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Label-free Hg(II) electrochemiluminescence sensor based on silica nanoparticles doped with a self-enhanced Ru(bpy)(3)(2+)-carbon nitride quantum dot luminophore

文献类型： 外文期刊

作者： Li, Libo 1 ; Zhao, Wanlin 1 ; Zhang, Jiayi 2 ; Luo, Lijun 1 ; Liu, Xiaohong 1 ; Li, Xia 3 ; You, Tianyan 1 ; Zhao, Chunjiang 4 ;

作者机构： 1.Jiangsu Univ, Sch Agr Engn, Key Lab Modern Agr Equipment & Technol, Minist Educ, Zhenjiang 212013, Jiangsu, Peoples R China

2.Qingdao Hengxing Univ Sci & Technol, Qingdao 266100, Shandong, Peoples R China

3.Liaocheng Univ, Dept Chem, Liaocheng 252059, Shandong, Peoples R China

4.Natl Engn Res Ctr Informat Technol Agr NERCITA, Beijing 100097, Peoples R China

关键词： Label-free; Self-enhanced ECL; SiO2 nanoparticles; Ru(bpy)(3)(2+); CNQDs; Hg(II)

期刊名称：JOURNAL OF COLLOID AND INTERFACE SCIENCE （ 影响因子：9.965； 五年影响因子：8.554 ）

ISSN： 0021-9797

年卷期： 2022 年 608 卷

页码：

收录情况： SCI

摘要： Herein, a label-free, self-enhanced electrochemiluminescence (ECL) sensing strategy for divalent mercury (Hg(II)) detection was presented. First, a novel self-enhanced ECL luminophore was prepared by combining the ECL reagent tris(2, 2'-bipyridyl) dichlororuthenium(II) hexahydrate (Ru(bpy)(3)(2+)) and its coreactant carbon nitride quantum dots (CNQDs) via electrostatic interactions. In contrast to traditional ECL systems where the emitter and its co-reactant underwent an intermolecular reaction, the self-enhanced ECL system exhibited a shortened electron-transfer distance and enhanced luminous efficiency because the electrons transferred from CNQDs to oxidized Ru(bpy)(3)(2+) via an intramolecular pathway. Furthermore, the as-prepared self-enhanced ECL material was encapsulated in silica (SiO2) nanoparticles to generate a Ru-QDs@SiO2 luminophore. Based on the different affinity of Ru-QDs@SiO2 nanoparticles for single-stranded DNA (ssDNA) and Hg(II)-triggered double-stranded DNA (dsDNA), a label-free ECL biosensor for Hg(II) detection was developed as follows: in the absence of Hg(II), ssDNA was adsorbed on Ru-QDs@SiO2 surface via hydrogen bond, electrostatic, and hydrophobic interaction. Thus, quenched ECL signal was observed. On the contrary, in the presence of Hg(II), stable dsDNA was formed and carried the ssDNA separating from Ru-QDs@SiO2 surface, resulting in most of Ru-QDs@SiO2 existing in their free state. Therefore, a recovered ECL intensity was obtained. On this basis, Hg(II) was measured by the proposed method in the range of 0.1 nM-10 mu M, with a detection limit of 33 pM. Finally, Hg(II) spiked in water samples was measured to evaluate the practicality of the fabricated biosensor. (C) 2021 Published by Elsevier Inc.

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