Electrochemiluminescence enhanced by isolating ACQphores in imine-linked covalent organic framework for organophosphorus pesticide assay

IF 5.6 1区化学 Q1 CHEMISTRY, ANALYTICAL

Talanta Pub Date : 2023-07-19 DOI:10.1016/j.talanta.2023.124964

Linlin Song , Qian Zhang , Lei Min , Xinyu Guo , Wenqiang Gao , Lin Cui , Chun-yang Zhang

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引用次数: 1

Abstract

Most of covalent organic frameworks (COFs) are non or weakly emissive due to either the molecular thermal motion-mediated energy dissipation or the aggregation-caused quenching (ACQ) effect. Herein, we synthesize an imine-linked COF (TFPPy-TPh-COF) with high electrochemiluminescence (ECL) emission and the capability of eliminating the ACQ effect and further construct an ECL sensor for malathion detection. The imine-linked COF is obtained by the condensation reaction of (1,1':3′,1″-terphenyl)-4,4″-diamine (TPh) and 1,3,6,8-tetrakis(p-formylphenyl)pyrene (TFPPy), and it has higher ECL efficiency than TFPPy aggregates due to the separation of ACQ luminophores (i.e., TFPPy) from each other by TPh and the restriction of intramolecular motions of TFPPy and TPh to reduce the nonradiative decay. The efficient quenching of ECL is achieved by electrochemiluminescence resonance energy transfer (ERET) from the excited state of the TFPPy-TPh-COF to zeolite imidazolate framework-8 (ZIF-8) and the steric hindrance of ZIF-8. Acetylcholinesterase (AChE) can enzymatically hydrolyze acetylcholine (ACh) to generate acetic acid. The resultant acetic acid can trigger the dissolution of ZIF-8 to produce an enhanced ECL signal. Malathion as an organophosphorus pesticide serves as an AChE inhibitor to prevent the production of acetic acid, inducing the decrease of ECL signal. This sensor displays a limit of detection (LOD) of 2.44 pg/mL and a wide dynamic detection range of 0.01–1000 ng/mL. Furthermore, it can be used to detect other organophosphates pesticides (e.g., methidathion, chlorpyrifos, and paraoxon) and measure malathion in real samples (i.e., pakchoi, lettuce, and apples).

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在亚胺连接的共价有机框架中分离ACQ载体增强电化学发光用于有机磷农药测定。

由于分子热运动介导的能量耗散或聚集引起的猝灭（ACQ）效应，大多数共价有机框架（COFs）是非发射或弱发射的。在此，我们合成了一种具有高电化学发光（ECL）发射和消除ACQ效应的亚胺连接的COF（TFPPy-TPh-COF），并进一步构建了一种用于马拉硫磷检测的ECL传感器。亚胺连接的COF是由（1，1’：3’，1〃-三苯基）-4，4〃-二胺（TPh）和1，3，6，8-四（对甲酰基苯基）芘（TFPPy）的缩合反应获得的，由于TPh使ACQ发光体（即TFPPy，TFPPy的相互分离以及TFPPy和TPh的分子内运动受到限制以减少非辐射衰变，因此它比TFPPy聚集体具有更高的ECL效率。ECL的有效猝灭是通过电化学发光共振能量转移（ERET）从TFPPy-TPh-COF的激发态到咪唑酸分子筛骨架-8（ZIF-8）和ZIF-8的空间位阻实现的。乙酰胆碱酯酶（AChE）可以酶解乙酰胆碱（ACh）生成乙酸。得到的乙酸可以触发ZIF-8的溶解以产生增强的ECL信号。马拉硫磷作为一种有机磷农药，可作为乙酰胆碱酯酶抑制剂阻止乙酸的产生，诱导ECL信号的降低。该传感器的检测限（LOD）为2.44 pg/mL，动态检测范围为0.01-1000 ng/mL。此外，它还可用于检测其他有机磷农药（如对硫磷、毒死蜱和对氧磷），并测量真实样品（如小白菜、生菜和苹果）中的马拉硫磷。

本文章由计算机程序翻译，如有差异，请以英文原文为准。

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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.