chemistry*
  • Salmonella enterica / cytology
  • Salmonella enterica / drug effects
  • Serum Albumin, Human / chemistry*
  • Staphylococcus aureus / cytology
  • Staphylococcus aureus / drug effects
  • Structure-Activity Relationship
  • Tumor Cells, Cultured
  • Xanthenes / chemical synthesis
  • Xanthenes / chemistry
  • Xanthenes / pharmacology*

Substances

  • Antineoplastic Agents
  • Circulating Tumor DNA
  • Lignans
  • RNA, Neoplasm
  • Xanthenes
  • Serum Albumin, Human