Scholarlink

<p>Precise incorporation of metal single-atom (SA) active sites into covalent organic frameworks (COFs) offers a powerful approach to enhance electrochemiluminescence (ECL) by facilitating co-reactant activation and charge transport. However, metal coordination usually triggers intramolecular electron-transfer quenching that degrades the ECL efficiency of COFs. Herein, we construct a pyrene-phenanthroline COF with coordinated Ag SA (Ag<sub>SA</sub>/PP-COF) that breaks the catalysis-quenching dilemma of metals, achieving enhanced ECL performance. Density functional theory calculations reveal that, among the screened metal catalysts, the <i>d</i><sup>10</sup>-configurated Ag (I) center exhibits the weakest electron coupling with the nitrogen atoms of PP-COF’s phenanthroline units. This minimal perturbation ensures that the framework’s intrinsic luminescence is largely retained. Specifically, Ag<sub>SA</sub> serves as highly efficient active sites, facilitating co-reactant adsorption and activation while accelerating interfacial electron transfer kinetics. Remarkably, the resultant Ag<sub>SA</sub>/PP-COF exhibits a 4.5-fold enhancement in ECL intensity. Moreover, Ag<sub>SA</sub>/PP-COF enables the construction of a highly sensitive ECL enzymatic biosensor for organophosphorus pesticide detection. This work provides a universal strategy for the design of high-performance solid-state ECL emitters.</p>

错误：搜索内容不能为空，请输入英文关键词
错误：关键词超出字数限制，请精简
高级检索

Breaking the catalysis-quenching dilemma in covalent organic frameworks with metal single-atom sites for enhanced electrochemiluminescence

  • 期刊论文

  • 出版模式：

    开放获取

  • 发表日期：

    2026年5月6日

查看全文
  • Haifei Wan,
  • Yuxin Du,
  • Juan He,
  • Yifei Chen,
  • Jingshuai Li,
  • Ying Qin,
  • Ruimin Li,
  • Liuyong Hu,
  • Wenling Gu,
  • Han Yu,
  • Chengzhou Zhu

摘要

Precise incorporation of metal single-atom (SA) active sites into covalent organic frameworks (COFs) offers a powerful approach to enhance electrochemiluminescence (ECL) by facilitating co-reactant activation and charge transport. However, metal coordination usually triggers intramolecular electron-transfer quenching that degrades the ECL efficiency of COFs. Herein, we construct a pyrene-phenanthroline COF with coordinated Ag SA (AgSA/PP-COF) that breaks the catalysis-quenching dilemma of metals, achieving enhanced ECL performance. Density functional theory calculations reveal that, among the screened metal catalysts, the d10-configurated Ag (I) center exhibits the weakest electron coupling with the nitrogen atoms of PP-COF’s phenanthroline units. This minimal perturbation ensures that the framework’s intrinsic luminescence is largely retained. Specifically, AgSA serves as highly efficient active sites, facilitating co-reactant adsorption and activation while accelerating interfacial electron transfer kinetics. Remarkably, the resultant AgSA/PP-COF exhibits a 4.5-fold enhancement in ECL intensity. Moreover, AgSA/PP-COF enables the construction of a highly sensitive ECL enzymatic biosensor for organophosphorus pesticide detection. This work provides a universal strategy for the design of high-performance solid-state ECL emitters.