College of Chemistry and Institute for Advanced Study, Nanchang University, Nanchang, Jiangxi 330031, China.
College of Chemistry and Institute for Advanced Study, Nanchang University, Nanchang, Jiangxi 330031, China; Department of Materials and Chemical Engineering, Pingxiang University, Pingxiang 337055, China.
Biosens Bioelectron. 2017 Aug 15;94:701-706. doi: 10.1016/j.bios.2017.03.057. Epub 2017 Mar 30.
Novel fluorescent DNA quantum dots (QDs) were synthesized by hydrothermal treatment of G-/T-rich ssDNA at relatively low reaction temperature. The obtained DNA QDs demonstrate unique optical properties, maintain the basic structure and biological activities of ssDNA precursors, which makes the DNA QDs able to specifically bind with arsenite, driving the (GT) region suffer conformation evolution and form well-ordered assembly rather than random aggregations. We speculate that the strong inter-molecule interaction and efficient stacking of base pairs stiffen the assembly structure, block the nonradiative relaxation channels, populate the radiative decay, and thus making the assembly be highly emissive as a new fluorescence center. The arsenite-induced specific fluorescence enhancement facilitates DNA QDs as light-up probes for arsenite sensing. Under optimal conditions, a linear relationship between the increased fluorescence intensity of DNA QDs and the logarithmic values of arsenite concentration in the range of 1-150ppb with a detection limit of 0.2ppb (3σ) was obtained. The nanosensor shows excellent selectivity for "turn on" arsenite determination and arsenate does not show any interference, facilitating its application in complex real water analysis.
新型荧光 DNA 量子点 (QD) 是通过在相对较低的反应温度下水热处理 G-/T-丰富的 ssDNA 合成的。所得到的 DNA QD 具有独特的光学性质,保持了 ssDNA 前体的基本结构和生物活性,这使得 DNA QD 能够与亚砷酸盐特异性结合,驱动(GT)区域发生构象演变并形成有序的组装,而不是随机聚集。我们推测,分子间的强相互作用和碱基对的有效堆积使组装结构变硬,阻塞非辐射弛豫通道,填充辐射衰变,从而使组装体作为新的荧光中心具有很强的发光性。亚砷酸盐诱导的特异性荧光增强使 DNA QD 成为亚砷酸盐传感的亮点探针。在最佳条件下,DNA QD 的荧光强度增加与 1-150ppb 范围内亚砷酸盐浓度的对数呈线性关系,检测限为 0.2ppb(3σ)。该纳米传感器对“开启”亚砷酸盐测定具有优异的选择性,而砷酸盐没有显示出任何干扰,有利于其在复杂实际水样分析中的应用。