Xia Yun-Sheng, Zhu Chang-Qing
Anhui Key Laboratory of Chemo-Biosensing, College of Chemistry and Materials Science, Anhui Normal University, Wuhu, 241000, PR China.
Talanta. 2008 Mar 15;75(1):215-21. doi: 10.1016/j.talanta.2007.11.008. Epub 2007 Nov 17.
Thioglycolic acid (TGA)-capped CdTe quantum dots (QDs) were synthesized in aqueous medium, and their interaction with metal cations was studied with UV-vis absorption, steady-state and time-resolved fluorescence spectra. The results demonstrated that Hg(II), Cu(II) and Ag(I) could effectively quench the QD emission based on different action mechanisms: Cu(II) and Ag(I) quenched CdTe QDs because they bound onto particle surface and facilitated non-radiative electron/hole recombination annihilation of QDs; electron transfer process between the capping ligands and Hg(II) was mainly responsible for the remarkable quenching effect of Hg(II). To prevent the approach of metal cations to QD core, the original TGA-capped CdTe QDs were further coated by denatured bovine serum albumin (dBSA). It was found that the dBSA-coated CdTe QDs could be quenched effectively by Hg(II), but Cu(II) and Ag(I) could hardly quench the QDs even at fairly higher concentration levels because the dBSA shell layer effectively prevented the binding of metal cations onto the QD core. On the basis of this fact, a simple, rapid and specific method for Hg(II) determination was proposed. Under optimal conditions, the quenched fluorescence intensity increased linearly with the concentration of Hg(II) ranging from 0.012 x 10(-6) to 1.5 x 10(-6) mol L(-1). The limit of detection for Hg(II) was 4.0 x 10(-9) mol L(-1). The developed method was successfully applied to the detection of trace Hg(II) in real samples.
在水相中合成了巯基乙酸(TGA)包覆的碲化镉量子点(QDs),并通过紫外可见吸收光谱、稳态荧光光谱和时间分辨荧光光谱研究了它们与金属阳离子的相互作用。结果表明,Hg(II)、Cu(II)和Ag(I)可基于不同作用机制有效猝灭量子点的发射:Cu(II)和Ag(I)猝灭碲化镉量子点是因为它们结合到颗粒表面并促进了量子点的非辐射电子/空穴复合湮灭;封端配体与Hg(II)之间的电子转移过程是Hg(II)显著猝灭效应的主要原因。为防止金属阳离子接近量子点核心,原始的TGA包覆碲化镉量子点进一步用变性牛血清白蛋白(dBSA)包覆。发现dBSA包覆的碲化镉量子点可被Hg(II)有效猝灭,但即使在相当高的浓度水平下,Cu(II)和Ag(I)也几乎不能猝灭量子点,因为dBSA壳层有效地阻止了金属阳离子与量子点核心的结合。基于这一事实,提出了一种简单、快速且特异的Hg(II)测定方法。在最佳条件下,猝灭荧光强度与Hg(II)浓度在0.012×10(-6)至1.5×10(-6) mol L(-1)范围内呈线性增加。Hg(II)的检测限为4.0×10(-9) mol L(-1)。所建立的方法成功应用于实际样品中痕量Hg(II)的检测。