化学
铀酰
离子
阳离子聚合
选择性
发光
检出限
质子化
金属有机骨架
背景(考古学)
猝灭(荧光)
离子键合
荧光
水溶液中的金属离子
无机化学
锕系元素
组合化学
物理化学
吸附
高分子化学
有机化学
色谱法
古生物学
物理
光电子学
量子力学
生物
催化作用
作者
Supriya Mondal,Annette Mariya Tedy,Santanu Chand,Rupam Sahoo,Arun K. Manna,Madhab C. Das
出处
期刊:Inorganic Chemistry
[American Chemical Society]
日期:2024-05-18
卷期号:63 (22): 10403-10413
被引量:5
标识
DOI:10.1021/acs.inorgchem.4c01422
摘要
Development of a simple, cost-efficient, and portable UO22+ sensory probe with high selectivity and sensitivity is highly desirable in the context of monitoring radioactive contaminants. Herein, we report a luminescent Co-based metal–organic framework (MOF), {[Me2NH2]0.5[Co(DATRz)0.5(NH2BDC)]·xG}n (1), equipped with abundant amino functionalities for the selective detection of uranyl cations. The ionic structure consists of two types of channels decorated with plentiful Lewis basic amino moieties, which trigger a stronger acid–base interaction with the diffused cationic units and thus can selectively quench the fluorescence intensity in the presence of other interfering ions. Furthermore, the limit of detection for selective UO22+ sensing was achieved to be as low as 0.13 μM (30.94 ppb) with rapid responsiveness and multiple recyclabilities, demonstrating its excellent efficacy. Density functional theory (DFT) calculations further unraveled the preferred binding sites of the UO22+ ions in the tubular channel of the MOF structure. Orbital hybridization between NH2BDC/DATRz and UO22+ together with its significantly large electron-accepting ability is identified as responsible for the luminescence quenching. More importantly, the prepared 1@PVDF {poly(vinylidene difluoride)} mixed-matrix membrane (MMM) displayed good fluorescence activity comparable to 1, which is of great significance for their practical employment as MOF-based luminosensors in real-world sensing application.
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