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洋葱状碳纳米酶:通过碳杂化模式控制类过氧化物酶活性用于抗菌治疗

Onion-Like Carbon Nanozyme: Controlling Peroxidase-Like Activity by Carbon Hybridization Patterns for Antibacterial Therapy.

作者信息

Shi Yuxi, Zheng Xiangyun, Zhao Qi, Feng Yuchen, Zhang Hanxin, Gao Guanyue, Wang Hao, Zhi Jinfang

机构信息

Key Laboratory of Photochemical Conversion and Optoelectronic Materials, Technical Institute of Physics and Chemistry, Chinese Academy of Sciences, Beijing, 100190, P. R. China.

University of Chinese Academy of Sciences, Beijing, 100049, P. R. China.

出版信息

Small. 2024 Dec;20(50):e2405577. doi: 10.1002/smll.202405577. Epub 2024 Oct 2.

Abstract

Since the inception of the concept of nanozymes, there has been a growing interest in the rational design and controllable synthesis of nanozymes with adjustable activities. In this study, onion-liked carbon (OLC) with remarkable peroxidase-like (POD) activity are developed through delicately controlling the sp/sp configuration. The investigation reveals that enzymatic activity of OLC increases first and then decreases with the increased graphitic degree, with the highest activity observed at a moderate sp/sp ratio of 17.17%. A series of experiments and theoretical calculations are conducted to elucidate the catalytic mechanism, and the structure-dependent activity is attributed to a synergistic effect of surface adsorption and electron transfer processes. The POD activity enables the OLC to catalyze the decomposition of HO, producing reactive oxygen species for eradicating Gram-positive and Gram-negative bacteria. Additionally, toxicity tests based on nematode and mouse models confirmed the excellent biocompatibility of OLC. Furthermore, the OLC exhibited antibacterial ability and promoted bacterial-infected wound healing in a mouse model. This work not only gives a deeper understanding of the structure-activity relationship and catalytic mechanism of carbon-based nanozymes, but also unveils a novel avenue for antibacterial therapy and wound healing applications.

摘要

自从纳米酶的概念诞生以来,人们对合理设计和可控合成具有可调活性的纳米酶的兴趣与日俱增。在本研究中,通过精细控制sp/sp构型,制备出了具有显著过氧化物酶样(POD)活性的洋葱状碳(OLC)。研究表明,随着石墨化程度的增加,OLC的酶活性先升高后降低,在17.17%的适度sp/sp比时观察到最高活性。进行了一系列实验和理论计算以阐明催化机制,结构依赖性活性归因于表面吸附和电子转移过程的协同作用。POD活性使OLC能够催化HO的分解,产生活性氧以根除革兰氏阳性菌和革兰氏阴性菌。此外,基于线虫和小鼠模型的毒性测试证实了OLC具有优异的生物相容性。此外,在小鼠模型中,OLC表现出抗菌能力并促进了细菌感染伤口的愈合。这项工作不仅使人们对碳基纳米酶的构效关系和催化机制有了更深入的了解,还为抗菌治疗和伤口愈合应用开辟了一条新途径。

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