Department of Chemical and Environmental Engineering, University of California, Riverside, California 92521, USA.
Department of Bioengineering, University of California, Riverside, California 92521, USA.
Analyst. 2016 Apr 25;141(9):2756-60. doi: 10.1039/c6an00018e.
Divalent mercuric (Hg(2+)) ion and monomethyl mercury (CH3Hg(+)) are two forms of mercury that are known to be highly toxic to humans. In this work, we present a highly selective, sensitive and label-free chemiresistive biosensor for the detection of both, Hg(2+) and CH3Hg(+) ions using DNA-functionalized single-walled carbon nanotubes (SWNTs). The SWNTs were functionalized with the capture oligonucleotide, polyT, using a linker molecule. The polyT was hybridized with polyA to form a polyT:polyA duplex. Upon exposure to mercury ions, the polyT:polyA duplex dehybridizes and a T-Hg(2+)-T duplex is formed. This structure switch leads to the release of polyA from the SWNT surface and correspondingly a change in the resistance of the chemiresistive biosensor is observed, which is used to quantify the mercury ion concentration. The biosensor showed a wide dynamic range of 0.5 to 100 nM for the detection of CH3Hg(+) ions in buffer solution with a sensitivity of 28.34% per log (nM) of CH3Hg(+). Finally, real world application of the biosensor was demonstrated by the detection of Hg(2+) and CH3Hg(+) ions in simulated saliva samples spiked with a known concentration of mercury ions.
二价汞(Hg(2+))离子和一甲基汞(CH3Hg(+))是两种已知对人类具有高毒性的汞形式。在这项工作中,我们提出了一种高度选择性、灵敏且无标记的电化学生物传感器,用于检测 Hg(2+)和 CH3Hg(+)离子,该传感器使用 DNA 功能化的单壁碳纳米管(SWNTs)。SWNTs 通过链接分子与捕获寡核苷酸聚 T 进行功能化。聚 T 与聚 A 杂交形成聚 T:聚 A 双链。暴露于汞离子后,聚 T:聚 A 双链解链,形成 T-Hg(2+)-T 双链。这种结构开关导致聚 A 从 SWNT 表面释放,相应地观察到电化学生物传感器的电阻发生变化,可用于定量检测汞离子浓度。该生物传感器在缓冲溶液中对 CH3Hg(+)离子的检测具有 0.5 至 100 nM 的宽动态范围,对 CH3Hg(+)的灵敏度为每对数(nM)增加 28.34%。最后,通过检测模拟唾液样本中添加已知浓度汞离子的 Hg(2+)和 CH3Hg(+)离子,证明了生物传感器的实际应用。