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具有过氧化物酶模拟活性的氮掺杂碳纳米酶中原子分散的铁-锰双位点用于硫氰酸盐的测定。

Atomically dispersed Fe-Mn dual sites in N-doped carbon nanozymes with peroxidase-mimetic activity for the determination of thiocyanate.

作者信息

Liang Huan, Wang Jia-Qi, Zhang Min, Sun Xiao-Dong, Wang Peng-Jiao, Zhang Shuo, Gao Xiu-Li

机构信息

State Key Laboratory of Discovery and Utilization of Functional Components in Traditional Chinese Medicine & School of Pharmaceutical Sciences, Guizhou Medical University, Guiyang, Guizhou, 561113, PR China.

Engineering Research Center of Microbiology and Biochemical Pharmaceutical, Guizhou Provincial Department of Education, Guiyang, Guizhou, 561113, PR China.

出版信息

Mikrochim Acta. 2025 Aug 5;192(9):556. doi: 10.1007/s00604-025-07400-w.

Abstract

FeMn dual-active-site single-atom catalyst (FeMn-N-C), featuring manganese-enhanced Fe-N-doped carbon with abundant FeMn-N4 and C-N active groups, was fabricated via hydrothermal synthesis followed by high-temperature pyrolysis. Thiocyanate (SCN⁻) can be adsorbed onto the FeMn-N-C surface by binding to Fe/Mn atoms, blocking the active sites of the mimic peroxidase and thereby inhibiting the corresponding chromogenic reaction of 3,3',5,5'-tetramethylbenzidine, achieving rapid and sensitive colorimetric detection of SCN⁻. Under optimal conditions, the established biosensor exhibited a linear range of 0.2-11 μmol L, with a detection limit of 66.7 nmol L. Experimental findings and theoretical calculations demonstrated that the superior activity of FeMn-N-C stemmed from the synergistic effect of the dual atoms, which boosted substrate adsorption and reduced the reaction barrier. This strategy provided mechanistic insights into the rational design of advanced nanozymes, highlighting their potential for food safety and environmental monitoring applications.

摘要

通过水热合成法,随后进行高温热解,制备了具有锰增强的铁氮掺杂碳、富含FeMn-N4和C-N活性基团的铁锰双活性位点单原子催化剂(FeMn-N-C)。硫氰酸盐(SCN⁻)可以通过与铁/锰原子结合吸附在FeMn-N-C表面,阻断模拟过氧化物酶的活性位点,从而抑制3,3',5,5'-四甲基联苯胺的相应显色反应,实现对SCN⁻的快速灵敏比色检测。在最佳条件下,所建立的生物传感器线性范围为0.2-11 μmol/L,检测限为66.7 nmol/L。实验结果和理论计算表明,FeMn-N-C的优异活性源于双原子的协同效应,这促进了底物吸附并降低了反应势垒。该策略为先进纳米酶的合理设计提供了机理见解,突出了其在食品安全和环境监测应用中的潜力。

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