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基于AgPO微立方体的汞刺激氧化酶模拟活性比色法测定汞。

Colorimetric determination of Hg based on the mercury-stimulated oxidase mimetic activity of AgPO microcubes.

作者信息

Zhang Yu, Ju Peng, Sun Liping, Wang Zhe, Zhai Xiaofan, Jiang Fenghua, Sun Chengjun

机构信息

Key Laboratory of Marine Eco-Environmental Science and Technology, Marine Bioresource and Environment Research Center, First Institute of Oceanography, Ministry of Natural Resources (MNR), 6 Xianxialing Road, Qingdao, 266061, People's Republic of China.

Laboratory for Marine Ecology and Environmental Science, Pilot National Laboratory for Marine Science and Technology (Qingdao), 1 Wenhai Road, Qingdao, 266237, People's Republic of China.

出版信息

Mikrochim Acta. 2020 Jul 2;187(7):422. doi: 10.1007/s00604-020-04399-0.

Abstract

Four kinds of AgPO materials were prepared by controlling the experimental conditions, which were developed as oxidase mimics. Experimental results showed that different synthesis methods led to distinct crystal structures, morphologies, and surface properties, which contributed to diverse oxidase-like activities of AgPO materials. Among them, AgPO microcubes (APMCs) can efficiently catalyze the oxidation of colorless 3,3',5,5'-tetramethylbenzidine in the presence of dissolved oxygen to form a blue-colored oxide, presenting the best intrinsic oxidase mimetic ability. The higher-energy [110] facets with more oxygen vacancies exposed and more active sites coupled with more negative charge and larger specific surface area of APMCs contributed to its enhanced oxidase mimetic performance. Besides, mercury ions were proved to remarkably and selectively stimulate the oxidase-like ability of APMCs owing to the formation of Ag-Hg amalgam on its surface. Based on the stimulating effect of Hg towards APMCs, a simple and rapid method for colorimetric determination of Hg was thus established via the significant signal amplification and megascopic color variation. Under the optimal conditions, the sensing system showed a good linear relationship ranging from 0.1 to 7.0 μM and a detection limit of 20 nM for Hg, exhibiting high selectivity and good colour stability. Moreover, the colorimetric method was successfully applied to determine Hg in real water samples. Considering these advantages, the developed colorimetric sensing system is expected to hold bright prospects for trace determination of Hg in biological, environmental, and food samples. Graphical abstract The preparation process of AgPO materials and Hg-stimulated enhanced oxidase-like ability of AgPO microcubes in catalyzing the oxidation of TMB to generate a typical blue color, which can be applied in rapid and ultrasensitive detection of Hg visually.

摘要

通过控制实验条件制备了四种AgPO材料,它们被开发为氧化酶模拟物。实验结果表明,不同的合成方法导致了不同的晶体结构、形态和表面性质,这使得AgPO材料具有多样的类氧化酶活性。其中,AgPO微立方体(APMCs)在溶解氧存在下能有效催化无色的3,3',5,5'-四甲基联苯胺氧化形成蓝色氧化物,呈现出最佳的固有氧化酶模拟能力。APMCs暴露更多氧空位且具有更多活性位点的高能[110]晶面,再加上更多的负电荷和更大的比表面积,有助于其增强的氧化酶模拟性能。此外,由于在其表面形成了Ag-Hg汞齐,汞离子被证明能显著且选择性地刺激APMCs的类氧化酶能力。基于Hg对APMCs的刺激作用,通过显著的信号放大和肉眼可见的颜色变化,建立了一种简单快速的Hg比色测定方法。在最佳条件下,传感系统在0.1至7.0 μM范围内呈现良好的线性关系,对Hg的检测限为20 nM,具有高选择性和良好的颜色稳定性。此外,该比色法成功应用于实际水样中Hg的测定。考虑到这些优点,所开发的比色传感系统有望在生物、环境和食品样品中Hg的痕量测定方面具有广阔前景。图形摘要AgPO材料的制备过程以及Hg刺激增强AgPO微立方体催化TMB氧化生成典型蓝色的类氧化酶能力,可用于直观快速超灵敏检测Hg。

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