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吸附剂辅助原位电催化:在金纳米粒子密集修饰的四氧化三铁纳米球上对水中砷(III)的超灵敏检测。

Adsorbent Assisted in Situ Electrocatalysis: An Ultra-Sensitive Detection of As(III) in Water at Fe3O4 Nanosphere Densely Decorated with Au Nanoparticles.

作者信息

Wei Juan, Li Shan-Shan, Guo Zheng, Chen Xing, Liu Jin-Huai, Huang Xing-Jiu

机构信息

Nanomaterials and Environmental Detection Laboratory, Institute of Intelligent Machines, Chinese Academy of Sciences , Hefei 230031, People's Republic of China.

Department of Chemistry, University of Science and Technology of China , Hefei 230026, People's Republic of China.

出版信息

Anal Chem. 2016 Jan 19;88(2):1154-61. doi: 10.1021/acs.analchem.5b02947. Epub 2015 Dec 31.

Abstract

Most gold nanoparticle-based electrodes have been utilized for the analysis of highly toxic As(III), while nano-Fe3O4 materials are currently attracting considerable interest as an adsorbent for the removal of As(III). However, the combination of gold nanoparticles with Fe3O4 nanoadsorbents for stripping voltammetry is, to the best of our knowledge, unexplored. Here, a sensing interface for ultrasensitive detection of As(III) is designed and constructed by abundantly dispersing Au nanoparticles (Au NPs) on the surface of the Fe3O4 nanosphere. The Au@Fe3O4 nanospheres are covered by the room temperature ionic liquid (RTIL) and then modified on the screen-printed carbon electrode (SPCE). By combining the excellent catalytic properties of the Au nanoparticles (∼3-9 nm in diameter) with the good adsorption capacity of Fe3O4 nanospheres toward As(III), as well as the good conductivity of RTIL, the Au@Fe3O4-RTIL shows excellent performance in the detection of arsenic under nearly neutral conditions without modifying the morphology of the sensing interface. Through optimization of the experimental conditions, an ultrahigh sensitivity of 458.66 μA ppb(-1) cm(-2) from 0.1 to 1 ppb with a detection limit (3σ method) of 0.0022 ppb was obtained. The reproducibility and reliability of the Au@Fe3O4-RTIL sensing interface was also evaluated with good results. Finally, we used this platform to analyze real samples.

摘要

大多数基于金纳米颗粒的电极已被用于分析剧毒的 As(III),而纳米 Fe3O4 材料作为去除 As(III) 的吸附剂目前正引起人们的极大兴趣。然而,据我们所知,金纳米颗粒与 Fe3O4 纳米吸附剂结合用于溶出伏安法尚未得到探索。在此,通过在 Fe3O4 纳米球表面大量分散金纳米颗粒(Au NPs),设计并构建了用于超灵敏检测 As(III) 的传感界面。Au@Fe3O4 纳米球被室温离子液体(RTIL)覆盖,然后修饰在丝网印刷碳电极(SPCE)上。通过将直径约为 3 - 9 nm 的金纳米颗粒的优异催化性能与 Fe3O4 纳米球对 As(III) 的良好吸附能力以及 RTIL 的良好导电性相结合,Au@Fe3O4 - RTIL 在几乎中性条件下检测砷时表现出优异性能,且无需改变传感界面的形态。通过优化实验条件,在 0.1 至 1 ppb 范围内获得了 458.66 μA ppb⁻¹ cm⁻² 的超高灵敏度,检测限(3σ 法)为 0.0022 ppb。还对 Au@Fe3O4 - RTIL 传感界面的重现性和可靠性进行了评估,结果良好。最后,我们使用该平台分析实际样品。

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