Flooding Control by Electrochemically Reduced Graphene Oxide Additives in Silver Catalyst Layers for CO₂ Electrolysis

Electrolyte flooding in porous catalyst layers on gas diffusion electrodes (GDE) limits the stability and high-current performance of CO₂ and CO electrolyzers. Here, we demonstrate the in situ electroreduction of graphene oxide (GO) to reduced graphene oxide (r-GO) within a silver catalyst layer on a carbon GDE. The r-GO introduces hydrophobicity regions in the catalyst layer that help mitigate electrolyte flooding during high current density CO₂ electrolysis to CO. The flooding-resistant r-GO/Ag-coated GDE achieves a sustained Faradaic efficiency of CO at 94% for more than 8 h, compared to a rapid drop from 95% to 66% in an Ag-coated GDE without r-GO at 100 mA·cm^-2. We found that GO enhances the electrochemically active surface area of the catalyst layer during CO₂ electrolysis tests because the incorporation of GO increases the roughness of the catalyst layer. The in situ method of electrochemically reducing GO to r-GO provides a low-cost, practical approach that can be applied during standard spray-deposition procedures to develop flooding-resistant GDEs.