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

Jiabin Wu, Xianyu Zhu, Qun Li, Qiang Fu (), Bingxue Wang, Beibei Li, Shanshan Wang, Qingchao Chang, Huandong Xiang, Chengliang Ye, Qiqiang Li, Liang Huang, Yan Liang (), Dingsheng Wang, Yuliang Zhao and Yadong Li ()
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Jiabin Wu: Tsinghua University
Xianyu Zhu: Chinese Academy of Sciences
Qun Li: Huazhong University of Science and Technology
Qiang Fu: University of Science and Technology of China
Bingxue Wang: University of Science and Technology of China
Beibei Li: Tsinghua University
Shanshan Wang: Chinese Academy of Agricultural Sciences
Qingchao Chang: Chinese Academy of Sciences
Huandong Xiang: Chinese Academy of Sciences
Chengliang Ye: Tsinghua University
Qiqiang Li: Shandong University
Liang Huang: Huazhong University of Science and Technology
Yan Liang: Chinese Academy of Sciences
Dingsheng Wang: Tsinghua University
Yuliang Zhao: Chinese Academy of Sciences
Yadong Li: Tsinghua University

Nature Communications, 2024, vol. 15, issue 1, 1-14

Abstract: Abstract 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.

Date: 2024
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DOI: 10.1038/s41467-024-50416-8

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