Linking electrocatalytic turnover to elementary step rates in hydrocarbon fuel oxidation

Alexander J. Zielinski, Christine Lucky and Marcel Schreier ()
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Alexander J. Zielinski: University of Wisconsin–Madison
Christine Lucky: University of Wisconsin–Madison
Marcel Schreier: University of Wisconsin–Madison

Nature Communications, 2025, vol. 16, issue 1, 1-14

Abstract: Abstract Maximizing steady-state turnover rates is a central goal in electrocatalysis research, but improving one reaction step often impedes others. Navigating these trade-offs requires methods that systematically reveal how a single parameter change affects all key steps of a reaction mechanism. Here, we use electrochemical mass spectrometry to determine the potential-dependent rates of each principal step in propane oxidation on Pt and directly relate them to the steady-state turnover rate. Our analysis reveals that low steady-state activity arises from a mismatch between the optimal potentials for adsorption, conversion, and *CO oxidation. By applying alternating potentials to individually optimize adsorption and oxidation, we overcome this limitation and achieve rates exceeding those under constant-potential operation. This step-resolved approach clarifies how individual processes interact to govern overall activity and provides a framework for the rational design of electrocatalysts carrying out complex reactions at steady-state.

Date: 2025
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DOI: 10.1038/s41467-025-63910-4

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