Paired Electrosynthesis at Interdigitated Microband Electrodes: Exploring Diffusion and Reaction Zones in the Absence of a Supporting Electrolyte

IF 4.6 Q1 CHEMISTRY, ANALYTICAL ACS Measurement Science Au Pub Date : 2024-04-17 DOI:10.1021/acsmeasuresciau.4c00009
Tingran Liu, Evaldo Batista Carneiro-Neto, Ernesto Pereira, James E. Taylor, Philip J. Fletcher and Frank Marken*, 
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Abstract

Electrosynthesis traditionally requires dedicated reactor systems and an added electrolyte, although some paired electrosynthesis processes are possible at interdigitated microband electrodes simply immersed in solution and without an intentionally added electrolyte. Here, 1,1′-ferrocenedimethanol oxidation and activated olefin electro-hydrogenation reactions are investigated as model processes at a Pt–Pt interdigitated microband array electrode with 5 μm width and with 5 μm interelectrode gap. Voltammetric responses for electro-hydrogenation are discussed, and product yields are determined in methanol (MeOH) in the presence/absence of an added electrolyte (LiClO4). An isotope effect is observed in CH3OD solvent, leading to olefin monodeuteration linked to a fast EC-type process close to the cathode surface (in the cathode reaction zone) rather than to charge annihilation in the interelectrode zone. A finite element simulation is employed to visualize/discuss reaction zones and to contrast the rate of charge annihilation processes with/without a supporting electrolyte.

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交织微带电极上的配对电合成:探索无支撑电解质时的扩散和反应区
电合成传统上需要专用的反应器系统和添加的电解液,但在仅仅浸入溶液中而不刻意添加电解液的交错微带电极上也可以进行一些成对的电合成过程。本文以 1,1′-二茂铁甲醇氧化反应和活化烯烃电加氢反应为模型,研究了在宽度为 5 μm、电极间隙为 5 μm 的铂-铂交错微带阵列电极上的反应过程。讨论了电加氢的伏安反应,并测定了在有/无添加电解质(LiClO4)的甲醇(MeOH)中的产物产率。在 CH3OD 溶剂中观察到同位素效应,导致烯烃单脱氢与靠近阴极表面(阴极反应区)的快速 EC 型过程有关,而不是与电极内区的电荷湮灭有关。采用有限元模拟来直观显示/讨论反应区,并对比有/无支撑电解质的电荷湮灭过程的速率。
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来源期刊
ACS Measurement Science Au
ACS Measurement Science Au 化学计量学-
CiteScore
5.20
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0.00%
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0
期刊介绍: ACS Measurement Science Au is an open access journal that publishes experimental computational or theoretical research in all areas of chemical measurement science. Short letters comprehensive articles reviews and perspectives are welcome on topics that report on any phase of analytical operations including sampling measurement and data analysis. This includes:Chemical Reactions and SelectivityChemometrics and Data ProcessingElectrochemistryElemental and Molecular CharacterizationImagingInstrumentationMass SpectrometryMicroscale and Nanoscale systemsOmics (Genomics Proteomics Metabonomics Metabolomics and Bioinformatics)Sensors and Sensing (Biosensors Chemical Sensors Gas Sensors Intracellular Sensors Single-Molecule Sensors Cell Chips Arrays Microfluidic Devices)SeparationsSpectroscopySurface analysisPapers dealing with established methods need to offer a significantly improved original application of the method.
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