Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.201
Publication date: 18th December 2023
Renewable-powered electrochemical carbon dioxide (CO2) reduction reaction (CO2R) offers an attractive approach for the generation of low-carbon footprint chemicals. CO2R in acid has emerged as a promising solution to overcome drawbacks of traditional CO2R alkaline electrolyzers, such as limited carbon efficiency, which can lead to low energy efficiencies. Ionic species in the electrolyte have proven crucial in CO2R.[1,2] Especially in acid, cations have been shown to be essential to enable CO2R.[3] The role of anions, on the other hand, has received less attention in this context. Further advances in the field rely on resolving the CO2R environment and the role of ionic species at increasing current densities, where CO2R onset takes place in acid (> 50 mA·cm-2).[4] Herein, we study the role of anionic species by assessing the local CO2R reaction environment at high current densities (> 200 mA·cm-2), using operando Surface Enhanced Raman Spectroscopy (SERS). We have done so by investigating the different adsorbed intermediates and anions at varying pHs using a copper catalyst and H2SO4/K2SO4 electrolyte. We correlated changes in selectivity with presence and stabilization of adsorbed species and CO2R intermediates, revealing the key dynamic role that anions play in the competition between CO2R, carbonate-loss-regeneration pathways, and the suppression of HER in acid. Our study shows the paramount importance of measuring these processes at high current densities, offering crucial insights for advancing in acid CO2R.
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