Dynamic Interfacial Reaction Rates from Electrochemistry-Mass Spectrometry

Kevin Krempl, Degenhart Hochfilzer, Soren B. Scott, Jakob Kibsgaard, Peter C.K. Vesborg, Ole Hansen, Ib Chorkendorff*

*Corresponding author for this work

Research output: Contribution to journalJournal articleResearchpeer-review

Abstract

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.

Original languageEnglish
JournalAnalytical Chemistry
Volume93
Issue number18
Pages (from-to)7022-7028
ISSN0003-2700
DOIs
Publication statusPublished - 2021

Bibliographical note

Funding Information:
Support was offered by the Villum Foundation V-SUSTAIN grant 9455 to the Villum Center for the Science of Sustainable Fuels and Chemicals.

Publisher Copyright:
© 2021 The Authors. Published by American Chemical Society.

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