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基于硫氮共掺杂有序介孔碳和胸腺嘧啶-汞-胸腺嘧啶错配结构的电化学适体传感器用于 Hg 检测。

Electrochemical Aptasensor Based on Sulfur-Nitrogen Codoped Ordered Mesoporous Carbon and Thymine-Hg-Thymine Mismatch Structure for Hg Detection.

机构信息

College of Environmental Science and Engineering , Hunan University , Changsha 410082 , P.R. China.

Key Laboratory of Environmental Biology and Pollution Control , Hunan University , Ministry of Education, Changsha 410082 , P.R. China.

出版信息

ACS Sens. 2018 Dec 28;3(12):2566-2573. doi: 10.1021/acssensors.8b00926. Epub 2018 Nov 20.

Abstract

A renewable electrochemical aptasensor was proposed for super-sensitive determination of Hg. The novel aptasensor, based on sulfur-nitrogen codoped ordered mesoporous carbon (SN-OMC) and thymine-Hg-thymine (T-Hg-T) mismatch structure, used ferrocene as signal molecules to achieve the conversion of current signals. In the absence of Hg, the thiol-modified T-rich probe 1 spontaneously formed a hairpin structure by base pairing. After being hybridized with the ferrocene-labeled probe 2 in the presence of Hg, the hairpin structure of probe 1 was opened due to the preferential formation of the T-Hg-T mismatch structure, and the ferrocene signal molecules approached the modified electrode surface. SN-OMC with high specific surface area and ample active sites acted as a signal amplification element in electrochemical sensing. The sensitive determination of Hg can be actualized by analyzing the relationship between the change of oxidation current caused by ferrocene signal molecules and the Hg concentrations. The aptasensor had a fine linear correlation in the range of 0.001-1000 nM with a detection limit of 0.45 pM. The aptasensor also displayed a good response in real sample detection and provided a promising possibility for in situ detection.

摘要

一种可再生电化学适体传感器被提出用于超灵敏测定 Hg。该新型适体传感器基于硫氮共掺杂有序介孔碳 (SN-OMC) 和胸腺嘧啶-Hg-胸腺嘧啶 (T-Hg-T) 错配结构,使用二茂铁作为信号分子来实现电流信号的转换。在不存在 Hg 的情况下,巯基修饰的富含 T 的探针 1 通过碱基配对自发形成发夹结构。在存在 Hg 的情况下,与二茂铁标记的探针 2 杂交后,由于 T-Hg-T 错配结构的优先形成,探针 1 的发夹结构被打开,并且二茂铁信号分子接近修饰电极表面。具有高比表面积和丰富活性位点的 SN-OMC 在电化学传感中充当信号放大元件。通过分析由于 ferrocene 信号分子引起的氧化电流变化与 Hg 浓度之间的关系,可以实现对 Hg 的灵敏测定。适体传感器在 0.001-1000 nM 的范围内具有良好的线性相关性,检测限为 0.45 pM。该适体传感器在实际样品检测中也表现出良好的响应,为原位检测提供了有前景的可能性。

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