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上转换发光纳米传感器用于 TNT 选择性和无标记定量混合物中的硝基芳香族爆炸物。

Upconversion luminescence nanosensor for TNT selective and label-free quantification in the mixture of nitroaromatic explosives.

机构信息

State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Environmentally Harmful Chemical Analysis, School of Science, Beijing University of Chemical Technology, Beijing 100029, China.

State Key Laboratory of Chemical Resource Engineering, Beijing Key Laboratory of Environmentally Harmful Chemical Analysis, School of Science, Beijing University of Chemical Technology, Beijing 100029, China.

出版信息

Talanta. 2014 Mar;120:100-5. doi: 10.1016/j.talanta.2013.12.009. Epub 2013 Dec 10.

DOI:10.1016/j.talanta.2013.12.009
PMID:24468348
Abstract

This paper reports a rapid, sensitive, and selective nanosensor for the detection of 2,4,6-trinitrotoluene (TNT) in the mixture aqueous solution of nitroaromatics independent of immunoassay or molecularly imprinted technology and complicated instruments. Despite many strategies including immunoassay and molecularly imprinted technologies been successfully developed for the detection of TNT, it is not easy to differentiate TNT from 2,4,6-trinitrophenol (TNP) due to their very similar chemical structures and properties. In this work, the amine functionalized NaYF4:Yb(3+)/Er(3+) upconversion luminescence nanoparticles (UCNPs) whose excitation (980 nm) and emission (543 nm) wavelength were far from the absorbance bands of other usual interference nitroaromatics including 2,4-dinitrotoluene (DNT), nitrobenzene (NB), and especially TNP, were utilized as the luminescent nanosensors for TNT luminescence detection. To make these UCNPs highly water stable and render the charge transfer from UCNPs to TNT easier, amino groups were introduced onto the surface of the UCNPs by coating a polymer layer of ethylene glycol dimethacrylate (EGDMA) hybridized with 3-aminopropyltriethoxysilane (APTS). After binding with TNT through amino groups on the UCNPs, the naked eye visible green upconversion luminescence of the UCNPs was dramatically quenched and thus a sensitive UC luminescence nanosensor was developed for TNT detection. However, other nitroaromatics including TNP, DNT, and NB have no influence on the green UC luminescence and thus no influence on the TNT detection. The luminescence intensity is negatively proportional to the concentration of TNT in the range of 0.01-9.0 µg/mL with the 3σ limit of detection (LOD) of 9.7 ng/mL. The present studies provide a novel and facile strategy to fabricate the upconversion luminescence sensors with highly selective recognition ability in aqueous media and are desirable for label free analysis of TNT in mixed solution independent of immunoassay and molecularly imprinted technology and complicated instruments.

摘要

本文报道了一种快速、灵敏、选择性的纳米传感器,用于检测混合水溶液中的 2,4,6-三硝基甲苯(TNT),该传感器独立于免疫测定或分子印迹技术和复杂仪器。尽管已经成功开发了许多包括免疫测定和分子印迹技术在内的策略来检测 TNT,但由于其化学结构和性质非常相似,因此不容易将 TNT 与 2,4,6-三硝基苯酚(TNP)区分开来。在这项工作中,胺功能化的 NaYF4:Yb(3+)/Er(3+)上转换发光纳米粒子(UCNPs)被用作 TNT 发光检测的发光纳米传感器,其激发(980nm)和发射(543nm)波长远于其他常见干扰硝基芳烃的吸收带,包括 2,4-二硝基甲苯(DNT)、硝基苯(NB),特别是 TNP。为了使这些 UCNPs 具有高度的水稳定性,并使电荷更容易从 UCNPs 转移到 TNT,通过涂覆由乙二醇二甲基丙烯酸酯(EGDMA)与 3-氨丙基三乙氧基硅烷(APTS)杂交而成的聚合物层,在 UCNPs 表面引入了氨基。与 UCNPs 上的氨基结合后,UCNPs 的肉眼可见的绿色上转换发光被显著猝灭,因此开发了一种用于 TNT 检测的灵敏 UC 发光纳米传感器。然而,其他硝基芳烃,包括 TNP、DNT 和 NB,对绿色 UC 发光没有影响,因此对 TNT 检测没有影响。发光强度与 TNT 浓度在 0.01-9.0μg/mL 范围内呈负相关,检测限(LOD)为 9.7ng/mL。本研究提供了一种在水介质中具有高选择性识别能力的上转换发光传感器的新型简便制备策略,是在不依赖免疫测定和分子印迹技术和复杂仪器的情况下,对混合溶液中 TNT 进行无标记分析的理想选择。

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