Jiangsu Key Laboratory of Advanced Catalytic Materials and Technology, School of Petrochemical Engineering, Changzhou University, Changzhou 213164, China.
Advanced Catalysis and Green Manufacturing Collaborative Innovation Center, Changzhou University, Changzhou 213164, China.
ACS Appl Mater Interfaces. 2023 Dec 6;15(48):55369-55378. doi: 10.1021/acsami.3c12201. Epub 2023 Nov 21.
Signal amplification is a powerful approach to increasing the detection sensitivity of electrochemiluminescence (ECL). Here, we developed synergistic multieffect catalytic strategies based on CuCoO nanorod combination of Ag NPs as coreaction accelerators to fabricate an efficient covalent organic framework (PTCA-COF)-based ternary ECL biosensor. Concretely, the high redox reversibility of Co/Co and Cu/Cu would constantly promote the decomposition of SO for ECL emission. Meanwhile, the introduction of Ag NPs with excellent electrocatalytic activity further realized multiple amplification of the ECL signal. Furthermore, the good hydrogen evolution reaction (HER) ability of Ag@CuCoO nanorods could accelerate the proton transmission rate of the system to amplify ECL behavior. In the presence of the target synthetic cathinone 4-chloroethcathinone (4-CEC) as the quenching ECL signal-response probe, the Ferrocene (Fc)-labeled aptamer folded into the conformationally limited stem-loop structure, bringing Fc near the ECL luminophore and resulting in quenched ECL emission. The quenching effect was connected with target-induced aptamer conformational changes and consequently reflected the target concentration. Under optimum conditions, the proposed biosensor realized a highly sensitive assay for 4-CEC with a large dynamic range from 1.0 × 10 to 1.0 × 10 g/L and a detection limit as low as 2.5 × 10 g/L. This study integrated multiple amplification strategies for efficient ECL enhancement, which provided a novel approach to constructing highly bioactive and sensitive sensors.
信号放大是提高电化学发光（ECL）检测灵敏度的一种有效方法。在这里，我们开发了基于 CuCoO 纳米棒结合 Ag NPs 的协同多效催化策略作为共反应加速剂，制备了一种高效的共价有机框架（PTCA-COF）基三元 ECL 生物传感器。具体来说，Co/Co 和 Cu/Cu 的高氧化还原可逆性会不断促进 SO 的分解以产生 ECL 发射。同时，引入具有优异电催化活性的 Ag NPs 进一步实现了 ECL 信号的多重放大。此外，Ag@CuCoO 纳米棒良好的析氢反应（HER）能力可以加速体系中质子的传递速率，从而放大 ECL 行为。在作为淬灭 ECL 信号响应探针的目标合成苯丙胺 4-氯乙基卡西酮（4-CEC）存在下，标记有 Ferrocene（Fc）的适配体折叠成构象受限的茎环结构，使 Fc 靠近 ECL 发光体，导致 ECL 发射被猝灭。猝灭效应与靶标诱导的适配体构象变化有关，因此反映了靶标浓度。在最佳条件下，该生物传感器实现了对 4-CEC 的高灵敏度检测，线性范围从 1.0×10 到 1.0×10 g/L，检测限低至 2.5×10 g/L。本研究集成了多种放大策略以实现有效的 ECL 增强，为构建高生物活性和高灵敏度的传感器提供了一种新方法。
