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<p>Controlling the intermolecular charge transfer between co-reactants and emitters represents a promising strategy for elucidating the luminescent mechanism and enhancing the efficiency of electrochemiluminescence (ECL) systems. Herein, a self-enhanced ECL microreactor was prepared by bimetallic Zn-/Co-porphyrin covalent organic framework (COF<sub>Zn/CoP−Ph</sub>@MWCNTs), in which co-reaction accelerators (cobalt porphyrin) and luminophores (zinc porphyrin) were precisely woven into the COFs skeleton via covalent bonds. Owing to the unique topological structure, the rational arrangement of co-reaction accelerators and luminophores in a spatially confined environment effectively controlled the intermolecular charge transfer. And the spatially restricted environment formed by the COF<sub>Zn/CoP−Ph</sub>@MWCNTs microreactor avoided the problem of disordered diffusion of active intermediates, leading to an enhanced ECL response. Thanks to the synergistic impacts of the factors above, the ECL intensity of the bimetallic COF<sub>Zn/CoP−Ph</sub>@MWCNTs was 10.2-folds stronger than the zinc porphyrin monomer. Therefore, the self-enhanced ECL sensor was constructed for miRNA-155 detection via an “on-off” ECL quenching mechanism and a cycling amplification strategy, displayed a broad linear range (0.10 pM–10 µM) and a low limit of detection (0.51 fM). In brief, studying the programmable structures and tunable electronic paths of high-performance COF materials would provide good access for the engineering self-enhanced ECL system and the construction of ultrasensitive sensors.</p>

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Self-Enhanced Electrochemiluminescence Microreactors Based on Bimetallic Porphyrin Covalent Organic Frameworks for MicroRNA Detection

  • 期刊论文

  • 发表日期：

    2025年11月17日

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  • Lina Zhang,
  • Wenqing Gao,
  • Liying Zhang,
  • Xiaojie Ma,
  • Yan Zhang,
  • Peihua Zhu,
  • Jinghua Yu

摘要

Controlling the intermolecular charge transfer between co-reactants and emitters represents a promising strategy for elucidating the luminescent mechanism and enhancing the efficiency of electrochemiluminescence (ECL) systems. Herein, a self-enhanced ECL microreactor was prepared by bimetallic Zn-/Co-porphyrin covalent organic framework (COFZn/CoP−Ph@MWCNTs), in which co-reaction accelerators (cobalt porphyrin) and luminophores (zinc porphyrin) were precisely woven into the COFs skeleton via covalent bonds. Owing to the unique topological structure, the rational arrangement of co-reaction accelerators and luminophores in a spatially confined environment effectively controlled the intermolecular charge transfer. And the spatially restricted environment formed by the COFZn/CoP−Ph@MWCNTs microreactor avoided the problem of disordered diffusion of active intermediates, leading to an enhanced ECL response. Thanks to the synergistic impacts of the factors above, the ECL intensity of the bimetallic COFZn/CoP−Ph@MWCNTs was 10.2-folds stronger than the zinc porphyrin monomer. Therefore, the self-enhanced ECL sensor was constructed for miRNA-155 detection via an “on-off” ECL quenching mechanism and a cycling amplification strategy, displayed a broad linear range (0.10 pM–10 µM) and a low limit of detection (0.51 fM). In brief, studying the programmable structures and tunable electronic paths of high-performance COF materials would provide good access for the engineering self-enhanced ECL system and the construction of ultrasensitive sensors.