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

查看全文 作　　者：Weiqing [1]Xu;Yikun [2]Kang;Lei [1]Jiao;Yu [1]Wu;Hongye [1]Yan;Jinli [1]Li;Wenling [1]Gu;Weiyu [2]Song;Chengzhou [1]Zhu 高影响力作者 机构地区：[1]Key Laboratory of Pesticide and Chemical Biology of Ministry of Education,International Joint Research Center for Intelligent Biosensing Technology and Health,College of Chemistry,Central China Normal University,Wuhan 430079,People’s Republic of China;[2]State Key Laboratory of Heavy Oil Processing,China University of Petroleum,Beijing 102249,People’s Republic of China高影响力机构 出　　处：《Nano-Micro Letters》索引2020年第12卷第12期,共12页高影响力期刊 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. 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 challenges.Herein,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 activity.Notably,the functionalization of nitro can enhance the peroxidase(POD)-like activity of MIL-101(Fe),while the amino is poles apart.Theoretical 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 sites.Benefiting 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 activity.As 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−1.Moreover,the detection of organophosphorus pesticides was also achieved.This 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. 关 键 词：Nanozymes Metal–organic frameworks Atomically dispersed sites Peroxidase-like activity Biosensors
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