Design and synthesis of biologically active cationic amphiphiles built on the calix[4]arene scaffold

Int J Pharm. 2018 Oct 5;549(1-2):436-445. doi: 10.1016/j.ijpharm.2018.08.020. Epub 2018 Aug 14.

Abstract

A promising strategy to design safer and more effective cationic lipids for gene delivery with inherent antibacterial properties is to covalently tether a lipophilic moiety with oligomeric aminoglycosides (AGs), a large family of Gram-negative-active antibiotics. Herein, we reported the development of a new class of multicationic-head AG-based amphiphiles built on the tetramino-tetrahexyloxycalix[4]arene (4A4Hex-calix-calix[4]) scaffold. Three different conjugates, namely 4A4Hex-calix-calix[4]-neomycin, -neamine, and -paromomycin, were synthesized and characterized. Due to the inherent multivalency of AGs and the amphiphilic behaviour, every 4A4Hex-calix-calix[4]-AG exhibited greater DNA binding ability than the gold standard transfectant 25 kDa bPEI and striking DNA packing ability. DNA/4A4Hex-calix-calix[4]-AG complexes at charge ratios (CRs, +/-) used for transfections displayed good colloidal stability, with a hydrodynamic diameters of ≈150 nm and an overall surface charges of ≈+30 mV. DNA/4A4Hex-calix[4]-AGs nanoassemblies, everyone tested at the optimal CR, invariably showed good transfection efficiency in two cell lines, along with low-to-negligible cytotoxicity. Besides, DNA/4A4Hex-calix-calix[4]-AG complexes exhibited appreciable antimicrobial activity against Gram-negative bacteria, even greater than uncomplexed 4A4Hex-calix-calix[4]-AGs. Altogether, these results disclose 4A4Hex-calix[4]-AGs as promising gene delivery tools with unique antibacterial properties.

Keywords: Aminoglycosides; Antibacterial activity; Calix[4]arenes; Lipoplexes; Non-viral gene delivery vectors; Transfection.

Publication types

  • Comparative Study

MeSH terms

  • Active Transport, Cell Nucleus
  • Anti-Bacterial Agents / chemical synthesis*
  • Anti-Bacterial Agents / metabolism
  • Anti-Bacterial Agents / pharmacology*
  • Binding Sites
  • Calixarenes / chemical synthesis*
  • Calixarenes / metabolism
  • Calixarenes / pharmacology*
  • DNA / chemistry
  • DNA / metabolism
  • Drug Design*
  • Escherichia coli / drug effects*
  • Escherichia coli / growth & development
  • Gene Expression Regulation
  • HeLa Cells
  • Humans
  • Molecular Structure
  • Nucleic Acid Conformation
  • Phenols / chemical synthesis*
  • Phenols / metabolism
  • Phenols / pharmacology*
  • Sarcina / drug effects
  • Sarcina / growth & development
  • Structure-Activity Relationship
  • Surface Properties
  • Surface-Active Agents / chemical synthesis*
  • Surface-Active Agents / metabolism
  • Surface-Active Agents / pharmacology*
  • Transfection / methods*

Substances

  • Anti-Bacterial Agents
  • Phenols
  • Surface-Active Agents
  • calix(4)arene
  • Calixarenes
  • DNA