Engineering copper nanoparticle electrodes for tunable electrochemical reduction of carbon dioxide

The electrochemical conversion of CO2 catalyzed by copper (Cu)-based materials is widely reported to produce different valuable molecules, and the selectivity for a specific product can be achieved by tuning the characteristics of catalytic materials. Differing from these studies on materials, the present work focuses on the engineering of gas diffusion electrodes in order to properly modify the selectivity, particularly by changing the Cu nanoparticle catalyst loading of the electrodes. Low catalyst loadings (≤ 0.25 mg cm−2) favor CH4 production, and intermediate (∼ 1.0 mg cm−2) loadings shift the selectivity toward C2H4. Eventually, larger values (≥ 2.0 mg cm−2) promote CO production. Detailed analyses reveal that both bulk and local CO generation rates, and charge transfer mechanism are responsible for the observed loading-dependent selectivity. The present work provides a new strategy for steering the CO2RR selectivity by simple electrode engineering beyond material development.