Amplified electrochemiluminescence of Ru(dcbpy)₃²⁺ via coreactant active sites on nitrogen-doped graphene quantum dots.

IF 5.6 1区化学 Q1 CHEMISTRY, ANALYTICAL Talanta Pub Date : 2025-05-01 Epub Date: 2025-01-13 DOI:10.1016/j.talanta.2025.127554

Lingyue Guo, Libo Li, Lijun Luo, Tianyan You

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引用次数: 0

Abstract

Searching for new alternative to tripropylamine (TPrA) with low toxicity and high chemical stability for the tris(4,4'-dicarboxylic acid-2,2'-bipyridyl)ruthenium (II) (Ru(dcbpy)₃²⁺) based coreactant electrochemiluminescence (ECL) system is essential for widespread analytical applications. Here, nitrogen-doped graphene quantum dots (NGQDs) have been discovered to significantly amplify the ECL emission and increase the ECL efficiency of Ru(dcbpy)₃²⁺ for the first time. However, the mechanism by which NGQDs act as coreactants is not well comprehended. Therefore, various optical and electrochemical technologies were employed to investigate the ECL mechanism. It is proposed that the amino and carboxyl groups on the surface of NGQDs play crucial roles as the coreactant active sites, catalyzing the oxidation of Ru(dcbpy)₃²⁺. Based on this foundation, an "on-off-on" ECL aptasensor for the quantification of acetamiprid was developed, exhibiting a broad linear range and a detection limit of 0.056 pM. Satisfactory recoveries, ranging from 98.0 % to 101.6 %, were achieved in pakchoi samples. Consequently, NGQDs could serve as coreactants for Ru(dcbpy)₃²⁺, offering new opportunities for constructing a variety of sensors with extensive analytical applications in the ECL field.

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氮掺杂石墨烯量子点上Ru(dcbpy)32+通过反应物活性位点的放大电化学发光。

寻找低毒性、高化学稳定性的三（4,4’-二羧酸-2,2’-联吡啶基）钌（II）（Ru(dcbpy)32+）基共反应电化学发光（ECL）体系的新替代品是广泛应用于分析的必要条件。本研究首次发现氮掺杂石墨烯量子点（NGQDs）可以显著增强Ru(dcbpy)32+的ECL发射，并提高其ECL效率。然而，ngqd作为共反应物的机制尚不清楚。因此，采用各种光学和电化学技术来研究ECL机理。研究表明，NGQDs表面的氨基和羧基作为反应物活性位点，在催化Ru(dcbpy)32+氧化过程中起着至关重要的作用。在此基础上，研制了一种具有宽线性范围、检出限为0.056 pM的“on-off-on”ECL感应传感器。小白菜样品的加样回收率为98.0% ~ 101.6%。因此，NGQDs可以作为Ru(dcbpy)32+的共反应物，为构建具有广泛分析应用的各种传感器提供了新的机会。

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来源期刊

Talanta 化学-分析化学

CiteScore

12.30

自引率

4.90%

发文量

861

审稿时长

29 days

期刊介绍： Talanta provides a forum for the publication of original research papers, short communications, and critical reviews in all branches of pure and applied analytical chemistry. Papers are evaluated based on established guidelines, including the fundamental nature of the study, scientific novelty, substantial improvement or advantage over existing technology or methods, and demonstrated analytical applicability. Original research papers on fundamental studies, and on novel sensor and instrumentation developments, are encouraged. Novel or improved applications in areas such as clinical and biological chemistry, environmental analysis, geochemistry, materials science and engineering, and analytical platforms for omics development are welcome. Analytical performance of methods should be determined, including interference and matrix effects, and methods should be validated by comparison with a standard method, or analysis of a certified reference material. Simple spiking recoveries may not be sufficient. The developed method should especially comprise information on selectivity, sensitivity, detection limits, accuracy, and reliability. However, applying official validation or robustness studies to a routine method or technique does not necessarily constitute novelty. Proper statistical treatment of the data should be provided. Relevant literature should be cited, including related publications by the authors, and authors should discuss how their proposed methodology compares with previously reported methods.