Mitochondrial-DNA-Targeted IrIII -Containing Metallohelices with Tunable Photodynamic Therapy Efficacy in Cancer Cells

Angew Chem Int Ed Engl. 2020 Apr 16;59(16):6420-6427. doi: 10.1002/anie.201915281. Epub 2020 Feb 25.

Abstract

The development of DNA-targeted photodynamic therapy (PDT) agents for cancer treatment has drawn substantial attention. Herein, the design and synthesis of dinuclear IrIII -containing luminescent metallohelices with tunable PDT efficacy that target mitochondrial DNA in cancer cells are reported. The metallohelices are fabricated using dynamic imine-coupling chemistry between aldehyde end-capped fac-Ir(ppy)3 handles and linear alkanediamine spacers, followed by reduction of the imine linkages. The length and odd-even character of the diamine alkyl linker determined the stereochemistry (helicates vs. mesocates). Compared to the helicates, the mesocates exhibit improved apoptosis-induction upon white-light irradiation. Molecular docking studies indicate that the mesocate with a proper length of diamine spacers shows stronger affinity for the minor groove of DNA. This study highlights the potential of DNA-targeting IrIII -containing metallohelices as PDT agents.

Keywords: DNA recognition; IrIII complex; cancer; helical structures; photodynamic therapy.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Apoptosis / drug effects
  • Binding Sites
  • Cell Line, Tumor
  • Coordination Complexes / chemistry*
  • Coordination Complexes / metabolism
  • Coordination Complexes / pharmacology
  • Crystallography, X-Ray
  • DNA, Mitochondrial / chemistry*
  • DNA, Mitochondrial / metabolism
  • Humans
  • Iridium / chemistry*
  • Light
  • Microscopy, Confocal
  • Mitochondria / drug effects
  • Mitochondria / metabolism
  • Molecular Conformation
  • Molecular Docking Simulation
  • Reactive Oxygen Species / metabolism
  • Stereoisomerism

Substances

  • Coordination Complexes
  • DNA, Mitochondrial
  • Reactive Oxygen Species
  • Iridium