School of Chemistry and Chemical Engineering, Nanchang University, Nanchang, 330031, PR China.
State Key Laboratory of Nuclear Resources and Environment, East China University of Technology (ECUT), Nanchang, 330013, PR China.
Anal Chim Acta. 2023 Apr 29;1252:341056. doi: 10.1016/j.aca.2023.341056. Epub 2023 Mar 6.
Previous researches of covalent organic frameworks (COFs) have shown their potential as fluorescent probes, but the regulation of their optical properties and recognition characteristics still remains a challenge, and most of reports required complicated post-decoration to improve the sensing performance. In this context, we propose a novel in-situ strategy to construct uracil-conjugated COFs and modulate their fluorescence properties for sensitive and selective mercury(II) detection. By using 1,3,6,8-tetrakis(4-formylphenyl)pyrene (TFPPy) and 1,3,6,8-tetrakis(4-aminophenyl)pyrene (TAPPy) as fundamental blocks and 5-aminouraci (5-AU) as the functional monomer, a series of COFs (Py-COFs and Py-U-COFs-1 to Py-U-COFs-5) with tunable fluorescence were solvothermally synthesized through an in-situ Schiff base reaction. The π-conjugated framework serves as a signal reporter, the evenly and densely distributed uracil acts as a mercury(II) receptor, and the regular pores (channels) make the rapid and sensitive detection of the mercury(II) possible. In this research, we manage to regulate the crystalline structure, the fluorescence properties, and the sensing performance of COFs by simply changing the molar ratio of precursors. We expect this research to open up a new strategy for effective and controllable construction of functionalized COFs for environmental analysis.
先前关于共价有机骨架(COFs)的研究表明,它们具有作为荧光探针的潜力,但调节其光学性质和识别特性仍然是一个挑战,而且大多数报道都需要复杂的后修饰来提高传感性能。在这种情况下,我们提出了一种构建尿嘧啶结合 COFs 的新原位策略,并调节其荧光性质,以实现对汞(II)的敏感和选择性检测。我们使用 1,3,6,8-四(4-醛基苯基)芘(TFPPy)和 1,3,6,8-四(4-氨基苯基)芘(TAPPy)作为基本砌块,5-氨基尿嘧啶(5-AU)作为功能单体,通过原位席夫碱反应,溶剂热合成了一系列具有可调荧光的 COFs(Py-COFs 和 Py-U-COFs-1 至 Py-U-COFs-5)。共轭骨架作为信号报告器,均匀且密集分布的尿嘧啶作为汞(II)受体,而规则的孔(通道)使得对汞(II)的快速和灵敏检测成为可能。在这项研究中,我们通过简单地改变前体的摩尔比,成功地调节了 COFs 的结晶结构、荧光性质和传感性能。我们希望这项研究为环境分析中有效和可控的功能化 COFs 的构建开辟一条新的策略。