Abstract

Previous work carried out in fully liquid environ-ments and at low current densities has demonstrated that highly uniform faceted copper nanocrystals display different selectivity profiles in CO2 reduction compared to polycrystalline copper. As part of ongoing upscaling efforts, it is a matter of interest to investigate whether the high selectivity toward ethylene of copper nanocubes, which show a preferential (100) orientation, is maintained in gas-fed electrolyzers, thus enabling the energy-efficient production of this valuable commodity chemical at industrially relevant current densities. In this work, we assessed the electrochemical CO2 reduction reaction performance of highly uniform copper nanocubes loaded onto gas diffusion electrodes (GDEs) in a zero-gap device. The copper nanocube-loaded GDEs maintained high Faradaic efficiencies toward ethylene at elevated total current densities, resulting in higher overall partial current densities toward this product compared to benchmark electrodes. Interestingly, CO2 reduction to propylene, albeit with low partial current densities, was also observed. However, double-layer capacitance measurements revealed that the performance observed at high current densities is significantly influenced by electrode flooding. The findings of this study can inform future efforts geared toward optimizing the electrodes with this promising class of catalysts.

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