4.8 Article

Pd-Single-Atom Coordinated Biocatalysts for Chem-/Sono-/Photo-Trimodal Tumor Therapies

Journal

ADVANCED MATERIALS
Volume 33, Issue 29, Pages -

Publisher

WILEY-V C H VERLAG GMBH
DOI: 10.1002/adma.202101095

Keywords

catalytic ROS generation; nanomedicines; porphyrin-based coordination polymer; single-atom biocatalysts; trimodal tumor therapy

Funding

  1. National Key R&D Program of China [2019YFA0110600, 2019YFA0110601]
  2. National Natural Science Foundation of China [82071938, 82001824, 82001829, 51903178, 81971622, 51803134]
  3. Science and Technology Project of Sichuan Province [2020YFH0087, 2020YJ0055, 2019YFS0219, 18YYJC1417]
  4. State Key Laboratory of Polymer Materials Engineering [sklpme2019-2-03]
  5. Fundamental Research Funds for the Central Universities, Thousand Youth Talents Plan
  6. Alexander von Humboldt Fellowship

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A novel and facile Pd-single-atom-coordinated porphyrin-based polymeric network for chem-/sono-/photo-trimodal tumor therapies has been designed, showing highly efficient biocatalytic sites and synergistic trimodal therapeutic effects in both in vitro and in vivo experiments.
The diversity, complexity, and heterogeneity of malignant tumor seriously undermine the efficiency of mono-modal treatment. Recently, multi-modal therapeutics with enhanced antitumor efficiencies have attracted increasing attention. However, designing a nanotherapeutic platform with uniform morphology in nanoscale that integrates with efficient chem-/sono-/photo-trimodal tumor therapies is still a great challenge. Here, new and facile Pd-single-atom coordinated porphyrin-based polymeric networks as biocatalysts, namely, Pd-Pta/Por, for chem-/sono-/photo-trimodal tumor therapies are designed. The atomic morphology and chemical structure analysis prove that the biocatalyst consists of atomic Pd-N coordination networks with a Pd-N-2-Cl-2 catalytic center. The characterization of peroxidase-like catalytic activities displays that the Pd-Pta/Por can generate abundant center dot OH radicals for chemodynamic therapies. The ultrasound irradiation or laser excitation can significantly boost the catalytic production of O-1(2) by the porphyrin-based sono-/photosensitizers to achieve combined sono-/photodynamic therapies. The superior catalytic production of center dot OH is further verified by density functional theory calculation. Finally, the corresponding in vitro and in vivo experiments have demonstrated their synergistic chem-/sono-/photo-trimodal antitumor efficacies. It is believed that this study provides new promising single-atom-coordinated polymeric networks with highly efficient biocatalytic sites and synergistic trimodal therapeutic effects, which may inspire many new findings in reactive oxygen species-related biological applications across broad therapeutics and biomedical fields.

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