Departamento de Química Analítica y Alimentaria, Área de Química Analítica, Facultad de Química, Universidad de Vigo, Vigo, Spain.
Anal Chem. 2012 May 15;84(10):4452-9. doi: 10.1021/ac300221s. Epub 2012 Apr 30.
Following a preliminary work (Costas-Mora, I.; Romero, V.; Pena-Pereira, F.; Lavilla, I.; Bendicho, C. Anal. Chem.2011, 83, 2388-2393), a quenching mechanism has been established for the selective detection of Se (as selenium hydride) by microfluorospectrometry using CdSe quantum dots (QDs) as luminescent probes stabilized with hexadecylamine and confined in an organic droplet. For this purpose, luminescence, luminescence lifetime, UV-vis absorption, total reflection X-ray fluorescence, transmission electron microscopy, and atomic force microscopy measurements were performed. The presence of stabilizing agents of QDs in the droplet was found to cause a critical effect on both extraction efficiency of selenium hydride in the drop and luminescence quenching. A self-quenching mechanism due to the aggregation of QDs is suggested. Aggregation is thought to occur as a result of the binding between selenide trapped into the organic drop as selenium hydride and Cd(2+) present in the surface of QDs, which in turn, may cause the loss of stabilizing hexadecylamine groups. After full optimization of main variables influencing the luminescent response, the analytical performance was established. A detection limit as low as 0.08 μg L(-1) Se(IV) and a repeatability expressed as relative standard deviation of 4.6% were obtained. The method was validated against CRM NWTM-27.2 lake water, and a recovery study was performed with synthetic seawater. The use of CdSe as luminescent probes in an organic drop may constitute an extremely selective, sensitive, and miniaturized assay for in situ detection of Se(IV) in water.
在初步研究(Costas-Mora,I.;Romero,V.;Pena-Pereira,F.;Lavilla,I.;Bendicho,C. Anal. Chem.2011, 83, 2388-2393)之后,我们建立了一种用 CdSe 量子点(QDs)作为荧光探针,用十六胺稳定并封装在有机液滴中的微荧光光谱法来选择性检测硒(以硒化氢的形式存在)的猝灭机制。为此,我们进行了发光、发光寿命、紫外-可见吸收、全反射 X 射线荧光、透射电子显微镜和原子力显微镜测量。研究发现,液滴中 QDs 的稳定剂的存在对硒化氢在液滴中的萃取效率和发光猝灭有重要影响。提出了由于 QDs 的聚集导致自猝灭的机制。认为这种聚集是由于硒化物作为硒化氢被捕获到有机液滴中与 QDs 表面存在的 Cd(2+)结合而发生的,这反过来又可能导致失去稳定的十六胺基团。在对影响发光响应的主要变量进行充分优化后,建立了分析性能。得到了低至 0.08μg L(-1) Se(IV)的检测限和 4.6%的相对标准偏差的重复性。该方法已通过 CRM NWTM-27.2 湖水标准物质进行验证,并对合成海水进行了回收研究。在有机液滴中使用 CdSe 作为荧光探针可能构成一种极其灵敏、选择性强、微型化的方法,用于水中 Se(IV)的原位检测。