纳米氧化硅表面自组装噻吩磺隆分子印迹材料电致化学发光免疫传感器  

Self-Assembled Thifensulfuron-Methyl Surface Molecular Imprinting Material on Silica Nanoparticles for Electrochemiluminescence Immunosensor

作　　者：侯建国 周佳宇 陈文梅 王现利 张敏 HOU Jianguo;ZHOU Jiayu;CHEN Wenmei;WANG Xianli;ZHANG Min(Zhejiang Geological Prospecting Institute,China Chemical Geology and Mine Bureau,Hangzhou 310000,China)

机构地区：[1]中化地质矿山总局浙江地质勘查院,杭州310000

出　　处：《理化检验（化学分册）》2024年第5期507-512,共6页Physical Testing and Chemical Analysis(Part B:Chemical Analysis)

基　　金：中化地质矿山总局污染土壤修复技术研发及应用团队建设项目(ZHTD202105)。

摘　　要：以噻吩磺隆(TFM)为模板,α-甲基丙烯酸(MAA)为功能单体,在纳米氧化硅(SiO_(2))表面自组装聚合TFM分子印迹膜,组建新型纳米氧化硅表面分子印迹材料电致化学发光(ECL)免疫传感器。结合扫描电子显微镜及紫外光谱分析优化了自组装的试验条件。取制备好的纳米SiO_(2) 100 mg,超声分散在50 mL无水甲苯中,迅速加入0.8 mL(3-氨基丙基)三乙氧基硅烷(APTS),在氮气保护下,于130℃回流24 h,得到表面改性的纳米氧化硅产物(APTS-SiO_(2)),用无水乙醇和乙腈分别洗涤3次,干燥24 h。取20 mg APTS-SiO_(2),超声分散在50 mL乙腈中,加入TFM 0.1 mmol、MAA 0.4 mmol、二甲基丙烯酸乙二醇酯(EGDMA)1.6 mmol、引发剂2,2-偶氮二异丁腈(AIBN)15 mg进行聚合反应,再用50 mmol·L^(-1)氢氧化钠-甲醇溶液洗脱模板分子,洗涤,离心得到中性的分子印迹材料TFM@Si-MIP。将TFM@Si-MIP的分散溶液滴加到打磨好的玻碳电极(GCE)表面,用红外灯烘干后即为TFM分子印迹材料修饰的传感器TFM@Si-MIP-ECL。组建的表面分子印迹材料电致化学发光免疫传感器结合鲁米诺体系实现了对TFM的高灵敏检测。结果表明,该分子印迹电致化学发光免疫传感器对目标分子具有较强的选择性,有效避免其他组分干扰。TFM的浓度在1.0×10^(-10)~1.0×10^(-7) mol·L^(-1)内,其对数与电致发光信号强度的对数呈线性关系,检出限(3S/N)为8.6×10^(-11) mol·L^(-1)。按照标准加入法对环境水样进行回收试验,回收率为94.1%~109%,测定值的相对标准偏差(n=7)均小于5.0%。Using thifensulfuron-methyl(TFM)as the template andα-methacrylic acid(MMA)as the functional monomer,a novel surface molecular imprinting material electrochemiluminescence(ECL)immunosensor was prepared by self-assembled TFM molecular imprinting film on the surface of silicon oxide(SiO_(2))nanoparticles.The experimental conditions for self-assembly were optimized by combining scanning electron microscopy and ultraviolet spectroscopy analysis.100 mg of the prepared SiO_(2) nanoparticles was taken and dispersed in 50 mL of anhydrous toluene by ultrasonic.And then 0.8 mL of(3-aminopropyl)triethoxysilane(APTS)was added fast and refluxed at 130℃ for 24 h under nitrogen protection to obtain surface modified nano silica oxide product(APTS-SiO2),followed by washing three times with anhydrous ethanol and acetonitrile,and drying for 24 h.20 mg of APTS-SiO_(2) was taken,and dispersed in 50 mL of acetonitrile by ultrasonic.0.1 mmol of TFM,0.4 mmol of MAA,1.6 mmol of ethylene glycol methacrylate(EGDMA),and 15 mg of initiator 2,2-azodiisobutyronitrile(AIBN)were added for polymerization reaction.The origin TFM molecules in the polymer(the template molecules)were eluted by 50 mmol·L-1 NaOH-CH3OH solution.After washing and centrifugation,a neutral molecular imprinting material TFM@Si-MIP was obtained.The TFM@Si-MIP disperse solution was immobilized at a surface polished glassy carbon electrode(GCE),and a sensor modified with TFM molecular imprinting material TFM@Si-MIP-ECL was got after drying with an infrared lamp.The TFM@Si-MIP-ECL combined with Luminol system achieved highly sensitive detection of TFM.As shown by the results,this molecular imprinting electrochemiluminescence immunosensor had strong selectivity for target molecules,effectively avoiding interference from other components.Linear relationship between logarithm of TFM concentration and logarithm of electrochemiluminescence signal intensity was found in the range of 1.0×10^(-10)-1.0×10^(-7)mol·L^(-1),with detection limit(3S/N)of 8.6×10^(-11)mol·L^(-1).Test fo

关 键 词：噻吩磺隆 电致化学发光免疫传感器 表面分子印迹 

分 类 号：O657.1[理学—分析化学]