Deng Chuti, Xu Juntong, Zhang Qi, Fan Yong
Department of Chemistry, Fudan University, Shanghai, China.
Shanghai RNA Cure Biopharma Co., Ltd., Shanghai, China.
Front Chem. 2024 Jun 5;12:1399519. doi: 10.3389/fchem.2024.1399519. eCollection 2024.
Developing a convenient and cost-effective platform for detecting homocysteine (Hcy) is of great interest as Hcy has been found to be a biomarker for Alzheimer's disease, gastric cancer, and other diseases. In this study, we synthesized five phosphorescent Ir(CN)(NN) compounds (Irn, n = 1-5) with various substituents (-CHO or -CHO/-NH), which were then doped into a covalent organic framework (COF) host via covalent bonding. The resulting optimal composites (denoted as Ir4/5@EBCOF) with -CHO/-NH substituents not only overcame the self-quenching issue of the bare Ir4/5 complexes but also showed rapid, highly selective, and sensitive detection of Hcy, with a limit of detection (LOD) of 0.23 μM and reaction time of 88 s. The sensing mechanism was revealed as the unique cyclization reaction between Ir(III) and Hcy that forms a six-membered ring. During the process, the color changes in the composites can be observed visually. It is expected that these phosphorescent Iridium (III) complexes with COFs will have the potential to serve as promising platforms for detecting thiols.
开发一种便捷且经济高效的同型半胱氨酸（Hcy）检测平台具有重大意义，因为Hcy已被发现是阿尔茨海默病、胃癌和其他疾病的生物标志物。在本研究中，我们合成了五种带有不同取代基（-CHO或-CHO/-NH）的磷光Ir(CN)(NN)化合物（Irn，n = 1 - 5），然后通过共价键将它们掺杂到共价有机框架（COF）主体中。所得具有-CHO/-NH取代基的最佳复合材料（表示为Ir4/5@EBCOF）不仅克服了裸Ir4/5配合物的自猝灭问题，还对Hcy表现出快速、高选择性和灵敏的检测，检测限（LOD）为0.23 μM，反应时间为88秒。传感机制被揭示为Ir(III)与Hcy之间独特的环化反应，形成一个六元环。在此过程中，可以直观地观察到复合材料的颜色变化。预计这些与COF结合的磷光铱（III）配合物有潜力成为检测硫醇的有前景的平台。
