Key Laboratory of Functional Molecular Solids, Ministry of Education, College of Chemistry and Materials Science , Anhui Normal University , Wuhu 241000 , China.
Anal Chem. 2018 Mar 20;90(6):3942-3949. doi: 10.1021/acs.analchem.7b04893. Epub 2018 Feb 28.
In this study, we present a simple but effective fluorescent system for highly sensitive and versatile sensing of 2,4,6-trinitrotoluene (TNT) using few layered planar MoS quantum dots (QDs) as reporters. Excitation-independent emitting MoS QDs were first fabricated by using the proposed ultrasonic-hydrothermal-based top-down method assisted by carbon-free hydroxylamine hydrochloride. The obtained pristine MoS QDs were then modified with cysteine for introducing amino groups as TNT binding sites. The as-prepared MoS QDs possess a planar structure, which can more adequately interact with flat aromatic TNT molecules due to π-π attraction and decreased steric effects, compared with traditional spherical/quasi-spherical QDs. As a result, they exhibit extremely high sensitivity for TNT sensing (1 nM and 2 ng for solution and substrate assay, respectively). The common ions containing in environmental water samples do not interfere with the sensing. Furthermore, the QDs-decorated test paper shows an instantaneous (within 1 min) response to trace amounts of deposited TNT, and the fluorescence quenching can even be well-visualized by the naked eye. Because of favorable analytical performances, the proposed MoS QDs-based TNT sensing system has potential applications in both environmental water monitoring and security screening.
在这项研究中,我们提出了一种简单但有效的荧光体系,使用少层平面 MoS 量子点 (QD) 作为报告物,用于高度灵敏和多功能的 2,4,6-三硝基甲苯 (TNT) 检测。首先,通过使用提出的超声-水热法自上而下方法,辅助无碳羟胺盐酸盐来制备无激发发射的 MoS QD。然后,用半胱氨酸对获得的原始 MoS QD 进行修饰,以引入氨基作为 TNT 结合位点。与传统的球形/准球形 QD 相比,所制备的 MoS QD 具有平面结构,由于π-π 吸引和降低的空间位阻效应,可以更充分地与平面芳香 TNT 分子相互作用。因此,它们对 TNT 检测表现出极高的灵敏度(溶液和基底检测分别为 1 nM 和 2 ng)。环境水样中的常见离子不会干扰检测。此外,QD 修饰的试纸对沉积的 TNT 的痕量表现出瞬时(1 分钟内)响应,荧光猝灭甚至可以用肉眼很好地观察到。由于具有良好的分析性能,基于 MoS QD 的 TNT 传感系统在环境水样监测和安全筛选方面具有潜在的应用。