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Antifouling membrane integrated renewable gold microelectrode for in situ detection of As(III)

机译:防污膜集成可再生金微电极用于原位检测As(III)

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摘要

Arsenic in the environment is of a global concern because of the widespread, chronic poisoning found in a number of countries and affecting large populations. Robust and sensitive analytical tools capable of direct, continuous in situ As(III) sensing is therefore of prime interest for As health risk assessment. For this purpose, we have developed here a microelectrode consisting of a gel integrated renewable gold nanoparticles plated iridium-based microelectrode (Au-GIME). The gel minimizes fouling problems by hindering diffusion of organic matters and inorganic colloids/macromolecules toward the sensor surface. Square Wave Anodic Stripping Voltammetry (SWASV) was used to characterize (i) the kinetics of As(III) diffusion in the agarose gel as a function of the gel thickness, (ii) the analytical performance of the sensor in synthetic and natural waters, and (iii) the influence of the temperature on the arsenic stripping peak current intensities. An evaluation of direct environmental application was performed in freshly collected lake water samples and validated by ICP-MS after separating As(V) and As(III) with an ion-exchange resin. The results reveal that the Au-GIME fulfills the requirements for direct measurements of (oxy)anions in freshwaters, i.e.: a reproducible mass transport of arsenite species in the gel; a gel equilibration time varying with the thickness of the gel in accordance with theory; a temperature effect on the SWASV As(III) signal intensities following a Arrhenius behavior and thus readily corrected using a factor defined in laboratory; and a nanomolar detection limit at pH 8.
机译:由于在许多国家中普遍存在的慢性中毒影响了大批人口,环境中的砷引起了全球关注。因此,能够直接,连续原位检测As(III)的稳健而灵敏的分析工具对于As健康风险评估尤为重要。为此,我们在此开发了一种微电极,该微电极由凝胶集成的可再生金纳米颗粒镀铱基微电极(Au-GIME)组成。该凝胶通过阻止有机物和无机胶体/大分子向传感器表面的扩散来最大程度地减少结垢问题。方波阳极溶出伏安法(SWASV)用于表征(i)琼脂糖凝胶中As(III)扩散的动力学与凝胶厚度的关系,(ii)合成水和天然水中传感器的分析性能, (iii)温度对砷溶出峰电流强度的影响。在新鲜收集的湖水样品中进行了直接环境应用的评估,并在用离子交换树脂分离了As(V)和As(III)之后通过ICP-MS进行了验证。结果表明,Au-GIME满足直接测量淡水中(氧)阴离子的要求,即:凝胶中亚砷酸盐物种的可重现质量传递;根据理论,凝胶平衡时间随凝胶的厚度而变化; Arrhenius行为后温度对SWASV As(III)信号强度的影响,因此可以使用实验室定义的因子轻松进行校正; pH值为8时的纳摩尔检测极限。

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