A Fluorinated BODIPY-Based Zirconium Metal–Organic Framework for In Vivo Enhanced Photodynamic Therapy

光动力疗法 化学 紧身衣 体内 肿瘤缺氧 金属有机骨架 缺氧(环境) 体内分布 氧气 组合化学 光化学 癌症研究 有机化学 体外 生物化学 放射治疗 荧光 吸附 生物技术 内科学 物理 生物 医学 量子力学
作者
Xu Chen,Bárbara B. Mendes,Yunhui Zhuang,João Conniot,Sergio Mercado Argandona,Francesca Melle,Diana P. Sousa,David Perl,Alexandru Chivu,Hirak K. Patra,William Shepard,João Conde,David Fairen‐Jimenez
出处
期刊:Journal of the American Chemical Society [American Chemical Society]
卷期号:146 (2): 1644-1656 被引量:41
标识
DOI:10.1021/jacs.3c12416
摘要

Photodynamic therapy (PDT), an emergent noninvasive cancer treatment, is largely dependent on the presence of efficient photosensitizers (PSs) and a sufficient oxygen supply. However, the therapeutic efficacy of PSs is greatly compromised by poor solubility, aggregation tendency, and oxygen depletion within solid tumors during PDT in hypoxic microenvironments. Despite the potential of PS-based metal–organic frameworks (MOFs), addressing hypoxia remains challenging. Boron dipyrromethene (BODIPY) chromophores, with excellent photostability, have exhibited great potential in PDT and bioimaging. However, their practical application suffers from limited chemical stability under harsh MOF synthesis conditions. Herein, we report the synthesis of the first example of a Zr-based MOF, namely, 69-L2, exclusively constructed from the BODIPY-derived ligands via a single-crystal to single-crystal post-synthetic exchange, where a direct solvothermal method is not applicable. To increase the PDT performance in hypoxia, we modify 69-L2 with fluorinated phosphate-functionalized methoxy poly(ethylene glycol). The resulting 69-L2@F is an oxygen carrier, enabling tumor oxygenation and simultaneously acting as a PS for reactive oxygen species (ROS) generation under LED irradiation. We demonstrate that 69-L2@F has an enhanced PDT effect in triple-negative breast cancer MDA-MB-231 cells under both normoxia and hypoxia. Following positive results, we evaluated the in vivo activity of 69-L2@F with a hydrogel, enabling local therapy in a triple-negative breast cancer mice model and achieving exceptional antitumor efficacy in only 2 days. We envision BODIPY-based Zr-MOFs to provide a solution for hypoxia relief and maximize efficacy during in vivo PDT, offering new insights into the design of promising MOF-based PSs for hypoxic tumors.
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