Qi Hongjie, Wang Zhixin, Li Haiyin, Li Feng
College of Chemistry and Pharmaceutical Sciences, Qingdao Agricultural University, Qingdao 266109, PR China.
College of Chemistry and Molecular Engineering, Qingdao University of Science and Technology, Qingdao 266042, PR China.
Anal Chem. 2023 Aug 15;95(32):12024-12031. doi: 10.1021/acs.analchem.3c01882. Epub 2023 Aug 1.
Manufacturing electrochemiluminescence (ECL) electrodes to detect analytes with high performance in the aqueous phase for water-insoluble metal complexes is a great challenge. Here, a directional self-assembling avenue for in situ fabricating iridium(III)-polyimine complex-encapsulated metal-organic framework (MOF) two-dimensional electrode Hf-MOF/IrPD/APS/ITO is developed. The electrode displayed bright red ECL emission with high stability in the aqueous phase and specific adsorption toward ssDNA against dsDNA and mNs. That is to say, a "high-performance and multifunctional ECL electrode" is presented and explored for sensitive detection of acetamiprid (Ace) with a limit of detection of 0.0025 nM, where Ace-aptamer recognition-switched Exonuclease III-mediated digestion to make large numbers of Fc-labeled ssDNA transform into Fc-mNs. Furthermore, the proposed method was triumphantly employed to monitor the change in the residual concentration of Ace in pakchoi. This work breaks through the bottleneck of metal complex-based ECL emission in organic solvents and provides a novel strategy to develop high-performance ECL sensors.
制造用于在水相中高效检测水不溶性金属配合物分析物的电化学发光(ECL)电极是一项巨大挑战。在此,开发了一种用于原位制备铱(III)-聚亚胺配合物封装的金属有机框架(MOF)二维电极Hf-MOF/IrPD/APS/ITO的定向自组装途径。该电极在水相中表现出明亮的红色ECL发射,具有高稳定性,并且对单链DNA(ssDNA)相对于双链DNA(dsDNA)和单链错配(mNs)具有特异性吸附。也就是说,提出并探索了一种“高性能和多功能ECL电极”,用于灵敏检测啶虫脒(Ace),检测限为0.0025 nM,其中Ace-适配体识别开关外切核酸酶III介导的消化使大量Fc标记的ssDNA转化为Fc-mNs。此外,所提出的方法成功用于监测小白菜中Ace残留浓度的变化。这项工作突破了基于金属配合物的ECL发射在有机溶剂中的瓶颈,并为开发高性能ECL传感器提供了一种新策略。