State Key Laboratory of Chemo/Biosensing and Chemometrics, College of Chemistry and Chemical Engineering, Hunan University , Changsha, 410082, China.
Anal Chem. 2013 Sep 17;85(18):8594-600. doi: 10.1021/ac401408m. Epub 2013 Aug 26.
Heavy metal ion pollution poses severe risks in human health and the environment. Driven by the need to detect trace amounts of mercury, this article demonstrates, for the first time, that silver/mercury amalgamation, combining with DNA-protected silver nanoparticles (AgNPs), can be used for rapid, easy and reliable screening of Hg(2+) ions with high sensitivity and selectivity over competing analytes. In our proposed approach, Hg(2+) detection is achieved by reducing the mercury species to elemental mercury, silver atoms were chosen as the mercury atoms' acceptors by forming Ag/Hg amalgam. To signal fluorescently this silver amalgamation event, a FAM-labeled ssDNA was employed as the signal reporter. AgNPs were grown on the DNA strand that resulted in greatly quenching the FAM fluorescence. Formation of Ag/Hg amalgam suppresses AgNPs growth on the DNA, leading to fluorescence signal increase relative to the fluorescence without Hg(2+) ions, as well as marked by fluorescence quenching. This FAM fluorescence enhancement can be used for detection of Hg(2+) at the a few nanomolar level. Moreover, due to excellent specificity of silver amalgamation with mercury, the sensing system is highly selective for Hg(2+) and does not respond to other metal ions with up to millimolar concentration levels. This sensor is successfully applied to determination of Hg(2+) in tap water, spring water and river water samples. The results shown herein have important implications in the development of new fluorescent sensors for the fast, easy, and selective detection and quantification of Hg(2+) in environmental and biological samples.
重金属离子污染对人类健康和环境构成了严重威胁。受检测痕量汞的需求驱动,本文首次展示了银/汞合金化与 DNA 保护的银纳米粒子(AgNPs)结合,可用于快速、简便和可靠地筛选 Hg(2+)离子,具有高灵敏度和选择性,可排除竞争分析物的干扰。在我们提出的方法中,通过将汞物种还原为元素汞来检测 Hg(2+),银原子被选为汞原子的受体,通过形成 Ag/Hg 汞齐。为了荧光信号检测银汞齐的形成,采用 FAM 标记的 ssDNA 作为信号报告。AgNPs 在 DNA 链上生长,导致 FAM 荧光大大猝灭。Ag/Hg 汞齐的形成抑制了 DNA 上 AgNPs 的生长,导致荧光信号相对于没有 Hg(2+)离子的荧光信号增加,同时伴有荧光猝灭。这种 FAM 荧光增强可用于检测几纳摩尔级别的 Hg(2+)。此外,由于银与汞的汞齐化具有优异的特异性,该传感系统对 Hg(2+)具有高度选择性,对高达毫摩尔浓度水平的其他金属离子没有响应。该传感器成功应用于自来水中 Hg(2+)的测定、泉水和河水样本。本文的结果对于开发新的荧光传感器具有重要意义,可用于环境和生物样本中 Hg(2+)的快速、简便和选择性检测和定量。