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用于汞(II)专属检测的可再生氨基功能化荧光共价有机框架的合理设计

Rational Design of Regenerable Amino-Functionalized Fluorescent Covalent Organic Framework for the Exclusive Detection of Mercury(II).

作者信息

Ren Yanbiao, Hou Yuzhen, Song Jusuo, Zhi Desheng, Li Ning, Yu Yanxin, Zhu Dandan

机构信息

College of Chemistry, Chemical Engineering and Materials Science, Zaozhuang University, Zaozhuang 277160, China.

Beijing National Laboratory for Molecular Sciences, CAS Key Laboratory of Engineering Plastics, Institute of Chemistry, Chinese Academy of Sciences, Beijing 100190, China.

出版信息

Langmuir. 2024 Oct 29;40(43):22990-22996. doi: 10.1021/acs.langmuir.4c03186. Epub 2024 Oct 15.

Abstract

Goal-oriented development of novel covalent organic frameworks (COFs) to construct a sensing platform for highly toxic mercury (II, Hg) is of tremendous significance. Recently, numerous COFs with sulfur-based ligands were developed for Hg monitoring; however, strong binding of Hg by sulfur makes their regeneration very tough. Herein, we designed and developed an amino-functionalized fluorescent COF (COF-NH) through facile postmodification for Hg detection in which the π-conjugation skeleton is the signal reader and the nitrogen-based side is the highly selective Hg receptor. More importantly, this nitrogen-based receptor permits the reversible binding of Hg. As a sensing platform, the outstanding performance of COF-NH for Hg detection was reached with respect to high sensitivity with an ultralow detection of 15.3 nM, real-time response with rapid signal change of 10 s, and facile visualization with significant fluorescence color change. Expectedly, COF-NH obtained facile recycling which still shows excellent response performance toward Hg after six cycles based on the reversible interaction between amino groups and Hg. Our work not only shows an attractive foreground of fluorescent COF for Hg detection but also emphasizes the easy construction of novel COF materials via the rational introduction of metal ligands for the recognition of other metal ions.

摘要

以目标为导向开发新型共价有机框架(COF)以构建用于检测剧毒汞(II,Hg)的传感平台具有极其重要的意义。最近,开发了许多具有硫基配体的COF用于汞监测;然而,硫与汞的强结合使得它们的再生非常困难。在此,我们通过简便的后修饰设计并开发了一种氨基功能化荧光COF(COF-NH)用于汞检测,其中π共轭骨架是信号读取器,氮基侧是高选择性汞受体。更重要的是,这种氮基受体允许汞的可逆结合。作为传感平台,COF-NH在汞检测方面表现出色,具有15.3 nM的超低检测限的高灵敏度、10秒快速信号变化的实时响应以及显著荧光颜色变化的简便可视化。预期,基于氨基与汞之间的可逆相互作用,COF-NH实现了简便的循环利用,在六个循环后仍对汞表现出优异的响应性能。我们的工作不仅展示了荧光COF在汞检测方面的诱人前景,还强调了通过合理引入金属配体来识别其他金属离子从而轻松构建新型COF材料的方法。

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