A temperature-controlled photoelectrochemical cell for quantitative product analysis
A temperature-controlled photoelectrochemical cell for quantitative product analysis
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DOI：
10.1063/1.5024802
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发表时间：
2018-05-01
影响因子：
1.6
通讯作者：
McCloskey, Bryan D.
中科院分区：
文献类型：
--
作者：
Corson, Elizabeth R.;Creel, Erin B.;McCloskey, Bryan D.
在这项研究中，我们描述了一个温度控制的光电化学电池的设计和操作，用于分析在照明工作电极下形成的气体和液体产物。该电池专为定量分析在低电流密度下产生多种气体和液体产物的光电化学过程而设计，并且表现出限制的反应物浓度，这使得这些过程无法在传统的单室电解槽中进行研究。本文提出的电池的几何结构使光电极能够进行正面照射，并使电极表面积与电解质体积比最大化，从而增加了液体产物浓度，从而提高了对它们的非原位光谱灵敏度。在操作过程中，气体通过工作电极室中的电解质起泡，以保持饱和的反应物浓度并连续混合电解质。气体产品由在线气相色谱仪检测，液体产品由核磁共振分析。通过检查银箔电极上的二氧化碳还原，验证了电池性能，显示出与文献报道的结果和在标准平行电极电化学电池中进行的相同实验相当的结果。为了证明该电池的光电化学应用，在等离子体纳米结构银光电阴极上进行了CO2还原实验，并在黑暗和光照条件下显示了不同的产物分布。AIP出版社出版。
In this study, we describe the design and operation of a temperature-controlled photoelectrochemical cell for analysis of gaseous and liquid products formed at an illuminated working electrode. This cell is specifically designed to quantitatively analyze photoelectrochemical processes that yield multiple gas and liquid products at low current densities and exhibit limiting reactant concentrations that prevent these processes from being studied in traditional single chamber electrolytic cells. The geometry of the cell presented in this paper enables front-illumination of the photoelectrode and maximizes the electrode surface area to electrolyte volume ratio to increase liquid product concentration and hence enhances ex situ spectroscopic sensitivity toward them. Gas is bubbled through the electrolyte in the working electrode chamber during operation to maintain a saturated reactant concentration and to continuously mix the electrolyte. Gaseous products are detected by an in-line gas chromatograph, and liquid products are analyzed ex situ by nuclear magnetic resonance. Cell performance was validated by examining carbon dioxide reduction on a silver foil electrode, showing comparable results both to those reported in the literature and identical experiments performed in a standard parallel-electrode electrochemical cell. To demonstrate a photoelectrochemical application of the cell, CO2 reduction experiments were carried out on a plasmonic nanostructured silver photocathode and showed different product distributions under dark and illuminated conditions. Published by AIP Publishing.