Proceedings of MATSUS Spring 2025 Conference (MATSUSSpring25)
DOI: https://doi.org/10.29363/nanoge.matsusspring.2025.139
Publication date: 16th December 2024
The current state-of-the-art copper electrode lifetime falls several orders of magnitude short from the 10.000 hours industrially relevant timespan.[1] Most copper catalyst cannot maintain their activity towards ethylene and other multicarbon products for more than 100 hours. Contributors to limited catalyst lifetime are copper restructuring[2] , salt formation[3] , flooding[4] and impurity deposition[5]. The restructuring of copper remains one of the least understood mechanisms. Scale up of CO2 electrolysers therefore requires a deeper understanding of the chemical processes leading up to copper instability as well as solutions on both an atomistic and system design level.
Several fundamental works have demonstrated that anodic/cathodic dissolution and redeposition of copper species is one of the main components of the restructuring process.[6] The degree of dissolution and redeposition of the positively charged copper-carbonyl complex was found to proportionate to the applied current density.[7] Based on these results, one would expect that low current CO2 electrolysis within H-cells results in very high electrode stability. Yet, it is the high current CO2 electrolysis in gas diffustion electrode (GDE) based cell configurations that demonstrate the most impressive numbers of operational hours.
In this work, restructuring on a poorly in-plane conducting PTFE based copper electrode is captured through ex situ SEM analysis. It is shown that, over time, copper migrates from the center of the electrode to the perimeter closest to the negatively charged current collector. Subsequently, a nonporous structure erupts, favouring the hydrogen evolution reaction (HER) over CO2 reduction reactions (CO2RR) after 45 minutes to 1 hour of operation at 200 mA cm-2. We then present confinement procedures that are commonly applied within (GDE) based systems to minimize the dissolution of copper species such as metaloxide nanoparticle coatings and ionomers. In addition, the redeposition location is brought closer to the dissolution location by distributing the potential more uniformly across the GDE. Using one or a combination of the outlined strategies allowed the catalyst lifetime to be lengthened to several hours.
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