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红光调控光氧化还原催化实现自报告型一氧化氮释放用于高效抗菌治疗。

Red-Light-Mediated Photoredox Catalysis Enables Self-Reporting Nitric Oxide Release for Efficient Antibacterial Treatment.

机构信息

CAS Key Laboratory of Soft Matter Chemistry, Hefei National Laboratory for Physical Science at the Microscale, Department of Polymer Science and Engineering, University of Science and Technology of China, Hefei, 230026, Anhui, China.

出版信息

Angew Chem Int Ed Engl. 2021 Sep 6;60(37):20452-20460. doi: 10.1002/anie.202107155. Epub 2021 Aug 6.

DOI:10.1002/anie.202107155
PMID:34196472
Abstract

Nitric oxide (NO) serves as a key regulator of many physiological processes and as a potent therapeutic agent. The local delivery of NO is important to achieve target therapeutic outcomes due to the toxicity of NO at high concentrations. Although light stimulus represents a non-invasive tool with spatiotemporal precision to mediate NO release, many photoresponsive NO-releasing molecules can only respond to ultraviolet (UV) or near-UV visible light with low penetration and high phototoxicity. We report that coumarin-based NO donors with maximal absorbances at 328 nm can be activated under (deep) red-light (630 or 700 nm) irradiation in the presence of palladium(II) tetraphenyltetrabenzoporphyrin, enabling stoichiometric and self-reporting NO release with a photolysis quantum yield of 8 % via photoredox catalysis. This NO-releasing platform with ciprofloxacin loading can eradicate Pseudomonas aeruginosa biofilm in vitro and treat cutaneous abscesses in vivo.

摘要

一氧化氮 (NO) 作为许多生理过程的关键调节剂和有效的治疗剂。由于高浓度的 NO 具有毒性,因此局部递送 NO 对于实现靶向治疗效果很重要。尽管光刺激是一种具有时空精度的非侵入性工具,可以介导 NO 的释放,但许多光响应型 NO 释放分子只能响应紫外线 (UV) 或近 UV 可见光,这些光的穿透能力低且具有高细胞毒性。我们报告说,在钯 (II) 四苯基四苯并卟啉存在下,最大吸收波长为 328nm 的香豆素基一氧化氮供体可以在(深)红光(630 或 700nm)照射下被激活,从而通过光还原催化实现化学计量比和自报告的一氧化氮释放,光解量子产率为 8%。这种带有环丙沙星负载的一氧化氮释放平台可以在体外消灭铜绿假单胞菌生物膜,并在体内治疗皮肤脓肿。

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