School of Chemistry and Chemical Engineering, University of Chinese Academy of Sciences, 19A YuQuan Road, 100049 Beijing, China.
Biosens Bioelectron. 2013 Oct 15;48:180-7. doi: 10.1016/j.bios.2013.04.013. Epub 2013 Apr 19.
A novel electrochemical biosensor for sensitive and selective detection of mercury (II) ions (Hg²⁺) based on a DNA grafted graphene is proposed. Graphene oxide (GO) was reduced by dopamine, and then the single-strand probe DNA modified at the 5'-end with an alkylamino modifier (NH₂-ssDNA) was grafted on the reduced graphene oxide (RGO) surface via Michael addition reaction. In the presence of Hg²⁺, the target DNA with four thymine-thymine (T-T) mismatches would hybridize with the probe DNA on the glassy carbon electrode (GCE) through T-Hg²⁺-T coordination chemistry. The hybridization of the two oligonucleotides leads to the increase in the peak currents of [Ru(NH₃)₆]³⁺, which could be used for electrochemical sensing of Hg²⁺. The difference in the value of the peak currents of [Ru(NH₃)₆]³⁺ before and after DNA hybridization was linear with the concentration of Hg²⁺ in the range from 8.0×10⁻⁹ to 1.0×10⁻⁷ M with a linear coefficiency of 0.996. The detection limit was 5.0×10⁻⁹ M (S/N=3). The proposed electrochemical biosensor is rapid, convenient and low-cost for effective sensing of Hg²⁺. Particularly, the proposed method was applied successfully to the determination of Hg²⁺ in real environmental samples.
提出了一种基于接枝石墨烯的新型电化学生物传感器,用于灵敏和选择性检测汞(II)离子(Hg²⁺)。多巴胺还原氧化石墨烯(GO),然后通过迈克尔加成反应将 5'-端带有烷基氨基修饰剂(NH₂-ssDNA)的单链探针 DNA 接枝在还原氧化石墨烯(RGO)表面上。在存在 Hg²⁺的情况下,具有四个胸腺嘧啶-胸腺嘧啶(T-T)错配的目标 DNA 会通过 T-Hg²⁺-T 配位化学与玻璃碳电极(GCE)上的探针 DNA 杂交。两种寡核苷酸的杂交导致 [Ru(NH₃)₆]³⁺的峰电流增加,可用于电化学检测 Hg²⁺。[Ru(NH₃)₆]³⁺的峰电流在 DNA 杂交前后的差值与 Hg²⁺的浓度在 8.0×10⁻⁹ 至 1.0×10⁻⁷ M 范围内呈线性关系,线性系数为 0.996。检测限为 5.0×10⁻⁹ M(S/N=3)。该电化学生物传感器快速、方便且成本低,可有效检测 Hg²⁺。特别是,该方法成功应用于实际环境样品中 Hg²⁺的测定。