Department of Physical and Environmental Sciences, University of Toronto, Scarborough, Toronto M1C 1A4, Canada.
Analyst. 2017 May 21;142(10):1827-1834. doi: 10.1039/c7an00238f. Epub 2017 May 5.
The present work describes the effect of the number of thymine-thymine mispairs in single strand DNA probes on Hg(ii) interactions and further to develop a highly sensitive DNA based impedimetric sensor for Hg(ii) detection. To achieve this goal, the influence of the number of T-T mispairs on the signal response prompted by DNA-Hg(ii) binding interactions was examined on three designed DNA probes: 5'-OH-(CH)-S-S-(CH)-AGTCCACACGTTCCTTACGC-3', 5'-OH-(CH)-S-S-(CH)-AGTCCACATTTTCCTTTTGC-3', 5'-OH-(CH)-S-S-(CH)-AGTCCATTTTTTCCTTTTTT-3' having 2T-T, 4T-T and 6T-T mispairs with identical length, respectively. This study revealed that the number of T-T mispairs plays a critical role in maximizing the signal intensity of DNA-Hg(ii) binding interactions. Based on these results, DNA comprising maximum number of T-T mispairs was further utilized for construction of the Hg(ii) sensor, which exhibited a linear correlation between the change in charge transfer resistance (ΔR) and the concentration of Hg(ii) over the range of 1.0 × 10 M to 1.0 × 10 M with a lower detection limit of 3.2 × 10 M. The selectivity was tested against 12 different metal ions including Hg(ii). The ΔR response from Hg(ii) is 3 times higher than the nearest competitor Pb(ii) and approximately 10 times than other ions. The potential application of such a robust and label-free DNA sensor was demonstrated by analyzing environmental samples collected from Lake Ontario.
本工作描述了单链 DNA 探针中胸腺嘧啶-胸腺嘧啶错配数对 Hg(ii) 相互作用的影响,并进一步开发了一种基于 DNA 的高灵敏度电化学阻抗传感器用于 Hg(ii)检测。为了实现这一目标,研究了 DNA-Hg(ii)结合相互作用引发的信号响应中 T-T 错配数对的影响,使用了三个设计的 DNA 探针:5'-OH-(CH)-S-S-(CH)-AGTCCACACGTTCCTTACGC-3'、5'-OH-(CH)-S-S-(CH)-AGTCCACATTTTCCTTTTGC-3'、5'-OH-(CH)-S-S-(CH)-AGTCCATTTTTTCCTTTTTT-3',它们分别具有 2 个、4 个和 6 个 T-T 错配,长度相同。这项研究表明,T-T 错配数对在最大限度地提高 DNA-Hg(ii)结合相互作用的信号强度方面起着关键作用。基于这些结果,进一步利用包含最多 T-T 错配的 DNA 构建了 Hg(ii)传感器,该传感器在 1.0×10^-7 M 至 1.0×10^-5 M 范围内,ΔR 与 Hg(ii)浓度之间呈现线性相关,检测限为 3.2×10^-7 M。该传感器的选择性通过对 12 种不同金属离子(包括 Hg(ii))进行测试得到了验证。来自 Hg(ii)的 ΔR 响应比最接近的竞争离子 Pb(ii)高 3 倍,比其他离子高约 10 倍。通过分析从安大略湖采集的环境样本,展示了这种稳健且无标记的 DNA 传感器的潜在应用。