Li Ya-Jie, Cui Wei-Rong, Jiang Qiao-Qiao, Wu Qiong, Liang Ru-Ping, Luo Qiu-Xia, Qiu Jian-Ding
College of Chemistry, Nanchang University, Nanchang, 330031, China.
College of Materials and Chemical Engineering, Pingxiang University, Pingxiang, 337055, China.
Nat Commun. 2021 Aug 5;12(1):4735. doi: 10.1038/s41467-021-25013-8.
Electrochemiluminescence (ECL) plays a key role in analysis and sensing because of its high sensitivity and low background. Its wide applications are however limited by a lack of highly tunable ECL luminophores. Here we develop a scalable method to design ECL emitters of covalent organic frameworks (COFs) in aqueous medium by simultaneously restricting the donor and acceptor to the COFs' tight electron configurations and constructing high-speed charge transport networks through olefin linkages. This design allows efficient intramolecular charge transfer for strong ECL, and no exogenous poisonous co-reactants are needed. Olefin-linked donor-acceptor conjugated COFs, systematically synthesized by combining non-ECL active monomers with C or C symmetry, exhibit strong ECL signals, which can be boosted by increasing the chain length and conjugation of monomers. The present concept demonstrates that the highly efficient COF-based ECL luminophores can be precisely designed, providing a promising direction toward COF-based ECL phosphors.
由于具有高灵敏度和低背景,电化学发光(ECL)在分析和传感中发挥着关键作用。然而,其广泛应用受到缺乏高度可调节的ECL发光体的限制。在此,我们开发了一种可扩展的方法,通过将供体和受体同时限制在共价有机框架(COF)紧密的电子构型中,并通过烯烃连接构建高速电荷传输网络,在水性介质中设计COF的ECL发射体。这种设计允许进行高效的分子内电荷转移以实现强ECL,并且无需外源性有毒共反应物。通过将非ECL活性单体与C或C对称性相结合系统合成的烯烃连接供体-受体共轭COF表现出强ECL信号,可通过增加单体的链长和共轭来增强该信号。本概念证明了基于COF的高效ECL发光体可以精确设计,为基于COF的ECL磷光体提供了一个有前景的方向。