氧化石墨烯/富勒烯复合材料增敏多金属离子印迹电化学传感器
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摘要
制备了一种对Pb(Ⅱ)、Cd(Ⅱ)和Cu(Ⅱ)等多金属离子具有灵敏、选择性响应的新型印迹传感器。以甲基丙烯酸与乙二胺四乙酸分别为功能单体与配体,乙二醇二甲基丙烯酸酯为交联剂制备出多金属离子印迹聚合物。采用滴涂法将离子印迹聚合物均匀地修饰至氧化石墨烯/富勒烯复合材料修饰碳电极表面,成功制备出灵敏的多金属离子印迹电化学传感器。采取循环伏安法、交流阻抗和差分脉冲法等技术对印迹电化学传感器的性能进行表征,结果表明该多金属离子印迹电化学传感器具有良好的选择性。在1. 0×10~(-9)～5. 0×10~(-7)mol/L范围内,该多金属离子印迹电极的响应电流与金属离子浓度呈现良好的线性关系,对Pb(Ⅱ)、Cd(Ⅱ)和Cu(Ⅱ)金属离子的最低检测限分别为5. 0×10~(-10)、5. 0×10~(-10)和1. 0×10~(-10)mol/L。该多金属离子印迹电化学传感器成功用于实际样品中微量Pb(Ⅱ)、Cd(Ⅱ)和Cu(Ⅱ)等金属离子的检测。
A novel multiple-ion imprinted sensor based on graphene oxide/fullerene composite( GO-C60) was developed for simultaneous and selective determination of Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ). The multiple-ion imprinted polymer was prepared with methacrylic acid and edetic acid as the functional monomer and ligand,respectively. The multiple-ion imprinted sensor was prepared by dispensing the imprinted polymer onto the GO-C60 modified carbon electrode surface. The performance of multiple-ion imprinted sensor was investigated using cyclic voltammetry, differential pulse voltammetry and electrochemical impedance spectroscopy in details. Under the optimized conditions,a linear relationship existed between the response currents of the multiple-ion imprinted sensor and the negative logarithm of ion concentrations ranging from 1. 0 × 10~(-9) mol/L to 5. 0 × 10~(-7) mol/L with the detection limit of 5. 0 × 10~(-10),5. 0 × 10~(-10) and 1. 0 × 10~(-10) mol/L for Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ),respectively. The multiple-ion imprinted sensor was successfully used for simultaneous detection of trace level Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ) ions in real samples.
A novel multiple-ion imprinted sensor based on graphene oxide/fullerene composite( GO-C60) was developed for simultaneous and selective determination of Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ). The multiple-ion imprinted polymer was prepared with methacrylic acid and edetic acid as the functional monomer and ligand,respectively. The multiple-ion imprinted sensor was prepared by dispensing the imprinted polymer onto the GO-C60 modified carbon electrode surface. The performance of multiple-ion imprinted sensor was investigated using cyclic voltammetry, differential pulse voltammetry and electrochemical impedance spectroscopy in details. Under the optimized conditions,a linear relationship existed between the response currents of the multiple-ion imprinted sensor and the negative logarithm of ion concentrations ranging from 1. 0 × 10~(-9) mol/L to 5. 0 × 10~(-7) mol/L with the detection limit of 5. 0 × 10~(-10),5. 0 × 10~(-10) and 1. 0 × 10~(-10) mol/L for Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ),respectively. The multiple-ion imprinted sensor was successfully used for simultaneous detection of trace level Pb( Ⅱ),Cd( Ⅱ) and Cu( Ⅱ) ions in real samples.
引文
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[15]Kokkios C,Economou A,Raptis I,et al. Lithographically Fabricated Disposable Bismuth-Film Electrodes for the Trace Determination of Pb(Ⅱ)and Cd(Ⅱ)by Anodic Stripping Voltammetry[J]. Electrochim Acta,2008,53(2):5294-5299.
[16]Hummers W S,Offeman R E. Functionalized Graphene and Graphene Oxide:Materials Synthesis and Electronic Applications[J]. J Am Chem Soc,1958,80:1339-1339.
[17]Zhang Z H,Yang X,Zhang H B,et al. Novel Molecularly Imprinted Polymers Based on Multi-Walled Carbon Nanotubes with Binary Functional Monomer for the Solid-Phase Extraction of Erythromycin from Chicken Muscle[J]. J Chromatogr B,2011,879:1617-1624.
[2]Yu J,Yang S,Sun D. Simultaneously Determination of Multi Metal Elements in Water Samples by Liquid Cathode Glow Discharge-Atomic Emission Spectrometry[J]. Microchem J,2016,128:325-330.
