Biocompatible Ruthenium Single-Atom Catalyst for Cascade Enzyme-Mimicking Therapy

ACS Appl Mater Interfaces. 2021 Sep 29;13(38):45269-45278. doi: 10.1021/acsami.1c12706. Epub 2021 Sep 14.

Abstract

Rationally constructing single-atom enzymes (SAEs) with superior activity, robust stability, and good biocompatibility is crucial for tumor therapy but still remains a substantial challenge. In this work, we adopt biocompatible carbon dots as the carrier material to load Ru single atoms, achieving Ru SAEs with superior multiple enzyme-like activity and stability. Ru SAEs behave as oxidase, peroxidase, and glutathione oxidase mimics to synchronously catalyze the generation of reactive oxygen species (ROS) and the depletion of glutathione, thus amplifying the ROS damage and finally causing the death of cancer cells. Notably, Ru SAEs exhibit excellent peroxidase-like activity with a specific activity of 7.5 U/mg, which surpasses most of the reported SAEs and is 20 times higher than that of Ru/C. Theoretical results reveal that the electrons of the Ru 4d orbital in Ru SAEs are transferred to O atoms in H2O2 and then efficiently activate H2O2 to produce OH. Our work may provide some inspiration for the design of SAEs for cancer therapy.

Keywords: ROS damage; carbon dots; multienzyme-mimicking activities; ruthenium; single-atom enzyme.

MeSH terms

  • Animals
  • Antineoplastic Agents / chemistry
  • Antineoplastic Agents / therapeutic use*
  • Apoptosis / drug effects
  • Carbon / chemistry
  • Catalysis
  • Cell Line, Tumor
  • Glutathione / metabolism
  • Hydrogen Peroxide / chemistry
  • Hydrogen Peroxide / metabolism
  • Kinetics
  • Mice
  • Neoplasms / drug therapy*
  • Oxidation-Reduction
  • Oxidative Stress / drug effects
  • Quantum Dots / chemistry
  • Quantum Dots / therapeutic use*
  • Ruthenium / chemistry
  • Ruthenium / therapeutic use*

Substances

  • Antineoplastic Agents
  • Carbon
  • Ruthenium
  • Hydrogen Peroxide
  • Glutathione