Proceedings of MATSUS Fall 2023 Conference (MATSUSFall23)
DOI: https://doi.org/10.29363/nanoge.matsus.2023.025
Publication date: 18th July 2023
Fe-N-C catalysts have made considerable advancements in their initial activity. However, their stability in acidic mediums presents a challenge that must be addressed to replace Pt in fuel cell cathodes. Unfortunately, the complicated phenomena present in fuel cells make it difficult to understand the deactivation mechanisms of Fe-N-C cathodes, hindering the development of prolonged stability solutions. Herein, we show time-resolved changes in active site density (SD) and turnover frequency (TOF) of Fe-N-C catalysts. These changes occur simultaneously with a decrease in oxygen reduction reaction (ORR) current in a temperature/gas controllable gas-diffusion electrode (GDE) flow cell. We identified a strong dependence of SD changes on operating parameters by conducting in operando diagnosis of Fe leaching. Furthermore, we drew a lifetime-dependent stability diagram that reveals a shift in the prime degradation mechanism during operations. We propose a stabilizer concept utilizing ORR-inactive site-isolated Pt ions to suppress undesirable Fe loss during ORR. Through this proof-of-concept strategy, we verified enhanced fuel cell stability with reduced Fe dissolution, offering a new design principle for durable Fe-N-C catalysts.