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油酸包覆的CdSe/ZnS量子点结构性质对汞离子检测的影响

Influence of Structural Properties of Oleic Acid-Capped CdSe/ZnS Quantum Dots in the Detection of Hg Ions.

作者信息

Ortiz Calderon Fredy Giovany, Gómez Pineros Brayan Stiven, McClenaghan Nathan D, Granados-Oliveros Gilma

机构信息

Grupo de Síntesis Orgánica Sostenible, Departamento de Química, Facultad de Ciencias, Universidad Nacional de Colombia, Bogotá, DC, Colombia.

Institut des Sciences Moléculaires, CNRS UMR 5255, University of Bordeaux, Talence, 33405, France.

出版信息

J Fluoresc. 2024 Jul 16. doi: 10.1007/s10895-024-03828-0.

Abstract

Oleic acid-capped CdSe/ZnS quantum dots (QDs) were used to investigate their photoluminescence (PL) response to Hg ions as a function of the surface properties of QDs. Three distinctly-size CdSe/ZnS QDs were obtained by varying the molar ratio of shell precursors, which were characterized by X-ray diffraction (XRD), high-resolution transmission electron microscopy (HR-TEM), Fourier-Transform infrared (FT-IR), X-ray photoelectron spectroscopy (XPS), absorption spectroscopy, and time-resolved fluorescence spectroscopy. Results revealed the obtention of zinc blende nanocrystals with sizes ranging from 2.7 to 3.2 nm (± 0.5) and ZnS thickness between 0.3 and 1.0 monolayer (ML). The variation of the [S]/[Zn] molar ratio introduced chemical species that act as traps, affecting the PL properties differently. Depending on the thickness of the shell and chemical speciation on surface, Hg ions could induce quenching or enhancement of PL. Detection of mercury ions was evaluated in terms of Stern-Volmer equation, where the limit of detection (LOD) for the PL quenching system was 11.2 nM, while for the PL enhancing systems were 8.98 nM and 10.7 nM. Results demonstrate the performance of oleic acid-capped CdSe/ZnS QDs to detect Hg and their capacity to turn the PL on/off depending on surface properties.

摘要

油酸包覆的CdSe/ZnS量子点(QDs)被用于研究其作为量子点表面性质函数对汞离子的光致发光(PL)响应。通过改变壳层前驱体的摩尔比获得了三种尺寸明显不同的CdSe/ZnS量子点,通过X射线衍射(XRD)、高分辨率透射电子显微镜(HR-TEM)、傅里叶变换红外光谱(FT-IR)、X射线光电子能谱(XPS)、吸收光谱和时间分辨荧光光谱对其进行了表征。结果表明获得了闪锌矿纳米晶体,尺寸范围为2.7至3.2纳米(±0.5),ZnS厚度在0.3至1.0单层(ML)之间。[S]/[Zn]摩尔比的变化引入了作为陷阱的化学物种,对PL性质产生不同影响。根据壳层厚度和表面化学形态,汞离子可诱导PL猝灭或增强。根据斯特恩-沃尔默方程评估了汞离子的检测,其中PL猝灭系统的检测限(LOD)为11.2 nM,而PL增强系统的检测限分别为8.98 nM和10.7 nM。结果证明了油酸包覆的CdSe/ZnS量子点检测汞的性能及其根据表面性质开启/关闭PL的能力。

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