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基于鲁米诺/ MoS 量子点@沸石咪唑酯骨架-8 作为发射体的高灵敏度电致化学发光用于 microRNA 的超灵敏检测。

Highly Efficient Electrochemiluminescence Based on Luminol/MoS Quantum Dots@Zeolitic Imidazolate Framework-8 as an Emitter for Ultrasensitive Detection of MicroRNA.

机构信息

Key Laboratory of Luminescence Analysis and Molecular Sensing (Southwest University), Ministry of Education, College of Chemistry and Chemical Engineering, Southwest University, Chongqing 400715, PR China.

Department of Kidney, Southwest Hospital, The Third Military Medical University (Army Medical University), Chongqing 400038, China.

出版信息

Anal Chem. 2022 Jun 28;94(25):9106-9113. doi: 10.1021/acs.analchem.2c01444. Epub 2022 Jun 15.

Abstract

Herein, a highly efficient electrochemiluminescence (ECL) emitter, luminol/MoS quantum dots@zeolitic imidazolate framework-8 (Lu/MoS QDs@ZIF-8), with a positive charge was prepared to construct a novel luminol-HO-MoS QD ternary ECL system for ultrasensitive detection of microRNA-21 (miRNA-21). The porous Lu/MoS QDs@ZIF-8 was beneficial for reducing the accessible distance between various participants in the ternary system wherein co-reaction accelerator MoS QDs promoted HO to generate superoxide anion radicals (O), which instantaneously reacted with luminol to produce robust ECL signals. Simultaneously, the positively charged Lu/MoS QDs@ZIF-8 facilitated the enrichment of O to further improve the ECL efficiency of luminol. Impressively, compared with the traditional binary luminol-HO system, the ECL efficiency of this ternary system was increased by 12.7 times. In the aid of a target-cycled and endogenous adenosine triphosphate-driven signal amplification strategy, the biosensor with Lu/MoS QDs@ZIF-8 as an ECL emitter achieved ultrasensitive detection for miRNA-21 with a detection limit of 14.6 aM. This work provides a promising perspective to construct a highly efficient ECL ternary system for biomolecule detection and potential disease diagnosis.

摘要

在此,制备了一种带正电荷的高效电致化学发光(ECL)发射器,即发光氨/钼量子点@沸石咪唑酯骨架-8(Lu/MoS QDs@ZIF-8),用于构建新型发光氨-HO-钼量子点三元 ECL 体系,以超灵敏检测 microRNA-21(miRNA-21)。多孔的 Lu/MoS QDs@ZIF-8 有利于减少三元体系中各种参与者之间的可及距离,其中共反应加速剂 MoS QDs 促进 HO 生成超氧阴离子自由基(O),O 瞬间与发光氨反应产生强 ECL 信号。同时,带正电荷的 Lu/MoS QDs@ZIF-8 有利于 O 的富集,从而进一步提高发光氨的 ECL 效率。令人印象深刻的是,与传统的二元发光氨-HO 体系相比,该三元体系的 ECL 效率提高了 12.7 倍。在目标循环和内源性三磷酸腺苷驱动的信号放大策略的辅助下,以 Lu/MoS QDs@ZIF-8 为 ECL 发射器的生物传感器实现了对 miRNA-21 的超灵敏检测,检测限低至 14.6 aM。这项工作为构建用于生物分子检测和潜在疾病诊断的高效 ECL 三元体系提供了有前景的视角。

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