Li Jing, Zhang Meng, Wang Yueyue, Lv Wenxin, Xu Ziran, Wang Bibi, Huang Rongqin, Mei Bingbao, Wang Yi
Center for Advanced Low-Dimension Materials, State Key Laboratory for Modification of Chemical Fibers and Polymer Materials, College of Chemistry, Chemical Engineering, Donghua University, Shanghai 201600, China.
School of Pharmacy, Key Laboratory of Smart Drug Delivery, Ministry of Education, Fudan University, Shanghai 201203, China.
ACS Nano. 2024 Dec 31;18(52):35606-35619. doi: 10.1021/acsnano.4c13899. Epub 2024 Dec 17.
Creating simple methods to produce antioxidant nanozymes with clear structure-activity relationships, particularly aiming to improve disinfection and create practical drug formulations for bacterial wound healing, remains a crucial challenge. Herein, we synthesized iron-loaded covalent organic framework nanospheres, which were then controllably transformed into a carbon-based nanozyme with both iron single atoms and iron clusters through simple pyrolysis. We discovered that the gradual growth of iron clusters significantly boosted the nanozyme's adsorption onto the substrate and electron transfer, greatly influencing its activity. The nanozyme, optimized by the coexistence of single iron atoms and Fe clusters, exhibited the strongest catalase and superoxide dismutase enzyme activities as well as high photothermal efficiency. Under physiological conditions, its peroxidase and oxidase enzymatic activities, which stimulate oxidative stress, remained low. Furthermore, we created an antibacterial self-gelling powder capable of dispersing the nanozyme using polyacrylamide and poly(acrylic acid). The powder can rapidly gel and adhere to wet wound areas, synergistically sterilizing the wound through the combined actions of the gel's amino groups and the nanozyme's photothermal effect, while leveraging the antioxidant enzymatic effects to mitigate wound inflammation. These properties contribute to the fast healing of infectious wounds, thus promising a clear formulation and treatment.
创建具有明确构效关系的抗氧化纳米酶的简单方法,特别是旨在改善消毒效果并为细菌性伤口愈合创建实用的药物制剂,仍然是一项关键挑战。在此,我们合成了负载铁的共价有机框架纳米球,然后通过简单的热解将其可控地转化为具有铁单原子和铁簇的碳基纳米酶。我们发现铁簇的逐渐生长显著增强了纳米酶对底物的吸附和电子转移,极大地影响了其活性。通过单铁原子和铁簇共存优化的纳米酶表现出最强的过氧化氢酶和超氧化物歧化酶活性以及高光热效率。在生理条件下,其刺激氧化应激的过氧化物酶和氧化酶活性仍然很低。此外,我们使用聚丙烯酰胺和聚丙烯酸创建了一种能够分散纳米酶的抗菌自凝胶粉末。该粉末可以迅速凝胶化并粘附在湿伤口区域,通过凝胶的氨基和纳米酶的光热效应的联合作用协同对伤口进行消毒,同时利用抗氧化酶效应减轻伤口炎症。这些特性有助于感染性伤口的快速愈合,因此有望实现明确的配方和治疗方法。