以氯化血红素作为指示剂的Hg~(2+)电化学传感器的制备与应用
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摘要
采用氯化血红素(hemin)作为电化学指示剂,设计了一种用于检测Hg~(2+)的电化学适配体传感器。适配体(aptamer)通过形成Au-S键自组装在氮掺杂石墨烯和纳米金修饰电极表面,当Hg~(2+)与T碱基特异性结合形成T-Hg~(2+)-T结构后,使电极表面负载的适配体形成多孔结构。Hemin能够吸附在电极表面上产生电化学信号,用示差脉冲伏安法进行检测,在5.0×10~(-8)～5.0×10~(-6 )mol/L范围内,还原峰电流与Hg~(2+)浓度的对数呈良好的线性关系,线性回归方程为Ipc(μA)=6.115+48.021 lg C(mol/L)(γ=0.995),检测限为1.67×10~(-8) mol/L (3σ),将本方法成功用于水样中Hg~(2+)的测定。
An electrochemical aptamer sensor was prepared by using hemin as redox indicator. Aptamer were self-assembled through Au-S bonding on N-doped graphene and gold nanoparticle modified electrode. T-Hg~(2+)-T structure was formed with Hg~(2+) bound specifically of T base,which led to the formation of porous structure on the electrode surface. Hemin could be further adsorbed on the electrode surface to produce electrochemical signals,which was detected by differential pulse voltammetry. The reduction peak current had a good linear relationship with the logarithm of Hg~(2+) concentration in the range of 5.0×10~(-8)～5.0×10~(-6) mol/L,with gave the linear regression equation and the detection limit as Ipc(μA)=6.115+48.021 lg C(mol/L)(γ= 0.995) and 1.67×10~(-8) mol/L(3σ),respectively. The proposed method was further applied to the Hg~(2+) concentration detection in water sample.
An electrochemical aptamer sensor was prepared by using hemin as redox indicator. Aptamer were self-assembled through Au-S bonding on N-doped graphene and gold nanoparticle modified electrode. T-Hg~(2+)-T structure was formed with Hg~(2+) bound specifically of T base,which led to the formation of porous structure on the electrode surface. Hemin could be further adsorbed on the electrode surface to produce electrochemical signals,which was detected by differential pulse voltammetry. The reduction peak current had a good linear relationship with the logarithm of Hg~(2+) concentration in the range of 5.0×10~(-8)～5.0×10~(-6) mol/L,with gave the linear regression equation and the detection limit as Ipc(μA)=6.115+48.021 lg C(mol/L)(γ= 0.995) and 1.67×10~(-8) mol/L(3σ),respectively. The proposed method was further applied to the Hg~(2+) concentration detection in water sample.
引文
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[2]Keith B,Amin S.Arsenic and mercury concentrations in marine fish sourced from local fishermen and fish markets in mine-impacted communities in Ratatotok Sub-district,North Sulawesi,Indonesia[J].Marine Pollution Bulletin,2017,120(1-2):75-81.
[3]宋畅,张翼,郝剑,等.燃煤电厂超低排放改造前后汞污染排放特征[J].环境科学研究,2017,30(5):672-677.
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[5]游元丁,田亚平,周楠迪.基于适配体的石墨烯修饰玻碳电极检测卡那霉素[J].分析测试学报,2015,34(5):600-604.
[6]王丹侠,崔世勇.血红素的应用分析研究进展[J].上海预防医学杂志,2002,14(5):219-221.
[7]赵美莲,倪丹丹,王建文,等.直接电沉积金纳米粒子修饰氧化铟锡电极测定亚硝酸根[J].分析化学,2008,36(12):1729-1731.
[8]于文强,易清风.电沉积纳米金修饰钛电极对甲醛的电催化氧化[J].传感技术学报,2009,22(11):1529-1532.
[9]Niu X L,Zheng W,Yin C X,et al.Electrochemical DNA biosensor based on gold nanoparticles and partially reduced graphene oxide modified electrode for the detection of Listeria monocytogenes hly gene sequence[J].Journal of Electroanalytical Chemistry,2017,806:116-122.
[10]Baker B R,Lai R Y,Word M S,et al.An electronic,aptamer-based small-molecule sensor for the rapid,label-free detection of cocaine in the adulterated samples and biological fluids[J].Journal of the American Chemical Society,2006,128 (10):3138-3139.
[11]Lai Youqun,Ma Yanyan,Sun Liping,et al.A highly selective electrochemical biosensor for Hg2+ using hemin as a redox indicator[J].Electrochimica Acta,2011,56:3153-3158.
[12]谢慧,闫丽君,孙伟,等.基于石墨烯-TiO2复合材料的蛋白质电化学传感器的研究[J].海南师范大学学报(自然科学版),2017,30(1):28-33.