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Ultrasensitive impedimetric mercury(II) sensor based on thymine-Hg(II)-thymine interaction and subsequent disintegration of multiple sandwich-structured DNA chains

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Abstract

An impedimetric method is described for ultrasensitive analysis of mercury(II). It is based on thymine-Hg(II)-thymine interaction which causes the disintegration of multiple-sandwich structured DNA chains. DNA strands were selected that are partially complementary to the T-rich Hg(II)-specific oligonucleotides (MSO). They were immobilized on a gold electrode via Au-S interaction. Next, the MSO and the bridging strands (BS) that can connect adjacent MSOs were alternately attached through layer-by-layer hybridization. Thus, a multiple-sandwich structured interface in created that carries numerous MSOs. This leads to a change-transfer resistance (Rct) values of the electrode-electrolyte interface at faradic electrochemical impedance spectroscopy measurements in the presence of the hexacyanoferrate(II)/(III) redox probe at 0.2 V (vs. Ag/AgCl). If Hg(II) is added to the solution, the MSOs selectively interact with Hg(II) to produce T-Hg(II)-T structures. Hence, the multiple-sandwich hybridization chains become disintegrated, and this causes a decrease in resistivity. The effect can be used to quantify Hg(II) over an analytical range that extends over four orders of magnitude (1 fM to 10 pM), and it has a 0.16 fM limit of detection under optimal conditions.

An electrochemical sensor for femtomolar level detection of Hg2+ is realized on the basis of thymine-Hg2+-thymine interaction which causes disintegration of multiple sandwich DNA hybridization strands.

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Acknowledgements

This work was financially supported by the National Natural Science Foundation of China (Nos. 21802064, 21575027), Natural Science Foundation of Fujian Province (Nos. 2018 J01435, 2017 J01419), and Foundation of Key Laboratory of Sensor Analysis of Tumor Marker from Ministry of Education, Qingdao University of Science and Technology.

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Authors and Affiliations

  1. College of Chemistry and Environment, Fujian Province Key Laboratory of Morden Analytical Science and Separation Technology, Minnan Normal University, Zhangzhou, 363000, People’s Republic of China

    Feng Gao, Taoshun Zhang, Yaru Chu, Qingxiang Wang, Juan Song & Weiwei Qiu

  2. Departement of Food and Biological Engineering, Zhangzhou Institute of Technology, Zhangzhou, 363000, People’s Republic of China

    Taoshun Zhang

  3. Ministry of Education Key Laboratory of Analysis and Detection for Food Safety, Fujian Provincial Key Laboratory of Analysis and Detection for Food Safety, Fuzhou University, Fuzhou, 350116, People’s Republic of China

    Zhenyu Lin

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  1. Feng Gao
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  2. Taoshun Zhang
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  3. Yaru Chu
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  4. Qingxiang Wang
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  5. Juan Song
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  6. Weiwei Qiu
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  7. Zhenyu Lin
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Correspondence to Qingxiang Wang or Zhenyu Lin.

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Gao, F., Zhang, T., Chu, Y. et al. Ultrasensitive impedimetric mercury(II) sensor based on thymine-Hg(II)-thymine interaction and subsequent disintegration of multiple sandwich-structured DNA chains. Microchim Acta 185, 555 (2018). https://doi.org/10.1007/s00604-018-3097-7

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