Huang Dawei, Niu Chenggang, Zeng Guangming, Wang Xiaoyu, Lv Xiaoxiao
College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Hunan University, Changsha 410082, China; South China Institute of Environmental Sciences, Ministry of Environmental Protection of PRC, Guangzhou 510655, China.
College of Environmental Science and Engineering, Key Laboratory of Environmental Biology and Pollution Control (Hunan University), Ministry of Education, Hunan University, Changsha 410082, China.
Talanta. 2015 Jan;132:606-12. doi: 10.1016/j.talanta.2014.10.015. Epub 2014 Oct 18.
In this paper, a sensitive time-gated fluorescent sensing strategy for mercury ions (Hg(2+)) monitoring is developed based on Hg(2+)-mediated thymine (T)-Hg(2+)-T structure and the mechanism of fluorescence resonance energy transfer from Mn-doped CdS/ZnS quantum dots to graphene oxide. The authors employ two T-rich single-stranded DNA (ssDNA) as the capture probes for Hg(2+), and one of them is modified with Mn-doped CdS/ZnS quantum dots. The addition of Hg(2+) makes the two T-rich ssDNA hybrids with each other to form stable T-Hg(2+)-T coordination chemistry, which makes Mn-doped CdS/ZnS quantum dots far away from the surface of graphene oxide. As a result, the fluorescence signal is increased obviously compared with that without Hg(2+). The time-gated fluorescence intensities are linear with the concentrations of Hg(2+) in the range from 0.20 to 10 nM with a limit of detection of 0.11 nM. The detection limit is much lower than the U.S. Environmental Protection Agency limit of the concentration of Hg(2+) for drinking water. The time-gated fluorescent sensing strategy is specific for Hg(2+) even with interference by other metal ions based on the results of selectivity experiments. Importantly, the proposed sensing strategy is applied successfully to the determination of Hg(2+) in environmental water samples.
本文基于汞离子(Hg(2+))介导的胸腺嘧啶(T)-Hg(2+)-T结构以及锰掺杂硫化镉/硫化锌量子点与氧化石墨烯之间的荧光共振能量转移机制,开发了一种用于汞离子监测的灵敏的时间分辨荧光传感策略。作者采用两条富含胸腺嘧啶的单链DNA(ssDNA)作为汞离子的捕获探针,其中一条用锰掺杂硫化镉/硫化锌量子点进行了修饰。加入汞离子会使两条富含胸腺嘧啶的单链DNA相互杂交,形成稳定的T-Hg(2+)-T配位化学结构,这使得锰掺杂硫化镉/硫化锌量子点远离氧化石墨烯表面。结果,与未加入汞离子时相比,荧光信号明显增强。时间分辨荧光强度与汞离子浓度在0.20至10 nM范围内呈线性关系,检测限为0.11 nM。该检测限远低于美国环境保护局规定的饮用水中汞离子浓度限值。基于选择性实验结果,即使存在其他金属离子的干扰,该时间分辨荧光传感策略对汞离子仍具有特异性。重要的是,所提出的传感策略已成功应用于环境水样中汞离子的测定。