Kauffmann Philip, Dick Jeffrey
Department of Chemistry, Purdue University, West Lafayette, IN, 47906, USA.
Elmore School of Electrical and Computer Engineering, Purdue University, West Lafayette, IN, 47906, USA.
Anal Bioanal Chem. 2023 Jul;415(18):4385-4390. doi: 10.1007/s00216-023-04557-2. Epub 2023 Feb 18.
Recently introduced as a method for aerosol electroanalysis, particle-into-liquid sampling for nanoliter electrochemical reactions (PILSNER) has shown promise as a versatile, highly sensitive analytical technique. To further validate the analytical figures of merit, we present correlated fluorescence microscopy and electrochemical data. The results show excellent agreement as to the detected concentration of a common redox mediator, ferrocyanide. Experimental data also suggest that PILSNER's unconventional two-electrode system is not a contributing source of error when appropriate controls are established. Finally, we address the concern that arises from two electrodes operating within such close proximity. COMSOL Multiphysics simulations confirm that with the present parameters, positive feedback is not a contributing source of error in voltammetric experiments. The simulations also show at what distances feedback could become a source of concern, which will be a factor in future investigations. Thus, this paper provides validation of PILSNER's analytical figures of merit, as well as voltammetric controls and COMSOL Multiphysics simulations to address possible confounding factors that could arise from PILSNER's experimental setup.
作为一种气溶胶电分析方法，用于纳升电化学反应的液滴进样（PILSNER）最近被引入，已显示出作为一种通用、高灵敏度分析技术的潜力。为了进一步验证其分析性能指标，我们展示了相关的荧光显微镜和电化学数据。结果表明，对于常见的氧化还原介质亚铁氰化物的检测浓度，两者具有极好的一致性。实验数据还表明，当建立适当的对照时，PILSNER非常规的双电极系统不是误差的来源。最后，我们解决了两个电极在如此近距离内工作所产生的问题。COMSOL Multiphysics模拟证实，在当前参数下，正反馈不是伏安实验中误差的来源。模拟还显示了在什么距离反馈可能成为一个问题因素，这将是未来研究中的一个因素。因此，本文对PILSNER的分析性能指标进行了验证，并提供了伏安控制和COMSOL Multiphysics模拟，以解决可能因PILSNER实验设置而产生的混杂因素。
