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基于溶菌酶 VI 型稳定的金纳米簇荧光猝灭对 Hg(2+)和 CH(3)Hg(+)的超灵敏传感。

Ultrasensitive sensing of Hg(2+) and CH(3)Hg(+) based on the fluorescence quenching of lysozyme type VI-stabilized gold nanoclusters.

机构信息

Department of Chemistry, National Sun Yat-sen University, 70, Lien-hai Road, Kaohsiung, Taiwan 804.

出版信息

Anal Chem. 2010 Nov 15;82(22):9194-200. doi: 10.1021/ac101427y. Epub 2010 Oct 18.

Abstract

This study presents a one-step approach to prepare lysozyme type VI-stabilized gold nanoclusters (Lys VI-AuNCs) for the ultrasensitive detection of Hg(2+) and CH(3)Hg(+) based on fluorescence quenching. The optical properties and size of Lys VI-AuNCs are highly dependent on the concentration of Lys VI, which acts as both a reducing and a stabilizing agent. With an increase in the concentration of Lys VI, we observed a systematic blue shift in the fluorescence maxima, an increase in the quantum yields, and a reduction in the particle size. When using 25 mg/mL Lys VI as a reducing agent, the formed Lys VI-AuNCs (denoted as Au-631) were found to be highly stable in a high-concentration glutathione or NaCl. Additionally, the Au-631 were capable of sensing Hg(2+) and CH(3)Hg(+) through the interaction between Hg(2+)/CH(3)Hg(+) and Au(+) on the Au surface; the limits of detection (LODs) for Hg(2+) and CH(3)Hg(+) were 3 pM and 4 nM, respectively. The selectivity of this probe is more than 500-fold for Hg(2+) over any metal ions. As compared to bovine serum albumin-stabilized AuNCs, Au-631 provided an approximately 330-fold improvement in the detection of Hg(2+). To the best of our knowledge, Au-631 not only provide the first example for detecting CH(3)Hg(+) but also have the lowest LOD value for Hg(2+) when compared to other AuNC-based Hg(2+) sensors. Importantly, this probe was successfully applied to the determination of Hg(2+) and CH(3)Hg(+) in seawater.

摘要

本研究提出了一种一步法制备溶菌酶 VI 稳定的金纳米簇(Lys VI-AuNCs),用于基于荧光猝灭的超灵敏检测 Hg(2+) 和 CH(3)Hg(+)。Lys VI-AuNCs 的光学性质和尺寸高度依赖于 Lys VI 的浓度,Lys VI 既作为还原剂又作为稳定剂。随着 Lys VI 浓度的增加,我们观察到荧光最大值的系统蓝移、量子产率的增加和粒径的减小。当使用 25 mg/mL Lys VI 作为还原剂时,形成的 Lys VI-AuNCs(表示为 Au-631)在高浓度谷胱甘肽或 NaCl 中表现出高度稳定性。此外,Au-631 能够通过 Hg(2+) / CH(3)Hg(+)与 Au 表面上的 Au(+)之间的相互作用来感测 Hg(2+)和 CH(3)Hg(+);Hg(2+)和 CH(3)Hg(+)的检测限(LOD)分别为 3 pM 和 4 nM。该探针对 Hg(2+)的选择性超过任何金属离子的 500 倍以上。与牛血清白蛋白稳定的 AuNCs 相比,Au-631 对 Hg(2+)的检测提高了约 330 倍。据我们所知,与其他基于 AuNC 的 Hg(2+)传感器相比,Au-631 不仅提供了检测 CH(3)Hg(+)的第一个例子,而且还具有最低的 Hg(2+)检测限。重要的是,该探针成功应用于海水中 Hg(2+)和 CH(3)Hg(+)的测定。

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