Zhou Genxiu, Dong Qingrong, Li Zhi, Yang Feifei, Shen Xiaomei, Liu Quan, Fang Ge, Ge Cuicui
State Key Laboratory of Radiation Medicine and Protection, School for Radiological and Interdisciplinary Sciences (RAD-X) & Collaborative Innovation Center of Radiation Medicine of Jiangsu Higher Education Institutions, Soochow University, Suzhou 215123, China.
College of Medical Imaging, Shanxi Medical University, Taiyuan 030001, China.
Nanoscale. 2024 Nov 21;16(45):21039-21047. doi: 10.1039/d4nr02142h.
Atom engineering has been demonstrated to be an efficient strategy for optimizing the activities of Prussian blue analogue (PBA)-based nanozymes. Herein, using a series of metal atom-coordinated N PBAs as models, a mechanistic insight into the effect of substituted metal centers on the antioxidant activities of PBA-based nanozymes is provided for the first time. The PBAs exhibit substituted metal atom-dependent antioxidant activities and the optimal Cu-substituted PBAs can effectively protect cells from oxidative stress. Experimental characterization reveals that the effect of low redox potential significantly improves the catalytic antioxidant efficiency. Furthermore, theoretical calculations show that the catalytic activities are well related to the magnetic moment of the adjacent Fe site, which features a linear correlation with the energy barrier of the rate-determining step or adsorption energy of the substrate, respectively. This study may inspire further exploration of PBAs and shed light on the rational design of advanced antioxidant nanozymes.
原子工程已被证明是优化基于普鲁士蓝类似物（PBA）的纳米酶活性的有效策略。在此，以一系列金属原子配位的N-PBA为模型，首次对取代金属中心对基于PBA的纳米酶抗氧化活性的影响提供了机理见解。PBA表现出依赖于取代金属原子的抗氧化活性，最佳的铜取代PBA可以有效保护细胞免受氧化应激。实验表征表明，低氧化还原电位的影响显著提高了催化抗氧化效率。此外，理论计算表明，催化活性与相邻铁位点的磁矩密切相关，磁矩分别与速率决定步骤的能垒或底物的吸附能呈线性相关。本研究可能会激发对PBA的进一步探索，并为先进抗氧化纳米酶的合理设计提供启示。
