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<p>Single-atom nanozymes (SANzymes) with multi-mimetic activities capable of altering the cellular redox balance demonstrate significant potential in tumor therapy. However, the catalytic treatment provided by SANzymes alone is insufficient to achieve optimal outcomes. Therefore, the combination of nanozyme catalysis with drug therapy is considered a promising alternative. Nonetheless, the leakage of drug molecules is a primary cause of chemotherapy resistance in cancer treatment. Consequently, developing novel drug immobilization methods to attach them to SANzymes is expected to enable multimodal synergistic therapy. Herein, a multifunctional nanoplatform is designed by modifying bioinspired PDA on iron-based SANzyme (Fe SANzyme) and immobilizing doxorubicin (DOX) through Michael addition/Schiff base reaction, which greatly promotes the drug loading efficiency. The Fe SAN-PDA@DOX@HA displays controllable drugs release behavior in the tumor microenvironment (TME), where the Fe SAN-PDA nanozyme can catalyze high level of H<sub>2</sub>O<sub>2</sub> to produce oxygen to alleviate hypoxia, convert H<sub>2</sub>O<sub>2</sub> to the toxic reactive oxygen species (ROS), and deplete intracellular glutathione via the catalase (CAT), peroxidase (POD), and glutathione oxidase (GSHOx)-like activities, respectively. The high drug loading, exceptional nanozyme catalysis, combined with the good photothermal performance of Fe SAN-PDA, resulted in sustained chemodynamic/photothermal/chemotherapy in a mouse mammary carcinoma model. The results reveal the synergistic antitumor potential of the novel conjugation of DOX on Fe SANzyme via PDA, offering a strategy for drug immobilization, TME remodeling and synergistic multimodal therapy.</p>

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Covalent conjugation of doxorubicin to polydopamine on the surface of single-atom nanozyme for effective synergistic cancer therapy

  • 期刊论文

  • 发表日期：

    2025年4月23日

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  • Jing Liu,
  • Minjuan Wang,
  • Xing Yang,
  • Haoyu Chen,
  • Mingjie Wei,
  • Xiaohua Zhu,
  • Youyu Zhang,
  • Meiling Liu,
  • Shouzhuo Yao

摘要

Single-atom nanozymes (SANzymes) with multi-mimetic activities capable of altering the cellular redox balance demonstrate significant potential in tumor therapy. However, the catalytic treatment provided by SANzymes alone is insufficient to achieve optimal outcomes. Therefore, the combination of nanozyme catalysis with drug therapy is considered a promising alternative. Nonetheless, the leakage of drug molecules is a primary cause of chemotherapy resistance in cancer treatment. Consequently, developing novel drug immobilization methods to attach them to SANzymes is expected to enable multimodal synergistic therapy. Herein, a multifunctional nanoplatform is designed by modifying bioinspired PDA on iron-based SANzyme (Fe SANzyme) and immobilizing doxorubicin (DOX) through Michael addition/Schiff base reaction, which greatly promotes the drug loading efficiency. The Fe SAN-PDA@DOX@HA displays controllable drugs release behavior in the tumor microenvironment (TME), where the Fe SAN-PDA nanozyme can catalyze high level of H2O2 to produce oxygen to alleviate hypoxia, convert H2O2 to the toxic reactive oxygen species (ROS), and deplete intracellular glutathione via the catalase (CAT), peroxidase (POD), and glutathione oxidase (GSHOx)-like activities, respectively. The high drug loading, exceptional nanozyme catalysis, combined with the good photothermal performance of Fe SAN-PDA, resulted in sustained chemodynamic/photothermal/chemotherapy in a mouse mammary carcinoma model. The results reveal the synergistic antitumor potential of the novel conjugation of DOX on Fe SANzyme via PDA, offering a strategy for drug immobilization, TME remodeling and synergistic multimodal therapy.