Abstract
Reactive oxygen species (ROS) are closely related to innate and adaptive immune responses in tumor immunotherapy. ROS-mediated therapies show great hope in improving therapeutic efficacy by inducing immunogenic cell death. However, the efficiency is still limited by the poor ROS production rate. Herein, a ROS nanogenerator is designed to boost antitumor immunity, integrating with pH-dissociable Fe3+-gallic acid (Fe-GA) complex as the shell and photosensitizer (Chlorin e6, Ce6)-coupled lanthanide-doped luminescence nanoparticles (LnNPs) as the core. Upon near-infrared (NIR) light irradiation, LnNPs exhibit multiband upconversion emission from ultraviolet (UV) to visible (Vis) and downshifting emission in the promising second NIR imaging region (NIR-II, 1550 nm). Especially, the UV photons and reducing agent GA could respectively mediate the reduction of Fe3+, allowing more Fe2+ to participate in the Fenton reaction to generate hydroxyl radicals (•OH) for ferroptosis therapy (FT). Besides, the UV–Vis upconversion emission can activate the coupling photosensitizer-Ce6 to generate 1O2 for photodynamic therapy (PDT). Additionally, Fe-GA can serve as a photothermal therapy (PTT) agent; in turn, hyperthermia enhances ROS generation. Our rational-designed Ln@Fe NPs could not only enhance the synergistic antitumor efficiency by boosting ROS generation but also effectively inhibit tumor metastasis by activating strong antitumor immunity, providing a paradigm for imaging-guided cancer treatment.
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