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用于快速灵敏地表面增强拉曼散射检测铀酰的磁性金属有机框架基底

Magnetic MOF Substrates for the Rapid and Sensitive Surface-Enhanced Raman Scattering Detection of Uranyl.

作者信息

Wang Ning, Du Jingjing, Li Xue, Ji Xunlong, Wu Yulin, Sun Zhenli

机构信息

MOE Key Laboratory of Resources and Environmental System Optimization, College of Environmental Science and Engineering, North China Electric Power University, Beijing 102206, China.

State Key Laboratory of Environmental Chemistry and Ecotoxicology, Research Center for Eco-Environmental Sciences, Chinese Academy of Sciences, Beijing 100085, China.

出版信息

Anal Chem. 2023 Aug 29;95(34):12956-12963. doi: 10.1021/acs.analchem.3c02696. Epub 2023 Aug 15.

Abstract

With the widespread use of uranium in the nuclear industry, achieving rapid and sensitive detection of uranium contaminants is critical for reducing environmental pollution. Surface-enhanced Raman scattering (SERS), with its high sensitivity and unique fingerprint properties, has been used for the analysis of uranyl. However, the weak affinity of Au for uranyl remains a challenge in the development of spherical Au-based SERS substrates. The metal-organic framework (MOF) material ZIF-8 exhibits excellent adsorption capacity for uranyl and could overcome this limitation. In this study, ZIF-8 porous structures were modified on a magnetic SERS substrate, FeO@SiO@Au (FA), for the rapid and sensitive detection and analysis of the uranyl species. Uranyl was adsorbed by ZIF-8, allowing ready access to the hot spots in the interstices of Au nanoparticles (AuNPs). Symmetrically stretched vibrating bonds of O═U═O were detected at 829 cm as the characteristic peak of uranyl by surface plasmon resonance between the AuNPs. The ZIF-8 coating had minimal influence on target detection as the detection limit for 4-MPY was only half an order of magnitude lower than before modification. The enhancement factor for uranyl reached 10. The substrate showed excellent sensing performance in a neutral or alkaline environment. It was used to detect uranyl in tap water and river water; rapid separation of the species from the water samples was achieved using an external magnet to extract radioactive waste. The proposed substrate offers a route for monitoring and detecting uranyl contamination and an approach for achieving rapid on-site detection, providing a promising application for environmental contaminant detection.

摘要

随着铀在核工业中的广泛应用,实现对铀污染物的快速灵敏检测对于减少环境污染至关重要。表面增强拉曼散射(SERS)具有高灵敏度和独特的指纹特性,已被用于铀酰的分析。然而,金对铀酰的弱亲和力仍然是开发基于球形金的SERS基底的一个挑战。金属有机框架(MOF)材料ZIF-8对铀酰表现出优异的吸附能力,能够克服这一限制。在本研究中,ZIF-8多孔结构被修饰在磁性SERS基底FeO@SiO@Au(FA)上,用于铀酰物种的快速灵敏检测和分析。铀酰被ZIF-8吸附,使得能够方便地进入金纳米颗粒(AuNP)间隙中的热点。通过AuNP之间的表面等离子体共振,在829 cm处检测到O═U═O的对称拉伸振动键作为铀酰的特征峰。ZIF-8涂层对目标检测的影响最小,因为4-甲基吡啶的检测限仅比修饰前低半个数量级。铀酰的增强因子达到10。该基底在中性或碱性环境中表现出优异的传感性能。它被用于检测自来水和河水中的铀酰;使用外部磁铁提取放射性废物,实现了从水样中快速分离该物种。所提出的基底为监测和检测铀酰污染提供了一条途径,以及一种实现快速现场检测的方法,为环境污染物检测提供了一个有前景的应用。

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