Publication date: 21st July 2025
Scalable electrocatalytic conversion of CO₂ to formate hinges on developing gas diffusion electrodes (GDEs) with high activity, selectivity, and durability. In the first study, we investigated how pulsed electrodeposition parameters modulate catalyst layer microstructure and impact CO₂ reduction performance. Lowering the duty cycle increased catalyst dispersity within the GDE’s three-dimensional matrix, improving catalyst utilization and generating smaller, denser nucleation sites. When paired with a CO₂-philic Sustainion XC-02 ionomer, these pulsed-deposited Bi-GDEs reached industrially relevant current densities (≈ 210 mA/cm²) with 94% faradaic efficiency at -1.0 V vs. RHE, superior to commercial GDEs in similar conditions. The second study tackled the stability challenge by alloying and mixing Sb into the GDE catalytic layer. Bi-based GDEs can suffer from rapid degradation in the first thirty minutes, leading to short electrode lifetimes. Our investigations revealed that adding Sb facilitates the re-deposition of the electrocatalyst during CO₂ reduction, and while the catalyst morphology in the catalytic layer changes during CO₂ reduction, the electrode activity remains nearly unchanged. In other words, the added Sb acts as a structural component in a self-repairing process, leading to elevated electrode resilience. These findings are part of an ongoing paradigm shift in energy materials design from ‘ultra stable’ materials to ‘dynamically resilient’ components and serve as an example for extending the self-repairing perspective from the electrocatalyst to a catalytic layer volume.
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