Proceedings of MATSUS Spring 2024 Conference (MATSUS24)
DOI: https://doi.org/10.29363/nanoge.matsus.2024.153
Publication date: 18th December 2023
CO2 electroreduction (CO2E) offers a path generate widely used chemicals using CO2 waste and renewable electricity. The viability of CO2E requires further progress in combined performance metrics such as selectivity, current density, and carbon utilization (among others). This is challenged by the loss of CO2 into carbonates in high pH systems. CO2E operation in acid is one strategy to overcome this loss process, as carbonate species would get locally regenerated into CO2 in a high-density H+ environment. Unfortunately, this approach also promotes the undesired hydrogen evolution reaction (HER). Control over the local CO2E reaction environment, and ion species in the double layer, has been shown as a promising direction to address this challenge.1–5 Here, we present a strategy that uses different ionomer coatings to modulate the local reaction environment. We perform mechanistic studies, including operando spectroscopies, to study how these affect the dynamics of key ion species and reaction intermediates over the catalyst surface, and correlate this with performance trends. The ionomer coated PTFE/Cu electrodes achieve a Faradaic Efficiency of 73±6% for CO2 to C2+ at 400 mA/cm2 using an acidic electrolyte. This approach opens new possibilities for optimizing CO2 electroreduction processes and achieving higher selectivity for value-added products, contributing to the advancement of sustainable and efficient energy conversion technologies.
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