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共反应物介导的低电位阳极电化学发光平台及其免疫传感应用。

Co-Reactant-Mediated Low-Potential Anodic Electrochemiluminescence Platform and Its Immunosensing Application.

机构信息

Department of Laboratory Medicine, Xiamen Key Laboratory of Genetic Testing, the First Affiliated Hospital of Xiamen University, School of Medicine, Xiamen University, Xiamen 361003, China.

School of Clinical Medicine, Fujian Medical University, Fuzhou 350004, China.

出版信息

Anal Chem. 2022 Sep 13;94(36):12500-12506. doi: 10.1021/acs.analchem.2c02726. Epub 2022 Aug 31.

DOI:10.1021/acs.analchem.2c02726
PMID:36044018
Abstract

Screening high-performance anodic electrochemiluminescence (ECL) systems with low triggering potential is a promising way to broaden their applications. In addition to electrochemiluminophore, co-reactant also plays an important role in the ECL process, since the oxidation of co-reactants is one of the most important steps in the anodic ECL process. Herein, a novel co-reactant-mediated high-performance low-potential Au nanocluster (AuNC)-based ECL system has been successfully developed. Benefiting from the isopropyl substitution and hydroxyl addition to the triethylamine (TEA), the BSA-AuNC/2-(diisopropylamino)ethanol (DIPEA-OH) ECL system achieved higher energy efficiency at a lower potential of 0.75 V. In addition, compared with the BSA-AuNC/TEA system, the ECL intensity and quantum yield () with DIPEA-OH as a co-reactant increased 22.34-fold and 13-fold (as high as 68.17%), respectively. Based on the low potential, high of the AuNC/DIPEA-OH ECL system, a sandwich-type immunosensor has been constructed for a highly selective SARS-CoV-2 N protein assay. In the absence of any complex signal amplification strategies, the ECL immunosensor for the SARS-CoV-2 N protein detection showed a linear range of 0.001-100 ng/mL and a detection limit of 0.35 pg/mL. Moreover, the ECL platform had good reproducibility and stability and exhibited acceptable detection performance in the detection of actual serum samples. This work established a framework for in-depth design and study of anode ECL co-reactants for AuNCs and other luminophores, and expanded the potential application of ECL sensors in the clinical diagnosis of COVID-19.

摘要

筛选具有低触发电位的高性能阳极电致化学发光 (ECL) 体系是拓宽其应用的一种有前途的方法。除了电致发光体之外,共反应物在 ECL 过程中也起着重要作用,因为共反应物的氧化是阳极 ECL 过程中最重要的步骤之一。在此,成功开发了一种新型的共反应物介导的高性能低电位 Au 纳米团簇 (AuNC) 基 ECL 体系。由于三乙胺 (TEA) 的异丙基取代和羟基加成,BSA-AuNC/2-(二异丙基氨基)乙醇 (DIPEA-OH) ECL 体系在 0.75 V 的更低电位下实现了更高的能量效率。此外,与 BSA-AuNC/TEA 体系相比,以 DIPEA-OH 作为共反应物的 ECL 强度和量子产率 () 分别增加了 22.34 倍和 13 倍(高达 68.17%)。基于 AuNC/DIPEA-OH ECL 体系的低电位、高,构建了用于高选择性 SARS-CoV-2 N 蛋白检测的三明治型免疫传感器。在没有任何复杂信号放大策略的情况下,用于 SARS-CoV-2 N 蛋白检测的 ECL 免疫传感器的线性范围为 0.001-100ng/mL,检测限为 0.35pg/mL。此外,ECL 平台具有良好的重现性和稳定性,在实际血清样品的检测中表现出可接受的检测性能。这项工作为深入设计和研究 AuNC 及其它发光体的阳极 ECL 共反应物奠定了基础,并扩展了 ECL 传感器在 COVID-19 临床诊断中的潜在应用。

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