Confinement of ionomer for electrocatalytic CO2 reduction reaction via efficient mass transfer pathways

ABSTRACT Gas diffusion electrodes (GDEs) mediate the transport of reactants, products and electrons for the electrocatalytic CO2 reduction reaction (CO2RR) in membrane electrode assemblies. The random distribution of ionomer, added by the traditional physical mixing method, in the catalyst layer of GDEs affects the transport of ions and CO2. Such a phenomenon results in elevated cell voltage and decaying selectivity at high current densities. This paper describes a pre-confinement method to construct GDEs with homogeneously distributed ionomer, which enhances mass transfer locally at the active centers. The optimized GDE exhibited comparatively low cell voltages and high CO Faradaic efficiencies (FE > 90%) at a wide range of current densities. It can also operate stably for over 220 h with the cell voltage staying almost unchanged. This good performance can be preserved even with diluted CO2 feeds, which is essential for pursuing a high single-pass conversion rate. This study provides a new approach to building efficient mass transfer pathways for ions and reactants in GDEs to promote the electrocatalytic CO2RR for practical applications.