Tuning Atomically Dispersed Fe Sites in Metal–Organic Frameworks Boosts Peroxidase‑Like Activity for Sensitive Biosensing

作     者：Weiqing Xu Yikun Kang Lei Jiao Yu Wu Hongye Yan Jinli Li Wenling Gu Weiyu Song Chengzhou Zhu Weiqing Xu;Yikun Kang;Lei Jiao;Yu Wu;Hongye Yan;Jinli Li;Wenling Gu;Weiyu Song;Chengzhou Zhu

作者机构：Key Laboratory of Pesticide and Chemical Biology of Ministry of EducationInternational Joint Research Center for Intelligent Biosensing Technology and HealthCollege of ChemistryCentral China Normal UniversityWuhan 430079People’s Republic of China State Key Laboratory of Heavy Oil ProcessingChina University of PetroleumBeijing 102249People’s Republic of China 

出 版 物：《Nano-Micro Letters》 (纳微快报（英文版）)

年 卷 期：2020年第12卷第12期

页      面：392-403页

核心收录：

学科分类：07[理学] 070205[理学-凝聚态物理] 080202[工学-机械电子工程] 08[工学] 080501[工学-材料物理与化学] 0805[工学-材料科学与工程（可授工学、理学学位）] 0802[工学-机械工程] 0702[理学-物理学] 

基　　金：The authors gratefully acknowledge the financial support of the Fundamental Research Funds for the Central Universities(CCNU20TS013) the National Natural Science Foundation of China(No.21503273) the Program of Introducing Talents of Discipline to Universities of China(111 program,B17019)and the Recruitment Program of Global Youth Experts of China 

主　　题：Nanozymes Metal–organic frameworks Atomically dispersed sites Peroxidase-like activity Biosensors 

摘      要：Although nanozymes have been widely developed,accurate design of highly active sites at the atomic level to mimic the electronic and geometrical structure of enzymes and the exploration of underlying mechanisms still face significant ***,two functional groups with opposite electron modulation abilities(nitro and amino)were introduced into the metal–organic frameworks(MIL-101(Fe))to tune the atomically dispersed metal sites and thus regulate the enzymelike ***,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles *** calculations demonstrate that the introduction of nitro can not only regulate the geometry of adsorbed intermediates but also improve the electronic structure of metal active *** from both geometric and electronic effects,the nitro-functionalized MIL-101(Fe)with a low reaction energy barrier for the HO*formation exhibits a superior POD-like *** a concept of the application,a nitro-functionalized MIL-101(Fe)-based biosensor was elaborately applied for the sensitive detection of acetylcholinesterase activity in the range of 0.2–50 mU mL−1 with a limit of detection of 0.14 mU mL−***,the detection of organophosphorus pesticides was also *** work not only opens up new prospects for the rational design of highly active nanozymes at the atomic scale but also enhances the performance of nanozyme-based biosensors.