Diatomic active sites nanozymes:Enhanced peroxidase-like activity for dopamine and intracellular H2O2 detection  

作　　者：Shan Wang Zunfu Hu Qiulian Wei Huimin Zhang Weina Tang Yunqiang Sun Haiqiang Duan Zhichao Dai Qingyun Liu Xiuwen Zheng 

机构地区：[1]Key Laboratory of Functional Nanomaterials and Technology in Universities of Shandong,College of Chemistry and Chemical Engineering,Linyi University,Linyi 276000,China [2]School of Chemical and Biological Engineering,Shandong University of Science and Technology,Qingdao 266510,China [3]School of Materials Science and Engineering,Linyi University,Linyi 276000,China

出　　处：《Nano Research》2022年第5期4266-4273,共8页纳米研究（英文版）

基　　金：This work was supported by the National Natural Science Foundation of China(Nos.22075122,21971152,and 21804067);the Primary Research and Development Plan of Shandong Province(No.2019GSF108093);Shandong Province Natural Science Foundation(Nos.ZR2020QB170,ZR2020MB003,and ZR2019BB038)。

摘　　要：Considering intracellular hydrogen peroxide(H_(2)O_(2))plays pivotal roles in the regulation of serial biological processes,the in-situ detection of intracellular H2O2 has attracted an extensive attention.In the present work,an atomically dispersed diatomic active sites Nanozymes(FeN_(3)/PtN_(4)-single-atom nanozymes(SAzyme))was prepared exhibiting enhanced peroxidase-like activity.The obvious synergistic effect between Fe-Pt heteronuclear diatomic active sites was confirmed by series of characterization and density functional theory(DFT).The peroxidase-like activity of Fe-sites could be substantially enhanced by the bonded Pt-sites via the modulation effect.As a consequence,the gap between the d-band centre(εd)of Fe 3d orbitals and the Fermi energy level was narrowed and the electronic interaction could be strengthened,leading to a lower free energy barrier and a lower activation energy as well as fortified metal-O bonding in the kinetic pathway.Therefore,the constructed FeN3/PtN4-SAzyme exhibited higher peroxidase-like activity than that of FeN4-SAzyme.The FeN3/PtN4-SAzyme-assisted oxidation of 3,3',5,5'-tetramethylbenzidine(TMB)facilitated the colorimetric detection of dopamine(DA),an important biomolecule.The linear detection range and limit of detection(LOD)of DA and H_(2)O_(2) were 1-10 μM,0.01-1.0 mM and 0.109 μM,7.97 μM,respectively.In addition,the constructed SAzymes were also applied for the in-situ detection of intracellular H2O2,expanding the application scope of the newborn SAzymes.

关 键 词：single-atom nanozymes heteronuclear diatomic active sites peroxidase-like DOPAMINE intracellular H_(2)O_(2) 

分 类 号：O62[理学—有机化学]