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Oxygen-Regenerative NIR Aza-BODIPY Photosensitizers for Hypoxia-Tolerant Photodynamic Therapy
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DOI：10.1002/adma.74272.png)
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Abstract
En 中文
Near-infrared (NIR) photosensitizers (PSs) capable of producing cytotoxic reactive oxygen species (ROS) via oxygen-engaged electron- and energy-transfer pathways under excitation beyond 800 nm are highly attractive for deep-tissue photodynamic therapy (PDT). However, their ROS generation is fundamentally limited by the low photon energy of long-wavelength excitation and the hypoxic tumor microenvironment. Herein, we report three oxygen-regenerative NIR aza-BODIPY PSs for efficient hypoxia-tolerant PDT under 808 nm excitation. Mechanistic studies identify PS radical-ion pairs as the key intermediates that couple water oxidation-driven in situ O2/proton (H+) generation with downstream oxygen reduction to enable efficient hypoxia-tolerant •OH production. In parallel, efficient H+ generation and strong H+ affinity of the target PS (NJ853) promote H+-engaged oxygen photoreduction, affording a ∼56-fold enhancement in •OH generation compared with commercial PS indocyanine green (ICG). This hypoxia-tolerant intracellular ROS generation enables NJ853@NPs to induce apoptosis-dominant cancer cell killing and superior in vivo PDT efficacy under 808 nm irradiation. This work establishes an oxygen-regenerative photoredox pathway for NIR PSs, opening a new avenue to overcome the longstanding hypoxia limitation in deep-tissue PDT.
Keywords:
aza-BODIPY
excited state
NIR-II photosensitizers
photodynamic therapy
reactive oxygen species
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