基于羧基化钌（II）配合物的多重信号增强电化学发光适体传感器用于检测吡虫啉。
Multiple signal-enhanced electrochemiluminescence aptamer sensors based on carboxylated ruthenium (II) complexes for acetamiprid detection.
机构信息
Provincial Key Laboratory of Rural Energy Engineering in Yunnan, Yunnan Normal University, Kunming, 650500, People's Republic of China; Collaborative Innovation Center for Green Chemical Manufacturing and Accurate Detection, Key Laboratory of Interfacial Reaction & Sensing Analysis in Universities of Shandong, School of Chemistry and Chemical Engineering, University of Jinan, Jinan, 250022, People's Republic of China.
Provincial Key Laboratory of Rural Energy Engineering in Yunnan, Yunnan Normal University, Kunming, 650500, People's Republic of China.
出版信息
Anal Chim Acta. 2024 Jun 22;1309:342677. doi: 10.1016/j.aca.2024.342677. Epub 2024 May 6.
BACKGROUND
Rapid and sensitive detection for acetamiprid, a kind of widely used neonicotinoid insecticide, is very meaningful for the development of modern agriculture and the protection of human health. Highly stable electrochemiluminescence (ECL) materials are one of the key factors in ECL sensing technology. ECL materials prepared by porous materials (e.g., MOFs) coated with chromophores have been used for ECL sensing detection, but these materials have poor stability because the chromophores escape when they are in aqueous solution. Therefore, the development of highly stable ECL materials is of great significance to improve the sensitivity of ECL sensing technology.
RESULTS
In this work, by combining etched metal-organic frameworks (E-UIO-66-NH) as carrier with Tris(4,4'-dicarboxylic acid-2,2'-bipyridine)Ru(II) chloride (Ru(dcbpy)) as signal probe via amide bonds, highly stable nanocomposites (E-UIO-66-NH-Ru) with excellent ECL performance were firstly prepared. Then, using MoS loaded with AuNPs as substrate material and co-reactant promoter, a signal off-on-off ECL aptamer sensor was prepared for sensitive detection of acetamiprid. Due to the excellent catalytic activity of E-UIO-66-NH-Ru and MoS@Au towards KSO, the ECL signals can be enhanced by multiple signal enhancement pathways, the prepared ECL aptamer sensor could achieve sensitive detection of acetamiprid in the linear range of 10 to10 mol L, with the limit of detection (LOD) of 2.78ⅹ10 mol L (S/N = 3). After the evaluation of actual sample testing, this sensing platform was proven to be an effective method for the detection of acetamiprid in food and agricultural products.
SIGNIFICANCE AND NOVELTY
The E-UIO-66-NH-Ru prepared by linking Ru(dcbpy) to E-UIO-66-NH via amide bonding has very high stability. The synergistic catalytic effect of MoS and AuNPs enhanced the ECL signal. By exploring the sensing mechanism and evaluating the actual sample tests, the proposed signal "on-off" ECL sensing strategy was proved to be an effective and excellent ECL sensing method for sensitive and stable detection of acetamiprid.
背景
快速灵敏地检测乙虫腈（一种广泛使用的新烟碱类杀虫剂）对于现代农业的发展和人类健康的保护具有重要意义。高稳定性的电致化学发光（ECL）材料是 ECL 传感技术的关键因素之一。用染料修饰的多孔材料（如 MOFs）制备的 ECL 材料已被用于 ECL 传感检测，但这些材料在水溶液中稳定性差，因为当染料处于水溶液中时会逸出。因此，开发高稳定性的 ECL 材料对于提高 ECL 传感技术的灵敏度具有重要意义。
结果
在这项工作中，通过将刻蚀的金属-有机骨架（E-UIO-66-NH）作为载体，通过酰胺键与三（4,4'-二羧酸-2,2'-联吡啶）钌（II）氯化物（Ru（dcbpy））结合，首次制备了具有优异 ECL 性能的高稳定性纳米复合材料（E-UIO-66-NH-Ru）。然后，以负载 AuNPs 的 MoS 作为基底材料和共反应物促进剂，制备了一种信号关-开-关 ECL 适体传感器，用于灵敏检测乙虫腈。由于 E-UIO-66-NH-Ru 和 MoS@Au 对 KSO 的出色催化活性，通过多种信号增强途径可以增强 ECL 信号，所制备的 ECL 适体传感器可以在 10 到 10-5 mol·L-1 的线性范围内实现对乙虫腈的灵敏检测，检测限（LOD）为 2.78×10-5 mol·L-1（S/N=3）。通过实际样品测试评估后，证明该传感平台是检测食品和农产品中乙虫腈的有效方法。
意义和创新性
通过酰胺键将 Ru（dcbpy）连接到 E-UIO-66-NH 制备的 E-UIO-66-NH-Ru 具有非常高的稳定性。MoS 和 AuNPs 的协同催化作用增强了 ECL 信号。通过探索传感机制并评估实际样品测试，证明了所提出的信号“开-关”ECL 传感策略是一种有效且出色的 ECL 传感方法，可用于灵敏稳定地检测乙虫腈。
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