Advanced Impedance Analysis for Performance Degradation during Low-Temperature CO₂ Electroreduction

Electrochemical impedance spectroscopy (EIS) is a powerful tool commonly used to study electrochemical systems. Nevertheless, its application in CO2 electroreduction has been so far limited due to its complex reaction mechanism and environment. Although initial findings have demonstrated the viability of applying EIS analysis in CO2 electrolyzers, the assignment of individual processes in the impedance spectra remains ambiguous. Therefore, a more detailed investigation, especially focused on its application in evaluating degradation mechanisms, is essential. In this study, a stable gas diffusion electrode (GDE) system was developed for a comprehensive EIS and distribution of relaxation time (DRT) evaluation to assess key degradation mechanisms under accelerated stress conditions such as high current density and low operating temperature. Validated by post-mortem analysis and complementary methods, we demonstrate the viability of this approach for operando monitoring of CO2 electroreduction by assigning individual mechanistic processes in the GDE and linking them to performance degradation over time.