[3]Boutorabi L,Rajabi M,Bazregar M,et al. Selective Determination of Chromium(Ⅵ)Ions Using In-Tube Electro-Membrane Extraction Followed by Flame Atomic Absorption Spectrometry[J]. Microchem J,2017,132:378-384.
[4]Silva F L,Duarte T A,Melo L S,et al. Development of a Wet Digestion Method for Paints for the Determination of Metals and Metalloids Using Inductively Coupled Plasma Optical Emission Spectrometry[J]. Talanta,2016,146(4/5):188-194.
[5]Jalalvand A R,Goicoechea H C,Rutledge D N,et al. Applications and Challenges of Multi-way Calibration in Electrochemical Analysis[J]. Tr AC-Trend Anal Chem,2017,87:32-48.
[6] ZHANG Minglei,ZHANG Zhaohui,LUO Lijuan,et al. Preparation and Adsorption Properties of Magnetic Fe3O4@Si O2@CS Cadmium Ion-Imprinted Polymer[J]. Chem J Chinese Univ,2011,32(12):2763-2768(in Chinese).张明磊,张朝晖,罗丽娟,等.磁性Fe3O4@Si O2@CS镉离子印迹聚合物研制及其吸附性能研究[J].高等学校化学学报,2011,32(12):2763-2768.
[7]LIU Qiuye,HE Xiwen,LI Wenyou,et al. Studies on Chitosan Coated on Silica for Imprinting Bovine Hemoglobin[J].Chem J Chinese Univ,2009,30(4):691-696(in Chinese).刘秋叶,何锡文,李文友,等.壳聚糖包裹硅胶载体印迹牛血红蛋白的研究[J].高等学校化学学报,2009,30(4):691-696.
[8]Laatikainen K,Udomsap D,Siren H,et al. Effect of Template Ion-Ligand Complex Stoichiometry on Selectivity of Ion-Imprinted Polymers[J]. Talanta,2015,134:538-545.
[9]AN Fuqiang,GAO Baojiao,LI Gang. Studies on Preparation of Ion-Imprinted Polyethyleneimine on Silica Gel Particles and Binding Properties for Metal Ions[J]. Acta Polym Sin,2007,(4):366-373(in Chinese).安富强,高保娇,李刚.硅胶表面铜(Ⅱ)离子印迹聚乙烯亚胺的制备及结合特性研究[J].高分子学报,2007,(4):366-373.
[10]Lin S,Wei W,Wu X,et al. Selective Recovery of Pd(Ⅱ)from Extremely Acidic Solution Using Ion-Imprinted Chitosan Fiber:Adsorption Performance and Mechanisms[J]. J Hazard Mater,2015,299(6):10-17.
[11]Liu H,Kong D,Sun W,et al. Effect of anions on the Polymerization and Adsorption Processes of Cu(Ⅱ)Ion-Imprinted Polymers[J]. Chem Eng J,2016,303:348-358.
[12]Luo X,Guo B,Luo J,et al. Recovery of Lithium from Wastewater Using Development of Li Ion-Imprinted Polymers[J].ACS Sustainable Chem Eng,2015,3:460-467.
[13]FAN Hongtao,SUI Dianpeng,ZHAO Lixing,et al. Preparation of Cobalt(Ⅱ)Ion Imprinted Silica Gel Sorbents by Surface Imprinting Technique and Its Adsorption Properties[J]. Chem J Chinese Univ,2011,32(12):2902-2907(in Chinese).范洪涛,隋殿鹏,赵立兴,等.表面印迹法制备钴(Ⅱ)离子印迹硅胶及性能[J].高等学校化学学报,2011,32(12):2902-2907.
[14]Li J,Zhang L,Wei G. Highly Sensitive and Doubly Orientated Selective Molecularly Imprinted Electrochemical Sensor for Cu2+[J]. Biosens Bioelectron,2015,69:316-320.
[15]Kokkios C,Economou A,Raptis I,et al. Lithographically Fabricated Disposable Bismuth-Film Electrodes for the Trace Determination of Pb(Ⅱ)and Cd(Ⅱ)by Anodic Stripping Voltammetry[J]. Electrochim Acta,2008,53(2):5294-5299.
[16]Hummers W S,Offeman R E. Functionalized Graphene and Graphene Oxide:Materials Synthesis and Electronic Applications[J]. J Am Chem Soc,1958,80:1339-1339.
[17]Zhang Z H,Yang X,Zhang H B,et al. Novel Molecularly Imprinted Polymers Based on Multi-Walled Carbon Nanotubes with Binary Functional Monomer for the Solid-Phase Extraction of Erythromycin from Chicken Muscle[J]. J Chromatogr B,2011,879:1617-1624.
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