Hydrophobicity graded gas diffusion electrode with enhanced CO intermediate coverage for high-performance electroreduction of CO₂ to ethylene

Electroreduction using a gas diffusion electrode (GDE) provides an efficient method for high rate conversion of CO₂ to value-added chemicals. However, long term production with high yields remains challenging due to rapid electrolyte flooding through the hydrophobic gas diffusion layer (GDL). Here, we report a universal strategy to convert a commercial GDL into a hydrophobicity graded GDL (HGGDL) that resists electrolyte flooding. The CO₂ electroreduction performance of a family of tandem catalysts consisting of a nickel-single-atom catalyst and Cu nanoparticles immobilized on GDLs and HGGDLs is compared with respect to ethylene production. In situ Raman studies reveal that the HGGDL increases the CO intermediate coverage as a result of the higher differential pressure across the electrodes. Lower carbonate formation also is observed. Enhanced ethylene production efficiency and an order of magnitude improvement in long term stability is achieved in a membrane electrode assembly electrolyzer.