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金属有机框架上的硫醚侧基对汞(II)离子的高选择性检测

High selective detection of mercury (II) ions by thioether side groups on metal-organic frameworks.

作者信息

Fu Li, Xie Kefeng, Wang Aiwu, Lyu Fucong, Ge Jingyuan, Zhang Luxi, Zhang Huaiwei, Su Weitao, Hou Yun-Long, Zhou Cangtao, Wang Chundong, Ruan Shuangchen

机构信息

College of Materials and Environmental Engineering, Hangzhou Dianzi University, Hangzhou, 310018, PR China.

School of Chemical and Biological Engineering, Lanzhou Jiaotong University, Lanzhou, Gansu, 730070, PR China.

出版信息

Anal Chim Acta. 2019 Nov 12;1081:51-58. doi: 10.1016/j.aca.2019.06.055. Epub 2019 Jun 28.

Abstract

Mercury ions can significantly affect the organism and environment even at a very low concentration. Thus, great efforts have been devoted to developing high sensitive electrochemical sensors, especially the one that not only detect the mercury ions but also effective sensitive to thymine-Hg-thymine in aqueous solution. Metal-organic-frameworks (MOFs) possess hollow nature and are easy for grafting functional groups, however, there is still no attempts for working as electrochemical sensors in detecting mercury ions. Herein, we report a novel type sensor of Zr(IV)-based MOFs with specifically attached thioether side groups allowing mercury ions to be easily adsorbed and detected. The Zr(IV)-involved MOFs show strong binding to mercury ions compared with the bare MOFs, as confirmed by both experiment measurements and theoretical calculations. The as-prepared senor is sensitive ranging from 0.01 nM to 3 μM with detection limitation of 7.3 fM, which is better than most of T-Hg-T- and enzyme-based sensors reported so far. The high sensitivity could be due to the straightforward adsorption pathway and the biomolecule exclusion nature of the Zr(IV)-involved MOFs sensor. We anticipate that our findings could pave the way for MOFs-based sensor exploration towards its commercial applications.

摘要

汞离子即使在极低浓度下也会对生物体和环境产生显著影响。因此,人们致力于开发高灵敏度的电化学传感器,尤其是那种不仅能检测汞离子,而且对水溶液中的胸腺嘧啶-汞-胸腺嘧啶具有有效敏感性的传感器。金属有机框架材料(MOFs)具有中空结构,易于接枝官能团,然而,尚未有将其用作检测汞离子的电化学传感器的尝试。在此,我们报道了一种新型的基于Zr(IV)的MOFs传感器,其带有特异性连接的硫醚侧基,能够使汞离子易于被吸附和检测。与未修饰的MOFs相比,含Zr(IV)的MOFs对汞离子表现出更强的结合能力,实验测量和理论计算均证实了这一点。所制备的传感器在0.01 nM至3 μM范围内具有灵敏度,检测限为7.3 fM,优于目前报道的大多数基于胸腺嘧啶-汞-胸腺嘧啶和酶的传感器。高灵敏度可能归因于含Zr(IV)的MOFs传感器直接的吸附途径和生物分子排斥特性。我们预计我们的研究结果可为基于MOFs的传感器探索其商业应用铺平道路。

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