Fe/Mn Bimetal-Doped ZIF-8-Coated Luminescent Nanoparticles with Up/Downconversion Dual-Mode Emission for Tumor Self-Enhanced NIR-II Imaging and Catalytic Therapy

作者：Chunsheng Li, Jin Ye, Xing Yang, Shuang Liu, Zhiyong Zhang, Jun Wang, Kefen Zhang, Jiating Xu, Yujie Fu, Piaoping Yang · 发表于：ACS Nano · 年份：2022 · DOI：10.1021/acsnano.2c05152 · 被引用次数：166 · 研究领域：Nanoplatforms for cancer theranostics、Luminescence Properties of Advanced Materials、Luminescence and Fluorescent Materials

ZIF-8, as an important photoresponsive metal–organic framework (MOF), holds great promise in the field of cancer theranostics owing to its versatile physiochemical properties. However, its photocatalytic anticancer application is still restricted because of the wide bandgap and specific response to ultraviolet light. Herein, we developed lanthanide-doped nanoparticles (LDNPs) coated with Fe/Mn bimetal-doped ZIF-8 (LDNPs@Fe/Mn-ZIF-8) for second near-infrared (NIR-II) imaging-guided synergistic photodynamic/chemodynamic therapy (PDT/CDT). The LDNPs were synthesized by encapsulating an optimal Yb 3+ /Ce 3+ -doped active shell on the NaErF 4:Tm core to achieve dual-mode red upconversion (UC) and NIR-II downconversion (DC) emission upon NIR laser irradiation. At the optimal doping concentration, the UC and DC NIR-II emission intensities of LDNPs were increased 30.2- and 13.2-fold above those of core nanoparticles, which endowed LDNPs@Fe/Mn-ZIF-8 with an outstanding capability to carry out UC-mediated PDT and NIR-II optical imaging. In addition, the dual doping of Fe 2+ /Mn 2+ markedly decreased the bandgap of the ZIF-8 photosensitizer from 5.1 to 1.7 eV, expanding the excitation threshold of ZIF-8 to the visible light region (∼650 nm), which enabled Fe/Mn-ZIF-8 to be efficiently excited by UC photons to achieve photocatalytic-driven PDT. Furthermore, Fe 2+ /Mn 2+ ions could be responsively released in the tumor microenvironment through degradation of Fe/Mn-ZIF-8, thereby producing...