基于石墨烯掺杂金纳米粒子的灭除威分子印迹电化学传感器的制备与性能研究  

Preparation of Molecularly Imprinted Electrochemical Sensor for Detection of 3,5-Xylyl Methylcarbamate Based on Gold Nanoparticles-dopped Graphene Modified Glassy Carbon Electrode

作　　者：胡琪[1] 谭学才[1] 吴佳雯[1] 李晓宇[1] 李鹏飞[1] 余会成[1] 李小燕[1] 雷福厚 

机构地区：[1]广西民族大学化学化工学院,广西林产化学与工程重点实验室,广西高校食品安全与药物分析化学重点实验室,广西南宁530008

出　　处：《分析测试学报》2015年第3期328-334,共7页Journal of Instrumental Analysis

基　　金：国家自然科学基金(21365004;21065001;21165003);广西自然科学重点基金(2013GXNSFDA019006);广西教育厅重点科研基金(2013ZD019);广西高等学校高水平创新团队及卓越学者资助计划(桂教人[2014]7号);广西民族大学研究生教育创新计划项目(GXUN-chx2013092)

摘　　要：以灭除威（XMC）为模板分子,甲基丙烯酸（MAA）为功能单体,合成的马来松香丙烯酸乙二醇酯（EGMRA）为交联剂,在石墨烯掺杂金纳米粒子修饰玻碳电极表面合成分子印迹膜,研制了测定XMC的分子印迹电化学传感器.采用扫描电镜（SEM）对传感膜的形貌进行表征,通过循环伏安法（CV）、电化学阻抗谱法（EIS）和差示脉冲伏安法（DPV）对传感器的性能进行研究.DPV测试表明,XMC的浓度在1.0×10-7～2.0×10-5 mol·L-1范围内呈良好线性关系,相关系数（r）为0.997 9,检出限（S/N=3）为1.5×10-8 mol·L-1.选择性识别实验结果表明,XMC印迹敏感膜的印迹因子（β）达到2.94,相对于干扰物的选择因子（α）均大于1,对与XMC结构相似的速灭威的选择因子达到2.39,说明该印迹膜对XMC具有良好的选择性.识别过程动力学研究结果表明,石墨烯掺杂金纳米粒子分子印迹传感器的动力学结合速率常数k为73.05 s.将此传感器应用于蔬菜样品的加标回收检测,加标回收率为95.4％～ 108.0％.A new molecular imprinted electrochemical sensor was developed for the detection of 3, 5- xylyl methylcarbamate（XMC） by combination of graphene and gold rlanoparticles. The molecularly imprinted polymer（M1P） was synthesized on the surface of grapheme and gold nanoparticles modified glassy carbon electrode by using XMC as template molecular, methyl acrylic acid（MAA） as function- al monomer, amt ethylene glycol maleic rosinate acrylate（EGMRA） as cross-linker. The morphology of the sensing membrane was characterized by scanning electron microscopy（SEM）. The performance of the sensor was investigated by cyclic voltammetry （CV） , differential pulse voltammetry （DPV） and electrochemical impedance spectroscopy（EIS）. A linear relationship between oxidation peak current and XMC concentration was obtained over the range of 1.0 × 10^-7 -2.0× 10^-5 mol L-1 with a cor- relation coefficient of 0. 997 9 and a detection limit（S/N = 3） of 1.5 × 10^8 mol L-1 The selectiv- ity experiments showed that the imprinting factor（,6） of XMC imprinted film was 2.94 and the selec- tivity factors（a） of XMC compared to interference were all larger than 1. Although a minor interfer- ence was generated by XMC for its structure similar to metolcarb, the selectivity factor also reached to 2. 39. The results indicated that the imprinted polymer films exhibited an excellent selectivity for XMC. The kinetics of recognition suggested that the process of the imprinted polymer films adsorbing XMC is Langmuir model and its kinetic rate constant is 73.05 s. The imprinted sensor was success- fully used to determine XMC in vegetable samples with recoveries of 95.4% - 108.0% by using the standard addition method.

关 键 词：灭除威 石墨烯掺杂金纳米粒子 马来松香丙烯酸乙二醇酯 分子印迹电化学传感器 选择性识别 

分 类 号：O657.1[理学—分析化学] F767.2[理学—化学]