Enhancing radiation-resistance and peroxidase-like activity of single-atom copper nanozyme via local coordination manipulation

文献类型： 外文期刊

第一作者： Wu, Jiabin

作者： Wu, Jiabin;Li, Beibei;Ye, Chengliang;Wang, Dingsheng;Li, Yadong;Zhu, Xianyu;Chang, Qingchao;Xiang, Huandong;Liang, Yan;Zhao, Yuliang;Zhu, Xianyu;Chang, Qingchao;Xiang, Huandong;Liang, Yan;Zhao, Yuliang;Zhu, Xianyu;Li, Qiqiang;Li, Qun;Huang, Liang;Fu, Qiang;Wang, Bingxue;Fu, Qiang;Wang, Shanshan;Xiang, Huandong;Zhao, Yuliang;Li, Yadong;Li, Yadong

作者机构：

期刊名称：NATURE COMMUNICATIONS （ 影响因子：14.7； 五年影响因子：16.1 ）

ISSN：

年卷期： 2024 年 15 卷 1 期

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收录情况： SCI

摘要： The inactivation of natural enzymes by radiation poses a great challenge to their applications for radiotherapy. Single-atom nanozymes (SAzymes) with high structural stability under such extreme conditions become a promising candidate for replacing natural enzymes to shrink tumors. Here, we report a CuN3-centered SAzyme (CuN3-SAzyme) that exhibits higher peroxidase-like catalytic activity than a CuN4-centered counterpart, by locally regulating the coordination environment of single copper sites. Density functional theory calculations reveal that the CuN3 active moiety confers optimal H2O2 adsorption and dissociation properties, thus contributing to high enzymatic activity of CuN3-SAzyme. The introduction of X-ray can improve the kinetics of the decomposition of H2O2 by CuN3-SAzyme. Moreover, CuN3-SAzyme is very stable after a total radiation dose of 500 Gy, without significant changes in its geometrical structure or coordination environment, and simultaneously still retains comparable peroxidase-like activity relative to natural enzymes. Finally, this developed CuN3-SAzyme with remarkable radioresistance can be used as an external field-improved therapeutics for enhancing radio-enzymatic therapy in vitro and in vivo. Overall, this study provides a paradigm for developing SAzymes with improved enzymatic activity through local coordination manipulation and high radioresistance over natural enzymes, for example, as sensitizers for cancer therapy. The inactivation of natural enzymes by radiation hinders their utility for radiotherapy. Here the authors report a single-atom copper nanozyme that can be utilized for enhanced radio-enzymatic therapy to resolve the crucial issues for the applications of natural enzymes.

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