Accurate regulation of carbon skeletons bonded to Fe-N_(4)single atom nanozymes for efficient generation of reactive oxygen species  

作　　者：Fuchun Nan Qilin Wei Tongtong Kou Yuxuan Zhao Lanbo Shen Dawei Li Tong Chang Lingyun Wang Fangfang Lang William W.Yu 

机构地区：[1]School of Chemistry and Chemical Engineering,Ministry of Education Key Laboratory of Special Functional Aggregated Materials,Shandong Key Laboratory of Advanced Organosilicon Materials and Technologies,Shandong University,Jinan 250100,China [2]Shandong Provincial Key Laboratory for Science of Material Creation and Energy Conversion,Science Center for Material Creation and Energy Conversion,Shandong University,Qingdao 266237,China [3]Department of Urology,Qilu Hospital of Shandong University,Jinan 250063,China [4]Jinan Central Hospital,Shandong First Medical University,Jinan 250013,China [5]School of Integrated Circuits,Shandong University,Jinan 250101,China [6]Shandong Provincial Maternal and Child Health Care Hospital,Qingdao University,Jinan 250014,China

出　　处：《Science China Chemistry》2025年第3期1067-1077,共11页中国科学(化学英文版)

基　　金：financially supported by the Natural Science Foundation of China (62374104);the Jinan Central Hospital (1190022050);the Shandong Provincial Natural Science Foundation (ZR2023QE322 and ZR2022QH069)。

摘　　要：Rational design of single atom nanozymes(SAzymes)could be achieved through the accurate configuration regulation of metal coordination sites,nevertheless,the un-defined carbon environment of traditional SAzymes synthesized by high-temperature pyrolysis makes it difficult to unveil the influence of carbon skeletons with enzyme mimicking activities of SAzymes.Herein,we investigated the relationship between the carbon skeletons and the enzyme mimicking activities through the construction of a series of fullyπ-conjugated covalent organic polymer(COP)-based SAzymes with analogous Fe-N_(4)sites.The experimental results and theoretical calculations demonstrated that carbon skeletons bonded to the Fe-N_(4)catalytic sites strongly affect the enzyme mimicking activities of COP SAzymes.When the number of benzene rings in carbon skeletons was 1,the COP SAzyme possessed much more remarkable oxidase(OXD)and peroxidase(POD)mimicking activities,and further reducing or increasing the benzene rings would dramatically inhibit the enzyme mimicking activity.Additionally,the fantastic enzyme mimicking activity of COP-1 could be applied to colorimetric detection of biological molecules and degradation of pollutants.These results provide a new perspective for the rational fabrication of SAzymes with high catalytic efficiency.

关 键 词：single atom nanozyme covalent organic polymer carbon skeleton reactive oxygen species generation 

分 类 号：TQ426[化学工程] TB383.1[一般工业技术—材料科学与工程]