Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.205
Publication date: 18th December 2023
Electrochemical reduction of CO2 into valuable chemicals from renewable electricity is envisioned as a means to avoid fossil resources in many applications. As the field is urged to increase its technology readiness, numerical models are necessary tools to accelerate device development.[1], [2] Nevertheless, fully reliable and accurate models have yet to be developed. The challenges lie in the complexity of the reaction and the convolution of many effects including mass-transport, microkinetics, and kinetics. In this study, we aim at deconvoluting these aspects by studying the reduction of CO2 into carbon monoxide at a flat silver electrode, one of the most studied catalyst material under controlled mass-transport conditions. We hypothesize that one of the major gap between previous model and experiments is the carbon monoxide affinity for some active sites that prevent other electrochemical reactions to take place. In order to model this effect independently, we conducted a series of measurement in presence of CO and determined equilibrium constants to be fed into a microkinetic model. These experiments confirmed our hypothesis that the produced CO significantly hinders the competitive hydrogen evolution reaction. We then developed a computational model and show that the consideration of the CO effect on hydrogen evolution reaction allows for improved accuracy in predicting experimental observations.[3] The study also provides unexpected insights in the different nature of active sites responsible for CO and H2 evolution at Ag electrodes.
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