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基于无共反应物电化学发光发光体 Gd-MOF 和 [Ru(bpy)dppz] 的“光开关”分子的高灵敏度啶虫脒比率型适配体传感器的潜能解析

Potential-Resolved Ratiometric Aptasensor for Sensitive Acetamiprid Analysis Based on Coreactant-free Electrochemiluminescence Luminophores of Gd-MOF and "Light Switch" Molecule of [Ru(bpy)dppz].

机构信息

National Key Laboratory of Green Pesticide, International Joint Research Center for Intelligent Biosensing Technology and Health, College of Chemistry, Central China Normal University, Wuhan 430079, P. R. China.

Hubei Key Laboratory of Plasma Chemistry and Advanced Materials, Hubei Engineering Technology Research Center of Optoelectronic and New Energy Materials, Wuhan Institute of Technology, Wuhan 430205, P. R. China.

出版信息

Anal Chem. 2024 Mar 26;96(12):5022-5028. doi: 10.1021/acs.analchem.4c00364. Epub 2024 Mar 12.

Abstract

For conventional potential-resolved ratiometric electrochemiluminescence (ECL) systems, the introduction of multiplex coreactants is imperative. However, the undesirable interactions between different coreactants inevitably affect analytical accuracy and sensitivity. Herein, through the coordination of aggregation-induced emission ligands with gadolinium cations, the self-luminescent metal-organic framework (Gd-MOF) is prepared and serves as a novel coreactant-free anodic ECL emitter. By the intercalation of [Ru(bpy)dppz] with light switch effect into DNA duplex, one high-efficiency cathodic ECL probe is obtained using KSO as a coreactant. In the presence of acetamiprid, the strong affinity between the target and its aptamer induces the release of [Ru(bpy)dppz], resulting in a decreasing cathode signal and an increasing anode signal owing to the ECL resonance energy transfer from Gd-MOF to [Ru(bpy)dppz]. In this way, an efficient dual-signal ECL aptasensor is constructed for the ratiometric analysis of acetamiprid, exhibiting a remarkably low detection limit of 0.033 pM. Strikingly, by using only one exogenous coreactant, the cross interference from multiple coreactants can be eliminated, thus improving the detection accuracy. The developed high-performance ECL sensing platform is successfully applied to monitor the residual level of acetamiprid in real samples, demonstrating its potential application in the field of food security.

摘要

对于传统的势分辨比率电化学发光(ECL)系统,引入多重共反应物是必不可少的。然而,不同共反应物之间的不良相互作用不可避免地会影响分析的准确性和灵敏度。在此,通过聚集诱导发射配体与钆阳离子的配位,制备了自发光的金属有机骨架(Gd-MOF),并将其用作新型无共反应物的阳极 ECL 发射器。通过将具有光开关效应的[Ru(bpy)dppz]插入 DNA 双链体中,使用 KSO 作为共反应物,获得了一种高效的阴极 ECL 探针。在啶虫脒存在的情况下,目标物与其适体之间的强亲和力诱导[Ru(bpy)dppz]的释放,导致由于 ECL 共振能量从 Gd-MOF 转移到[Ru(bpy)dppz],阴极信号减小,阳极信号增加。通过这种方式,构建了一种用于啶虫脒比率分析的高效双信号 ECL 适体传感器,具有非常低的检测限为 0.033 pM。引人注目的是,通过仅使用一种外源性共反应物,可以消除多种共反应物的交叉干扰,从而提高检测准确性。所开发的高性能 ECL 传感平台成功应用于监测实际样品中啶虫脒的残留水平,展示了其在食品安全领域的潜在应用。

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