Potent Ruthenium-Ferrocene Bimetallic Antitumor Antiangiogenic Agent That Circumvents Platinum Resistance: From Synthesis and Mechanistic Studies to In Vivo Evaluation in Zebrafish

J Med Chem. 2022 Dec 22;65(24):16353-16371. doi: 10.1021/acs.jmedchem.2c01174. Epub 2022 Dec 2.

Abstract

Emergence of resistance in cancer cells and dose-limiting side effects severely limit the widespread use of platinum (Pt) anticancer drugs. Multi-action hybrid anticancer agents that are constructed by merging two or more pharmacophores offer the prospect of circumventing issues of Pt drugs. Herein, we report the design, synthesis, and in-depth biological evaluation of a ruthenium-ferrocene (Ru-Fc) bimetallic agent [(η6-p-cymene)Ru(1,1,1-trifluoro-4-oxo-4-ferrocenyl-but-2-en-2-olate)Cl] and its five analogues. Along with aquation/anation chemistry, we evaluated the in vitro antitumor potency, Pt cross-resistance profile, and in vivo antiangiogenic properties. A structure activity analysis was performed to understand the impact of Fc, CF3, and p-cymene groups on the anticancer potency of the Ru-Fc hybrid. Finally, in addition to assessing cellular uptake and intracellular distribution, we demonstrated that the Ru-Fc hybrid binds to nucleophilic biomolecules and produces reactive oxygen species, which causes mitochondrial dysfunction and induces ER stress, leading to poly(ADP-ribose) polymerase-mediated necroptotic cell death.

Publication types

  • Research Support, Non-U.S. Gov't

MeSH terms

  • Angiogenesis Inhibitors / pharmacology
  • Animals
  • Antineoplastic Agents* / chemistry
  • Cell Line, Tumor
  • Coordination Complexes* / chemistry
  • Metallocenes
  • Platinum / chemistry
  • Platinum / pharmacology
  • Ruthenium* / chemistry
  • Ruthenium* / pharmacology
  • Zebrafish

Substances

  • 4-cymene
  • ferrocene
  • Metallocenes
  • Angiogenesis Inhibitors
  • Ruthenium
  • Platinum
  • Antineoplastic Agents
  • Coordination Complexes