Fine-tuned combination of cell and electrode designs unlocks month-long stable low temperature Cu-based CO2 electrolysis

The urgency of achieving green chemical production through Cu-based CO2 electroreduction necessitates a rapid transition towards technical maturity and commercialization in the pursuit of addressing the global imperative of decarbonization. Surprisingly, limited emphasis has been placed on exploration of readily scalable cell and electrode designs, which are pivotal in ushering in the era of stable and selective CO2 electrolyzers, showcasing the innovative potential within this area. Herein, we report a breakthrough in achieving month-long stability in the production of C2H4, representing an unprecedented milestone in low-temperature CO2 to C2+ electrolysis. Initial investigations involved the evaluation of five distinct cell architectures for Cu-based CO2 electrolyzers, guided by considerations of cell potentials, scalability with current technology, and CO2 crossover. An innovative multilayer Gas Diffusion Electrode (GDE), featuring an anion exchange ionomer and metal oxide layer, is introduced for CEM-based zero-gap cells, enabling C2H4 formation despite acidic surroundings. However, selectivity towards C2H4 proved suboptimal for extended stability testing. Conversely, the tailored multilayer GDE for one-gap cell architecture achieves a commendable 54 % faradaic efficiency (FE) towards C2+ products at 300 mA/cm2. Remarkably, chronopotentiometric tests demonstrate 720 h of stability (FEC2H4 > 20 %) at 100 mA/cm2. At higher current densities (300 mA/cm2), stability is reduced to 75 h, with detailed analyses revealing distinct degradation mechanisms. At 100 mA/cm2, salt formation predominates, while at 300 mA/cm2, catalyst layer restructuring degrades catalytic activity towards C2H4. Our research underscores the potential for stable, high C2+ selectivity through innovative electrode design and scalable cell architectures, advancing sustainable CO2 utilization.