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基于氮掺杂碳量子点作为Ru(dcbpy)共反应剂的用于检测17β-雌二醇的诱导自增强电化学发光适体传感器:分子间氢键在该体系中起什么作用?

Induced self-enhanced electrochemiluminescence aptamer sensor for 17β-estradiol detection based on nitrogen-doped carbon quantum dots as Ru(dcbpy) coreactant: What role of intermolecular hydrogen bonds play in the system?

作者信息

Liu Xiaohong, Li Libo, Luo Lijun, Bi Xiaoya, Yan Hui, Li Xia, You Tianyan

机构信息

Key Laboratory of Modern Agricultural Equipment and Technology, Ministry of Education, School of Agricultural Engineering, Jiangsu University, Zhenjiang, Jiangsu 212013, China.

Key Laboratory of Modern Agricultural Equipment and Technology, Ministry of Education, School of Agricultural Engineering, Jiangsu University, Zhenjiang, Jiangsu 212013, China.

出版信息

J Colloid Interface Sci. 2021 Mar 15;586:103-109. doi: 10.1016/j.jcis.2020.10.074. Epub 2020 Oct 28.

DOI:10.1016/j.jcis.2020.10.074
PMID:33160631
Abstract

Herein, an induced self-enhanced electrochemiluminescence (ECL) sensor with superior ECL performances was simply fabricated by just dropping the ECL reagent (tris(4,4'-dicarboxylicacid-2,2'-bipyridyl) ruthenium (II) dichloride, Ru(dcbpy)Cl) and coreactant (nitrogen-doped carbon quantum dots, NCQDs) pair onto the surface of glassy carbon electrode. In this strategy, based on the carboxyl (-COOH) groups in Ru(dcbpy) and oxygen, nitrogen-containing groups on NCQDs surface, an intermolecular hydrogen bonds-induced self-enhanced ECL composite was generated in the solid contact layer for the first time. Since Ru(dcbpy) and NCQDs were co-existing in the same composite, the electron-transfer distance between them was shortened and the energy loss was decreased, thereby higher ECL efficiency was acquired. This working process greatly avoided the introduction of signal amplifier and simplified the experimental operation. On this basis, 17β-estradiol (E2) was selected as a target model to fabricate a self-enhanced ECL aptamer sensor for the investigation of its analytical performances. Resultantly, excellent detection properties of E2, including wider linear range of 1.0 × 10 - 1.0 × 10 mol L and lower detection limit of 1.0 × 10 mol L with superior selectivity, were successfully achieved. Finally, E2 spiked into milk powder was quantified to assess the practicability of this sensor. Prospectively, this strategy could be extensively applied for other analytes determination by adjusting the corresponding target aptamers.

摘要

在此,通过将电化学发光(ECL)试剂(二氯双(4,4'-二羧酸-2,2'-联吡啶)钌(II),Ru(dcbpy)Cl)和共反应剂(氮掺杂碳量子点,NCQDs)对简单滴加到玻碳电极表面,制备了一种具有优异ECL性能的诱导自增强电化学发光传感器。在该策略中,基于Ru(dcbpy)中的羧基(-COOH)基团以及NCQDs表面的含氧、含氮基团,首次在固体接触层中生成了分子间氢键诱导的自增强ECL复合材料。由于Ru(dcbpy)和NCQDs共存于同一复合材料中,它们之间的电子转移距离缩短,能量损失降低,从而获得了更高的ECL效率。这一工作过程极大地避免了信号放大器的引入,简化了实验操作。在此基础上,选择17β-雌二醇(E2)作为目标模型,制备了一种自增强ECL适体传感器,以研究其分析性能。结果成功实现了E2的优异检测性能,包括1.0×10 - 1.0×10 mol L的更宽线性范围和1.0×10 mol L的更低检测限以及优异的选择性。最后,对添加到奶粉中的E2进行了定量分析,以评估该传感器的实用性。前瞻性地,通过调整相应的目标适体,该策略可广泛应用于其他分析物的测定。

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