首页|MOFs衍生的Fe-N-C纳米酶用于对苯二酚的比色检测

MOFs衍生的Fe-N-C纳米酶用于对苯二酚的比色检测

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[目的]建立-种方便的检测对苯二酚(hydroquinone,HQ)的方法.[方法]采用化学掺杂法合成Fe-ZIF-8前驱体,对前驱体热解处理,得到Fe-N-C纳米酶粉末;通过活性对比、自由基捕获和动力学实验,系统探究Fe-N-C的类酶活性;依据HQ具有还原性强、可将3,3',5,5'-四甲基联苯胺(TMB)显色体系还原为无色状态的特性,构建比色法检测HQ的传感平台.[结果]Fe-N-C表现出优异的过氧化物酶样活性,可以快速将显色底物TMB催化氧化为蓝色;Fe-Nx是Fe-N-C 主要的活性位点,羟基自由基(·OH)、超氧自由基(O2·-)和单线态氧(1O2)是起主要作用的活性氧;Fe-N-C纳米酶对TMB的亲和力优于天然辣根过氧化物酶,该方法检测HQ的线性范围为0~33 μmol/L,检测限为0.356 μmol/L,同时具有良好的抗干扰能力.[结论]构建一种用于环境分析的金属有机骨架化合物(metal organic framework,MOFs)衍生物纳米酶,可实现HQ的简单和灵敏检测.
MOFs-derived Fe-N-C nanozyme for colorimetric detection of hdroquinone
Objective Hydroquinone is a phenolic compound widely used in industry.It is difficult to degrade in the aquatic ecological envi-ronment and is harmful to human health.Therefore,constructing a simple and sensitive method for the detection of hydroqui-none is of great significant.Methods In this study,an MOFs-derived Fe-N-C catalyst was synthesized through a simple chemical doping method and high-temperature pyrolysis,using an Fe-ZIF-8 precursor.The physicochemical properties of Fe-N-C were characterized in detail through SEM,TEM,XRD,FTIR,and XPS.The effect of the introducing Fe3+on the enzyme activity of the catalyst was stud-ied.The enzyme-like activity,catalytic mechanism,and kinetic parameters of Fe-N-C were systematically investigated.Based on the enzyme-like activity of Fe-N-C,a colorimetric sensor for the detection of hydroquinone was developed.Results and Discussion Based on the aforementioned characterization and experimental findings,Fe-N-C exhibited excellent peroxidase-like activity and weak oxidase-like activity.In addition,in the presence of hydrogen peroxide,OPD and ABTS as substrates were also oxidized to yellow and blue products by Fe-N-C,with characteristic absorption peaks at 448 nm and 416 nm,respectively.Additionally,the poisoning experiment with KSCN showed that Fe-Nx was the main active site in Fe-N-C catalyst.The study of the catalytic mechanism confirmed that·OH,O2·-and 1O2 were active oxygen radicals playing a major role in the catalytic oxidation of TMB.The catalytic activity of Fe-N-C nanozymes was further studied through steady-state kinetic analysis.The Km and Vmax of Fe-N-C for TMB were 0.134 mmol/L and 0.754 × 10-7 M·s-1,respectively,while those for H2O2 were 16.535 mmol/L and 2.533 × 10-7 M·s-1,respectively.Finally,the colorimetric sensor detected HQ in a linear range of 0~33 μmol/L with a detection limit of 0.356 μmol/L.Through anti-interference experiments,the established colorimet-ric sensing platform showed robust anti-interference ability and selectivity in detecting hydroquinone.Conclusion The introduction of Fe3+significantly improves the enzyme-like activity of N-C nanomaterials.Fe-N-C exhibits excellent peroxidase-like activity,which can rapidly oxidize the chromogenic substrate 3,3',5,5'-tetramethylbenzidine(TMB)to blue.Fe-Nx is the main active site of Fe-N-C nanozymes,and hydroxyl radical(·OH),superoxide radicals(O2·-)and singlet oxygen(1O2)are the main reactive oxygen species(ROS).Hydroquinone is a strong reducing organic pollutant that can reduce blue oxTMB to a colorless state.Based on this,a sensing platform for colorimetric detection of HQ was constructed.This method has good sensitivity and selectivity for hydroquinone,which expands the application of MOFs-based nanozymes in the field of environmental pollutant detection.

nanozymemetal-organic frameworkcolorimetric detectionhydroquinone

张元杰、李金凯、刘宗明

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济南大学材料科学与工程学院,山东济南 250022

纳米酶 金属-有机骨架 比色检测 对苯二酚

国家自然科学基金项目山东省自然科学基金项目山东省自然科学基金项目济南市"新高校20条"基金项目济南市"新高校20条"基金项目

51402125ZR2020ME045ZR2020ME0462021GXRCO99T202204

2024

中国粉体技术
中国颗粒学会,济南大学,中国非金属矿工业协会矿物加工利用专业委员会

中国粉体技术

CSTPCD
影响因子:0.469
ISSN:1008-5548
年,卷(期):2024.30(4)