期刊
ANALYTICAL CHEMISTRY
卷 93, 期 18, 页码 7022-7028出版社
AMER CHEMICAL SOC
DOI: 10.1021/acs.analchem.1c00110
关键词
-
资金
- Villum Foundation V-SUSTAIN grant [9455]
The study introduces a mathematical framework based on a mass transport model to obtain a quantitative and truly dynamic partial current density from measured mass spectrometer signal by deconvolution. The time resolution of electrochemistry-mass spectrometry is limited by entropy-driven processes during mass transport to the mass spectrometer. The methodology is validated by comparing measured impulse responses of hydrogen and oxygen evolution to model predictions and applied to uncover dynamic phenomena during hydrogen and oxygen evolution in an acidic electrolyte.
Electrochemistry-mass spectrometry is a versatile and reliable tool to study the interfacial reaction rates of Faradaic processes with high temporal resolutions. However, the measured mass spectrometric signals typically do not directly correspond to the partial current density toward the analyte due to mass transport effects. Here, we introduce a mathematical framework, grounded on a mass transport model, to obtain a quantitative and truly dynamic partial current density from a measured mass spectrometer signal by means of deconvolution. Furthermore, it is shown that the time resolution of electrochemistry-mass spectrometry is limited by entropy-driven processes during mass transport to the mass spectrometer. The methodology is validated by comparing the measured impulse responses of hydrogen and oxygen evolution to the model predictions and subsequently applied to uncover dynamic phenomena during hydrogen and oxygen evolution in an acidic electrolyte.
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