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基于供体-受体结构共价有机框架增强纳米酶活性的先进“开启”比色铀检测平台。

Advanced "turn-on" colorimetric uranium platform based on the enhanced nanozyme activity of a donor-acceptor structured covalent organic framework.

作者信息

Xiao Sai Jin, Huang Jing, Qiu An Ting, Liu Guang Zhou, Zhang Li, Wu Ting, Shi Ya Di, Qiu Jian-Ding

机构信息

State Key Laboratory of Nuclear Resources and Environment, East China University of Technology, Nanchang, 330013, Jiangxi, China.

School of Chemistry and Material Science, East China University of Technology, Nanchang, 330013, Jiangxi, China.

出版信息

Anal Chim Acta. 2024 May 8;1302:342503. doi: 10.1016/j.aca.2024.342503. Epub 2024 Mar 19.

Abstract

BACKGROUND

The increasing uranium containing wastes generated during uranium mining and finishing pose a huge threat to the environment and human health, and thus robust strategies for on-site monitoring of uranium pollutant are of great significance for environmental protection around uranium tailings.

RESULTS

Herein, a facile "turn-on" colorimetric platform that can achieve uranium detection by spectrometry and naked eyes was developed based on the uranium-enhanced nanozyme activity of covalent organic framework (JUC-505). Thanks to the extended π-conjugated skeleton and donor-acceptor (D-A) structure, JUC-505 exhibited superior photo-activated nanozyme activity, which would be prohibited when the cyano group in JUC-505 skeleton was transformed to the amidoxime group. Further results elucidated that the coordination of uranium with amidoxime groups led to the electron transfer between uranium and the JUC-505-AO skeleton, and thus significantly restored the nanozymatic activity of JUC-505-AO with the subsequent remarkable color changes. Moreover, the uranium concentrations in uranium tailing wastewater detected by the present "turn-on" colorimetric method were well agreed with those by ICP-MS, demonstrating a high accuracy of the present method in real samples.

SIGNIFICANCE

The D-A structured JUC-505 with superior photocatalytic property and nanozymatic activity was applied to facilitate colorimetric detection of uranium, which displays the advantages of low detection limit, excellent selectivity, fast response and simple operation for uranium detection in real samples, and shows a great potential in on-site monitoring of uranium pollutant around uranium tailings as well as nuclear power plant.

摘要

背景

铀矿开采和提炼过程中产生的含铀废物不断增加,对环境和人类健康构成巨大威胁,因此,强有力的铀污染物现场监测策略对于铀尾矿周围的环境保护具有重要意义。

结果

在此,基于共价有机框架(JUC-505)的铀增强纳米酶活性,开发了一种简便的“开启”比色平台,该平台可通过光谱法和肉眼实现铀检测。由于扩展的π共轭骨架和供体-受体(D-A)结构,JUC-505表现出优异的光激活纳米酶活性,当JUC-505骨架中的氰基转化为偕胺肟基时,该活性将被抑制。进一步的结果表明,铀与偕胺肟基的配位导致铀与JUC-505-AO骨架之间的电子转移,从而显著恢复了JUC-505-AO的纳米酶活性,并随后发生显著的颜色变化。此外,用本“开启”比色法检测的铀尾矿废水中的铀浓度与电感耦合等离子体质谱法检测的结果高度一致,表明本方法在实际样品中具有很高的准确性。

意义

具有优异光催化性能和纳米酶活性的D-A结构JUC-505被应用于促进铀的比色检测,该方法在实际样品中检测铀具有检测限低、选择性好、响应快、操作简单等优点,在铀尾矿及核电站周围铀污染物的现场监测中显示出巨大潜力。

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