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检测痕量Hg2+的DNA电化学生物传感器

DNA Electrochemical Biosensor for Trace Hg2+ Detection

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【作者】 戈芳曹瑞国朱斌李经建徐东升

【Author】 GE Fang1,2 CAO Rui-Guo1 ZHU Bin1 LI Jing-Jian1, XU Dong-Sheng1, (1Beijing National Laboratory for Molecular Sciences, State Key Laboratory for Structural Chemistry of Unstable and Stable Species, College of Chemistry and Molecular Engineering, Peking University, Beijing 100871, P.R.China; 2Department of Chemical and Biological Engineering, College of Sanming, Sanming 365004, Fujian Province, P.R.China)

【机构】 北京大学化学与分子工程学院,分子动态与稳态结构国家重点实验室,北京分子科学国家实验室三明学院化学与生物工程系

【摘要】 通过自组装方法将修饰有二茂铁基团的富T序列DNA分子(DNA-Fc)固定在金电极表面,得到了一种基于DNA修饰电极的电化学汞离子(Hg2+)传感器.当溶液中有Hg2+存在时,Hg2+可与修饰电极上DNA的T碱基发生较强的特异结合,形成T-Hg2+-T发卡结构,使DNA分子构象发生改变,其末端具有电化学活性的二茂铁基团远离电极表面,电化学响应随之发生变化.示差脉冲伏安法(DPV)结果显示:DNA末端二茂铁基团的还原峰在0.26V(vs饱和甘汞电极(SCE))附近,峰电流随溶液中Hg2+浓度的增加而降低;Hg2+浓度范围在0.1nmol·L-1-1μmol·L-1时,电流相对变化率与Hg2+浓度的对数呈现良好的线性关系.该修饰电极对Hg2+的检测限为0.1nmol·L-1,可作为痕量Hg2+检测的电化学生物传感器.干扰实验也表明,该传感器对Hg2+具有良好的特异性与灵敏度.

【Abstract】 In this paper we demonstrated a novel type of electrochemical Hg2+ biosensor based on a DNA-modified electrode.Ferrocenyl-modified T-rich DNA (DNA-Fc) molecules were synthesized for use as electrochemical probes.We then fixed these DNA-Fc probes onto a gold electrode surface by self-assembly.In the presence of Hg2+, the single strand DNA on the electrode surface turned to a thymine-Hg2+-thymine (T-Hg2+-T) hairpin structure.The ferrocenyl groups were kept away from the surface of the electrode, and this could be measured sensitively by differential pulse voltammetry (DPV).The results show a reduction peak of ferrocene at 0.26 V (vs saturated calomel electrode (SCE)) and the peak current of DPV decreased with increasing the concentration of Hg2+.The rate of current change is linear with regards to lgcHg2+ over a concentration range from 0.1 nmol·L-1 to 1 μmol·L-1 and with a detection limit of 0.1 nmol·L-1.A test for interference metal ions showed that this electrochemical biosensor based on a DNA modified electrode is highly sensitive and selective, and it can be widely used for trace Hg2+ detection.

【基金】 国家自然科学基金(20573008,50821061);国家重点基础研究项目特别基金(2006CB806102);国家重点基础研究发展计划项目(973)(2007CB936201)资助项目~~
  • 【文献出处】 物理化学学报 ,Acta Physico-Chimica Sinica , 编辑部邮箱 ,2010年07期
  • 【分类号】O646.54
  • 【被引频次】40
  • 【下载频次】673
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