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Manganese(III)meso-tetrakis(4-N-methylpyridyl)-porphyrin and mediator thionine co-decorated DNA nanowires for sensitive electrochemical monitoring of mercury(II)

机译:锰(III)间-四(4-N-甲基吡啶基)-卟啉和介体亚硫氨酸共修饰的DNA纳米线,用于汞(II)的电化学监测

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摘要

We developed a novel electrochemical DNA biosensor for mercury(II) ion (Hg2+) detection on the basis of manganese(III) meso-tetrakis(4-N-methylpyridyl)-porphyrin (MnTMPyP) and electron mediator thionine (Thi) co-decorated DNA nanowires for signal amplification. The T-rich capture DNA assembled on the electrode could successfully immobilize the primer DNA via specific base-pairing, which triggered the hybridization chain reaction (HCR) to form long DNA nanowires with the aim of loading abundant MnTMPyP and electron mediator Thi. In the electrolyte containing H2O2, the MnTMPyP loaded in the DNA nanowires showed superior peroxidase-like activity and electrocatalyzed the reduction of H2O2, promoting the redox reaction of Thi with a dramatically amplified electrochemical signal. However, in the presence of target Hg2+, Hg2+-mediated thymine base pairs (T-Hg2+-T) are formed between the two neighboring T-rich capture DNAs, which resulted in the release of the MnTMPyP and Thi co-decorated DNA nanowires from the electrode surface, providing a reduced readout signal for the quantitative electrochemical detection of Hg2+. The results showed that the proposed electrochemical DNA biosensor was highly sensitive to Hg2+ in the concentration of 1.0 ng L-1 to 10(7) ng L-1 with a detection limit of 0.5 ng L-1 (2.5 pM), and it also exhibited excellent selectivity against other interferential metal ions.
机译:我们开发了一种基于锰(III)介孔四(4-N-甲基吡啶基)-卟啉(MnTMPyP)和电子介体亚硫氨酸(Thi)的新型电化学DNA生物传感器,用于检测汞(II)离子(Hg2 +) DNA纳米线用于信号放大。组装在电极上的富T捕获DNA可以通过特定的碱基配对成功固定引物DNA,从而引发杂交链反应(HCR)以形成长的DNA纳米线,目的是装载大量的MnTMPyP和电子介体Thi。在含有H2O2的电解质中,DNA纳米线中装载的MnTMPyP显示出优异的过氧化物酶样活性,并电催化H2O2的还原,从而以显着放大的电化学信号促进Thi的氧化还原反应。但是,在存在目标Hg2 +的情况下,在两个相邻的富含T的捕获DNA之间形成了Hg2 +介导的胸腺嘧啶碱基对(T-Hg2 + -T),这导致MnTMPyP和Thi共修饰的DNA纳米线从电极表面,减少了读出信号,用于Hg2 +的定量电化学检测。结果表明,所提出的电化学DNA生物传感器在1.0 ng L-1至10(7)ng L-1的浓度下对Hg2 +高度敏感,检测极限为0.5 ng L-1(2.5 pM),并且对其他干扰金属离子具有极好的选择性。

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