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Mercury(II) Trace Detection Using a Glassy Carbon Electrode Functionalized by Chemically Prepared Gold Nanoparticles. Influence of Coating Process on Surface Reactivity and Analytical Performances

机译:使用化学制备的金纳米粒子功能化的玻碳电极进行痕量汞(II)检测。涂层工艺对表面反应性和分析性能的影响

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摘要

An electrochemical sensor dedicated to Hg(II) trace detection was elaborated based on a gold nanoparticles (AuNPs) modified glassy carbon (GC) electrode. AuNPs were prepared using the Turkevich method and deposited on GC by drop casting. Different protocols including suspension filtration and evaporation temperature control were tested and their influence both on coating morphology and electrochemical activity assessed. From structural characterization, it can be concluded that neither the filtration step nor the drop evaporating temperature have a significant impact on coating morphology at the mesoscale level. However, regarding to the electrochemical activity of the functionalized electrodes, results showed that when some heterogeneities due to (AuNPs) aggregation were present in the coating, the electrochemical activity was reduced. Contrary to what was observed in our previous studies dealing with electrodeposited AuNPs, cycling an AuNPs-GC electrode in H2SO4 lead in all cases to a decrease in active surface area and in a higher density of surface defects, thus revealing a higher surface reactivity of chemically-synthesized AuNPs. The electrochemical activation procedure was found to influence the analytical performances of the functionalized electrode with respect to Hg(II) assay in the picomolar range, but not in the nanomolar range, as a consequence of a saturated concentration effect. A linear concentration range was obtained between 2 and 12 pM with a normalized sensitivity of 0.296 μA pM-1 min-1 using square wave anodic stripping voltammetry (SWASV) as the detection mode. A limit of detection (LOD) down to 1 pM was reached.
机译:基于金纳米粒子(AuNPs)修饰的玻碳(GC)电极,精心设计了一种用于Hg(II)痕量检测的电化学传感器。使用Turkevich方法制备AuNP,并通过滴铸法将其沉积在GC上。测试了包括悬浮液过滤和蒸发温度控制在内的不同方案,并评估了它们对涂层形态和电化学活性的影响。从结构特征可以得出结论,在中尺度水平上,过滤步骤和液滴蒸发温度都不会对涂层形态产生重大影响。然而,关于功能化电极的电化学活性,结果表明,当涂层中由于(AuNPs)聚集而存在某些异质性时,电化学活性会降低。与我们先前关于电沉积AuNPs的研究相反,在所有情况下,在H2SO4中循环AuNPs-GC电极都会导致活性表面积减小和表面缺陷密度更高,从而揭示出化学上更高的表面反应性合成的AuNP。由于饱和浓度效应,发现电化学活化程序会影响功能化电极相对于Hg(II)分析的分析性能(在皮摩尔范围内,但不在纳摩尔范围内)。使用方波阳极溶出伏安法(SWASV)作为检测模式,得到的线性浓度范围为2至12 pM,归一化灵敏度为0.296μApM-1 min-1。检出限(LOD)降至1 pM。

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