Surface Engineering on Commercial Cu Foil for Steering C2H4/CH4 Ratio in CO2 Electroreduction.

Abstract

Designing catalysts with high selectivity toward C2 products in CO2 electroreduction is crucial to energy storage and sustainable development. Here, we propose a Cu foil kinetic model with abundant nanocavities possessing higher reaction rate constant k to steer the ratio of C2H4 to the competing CH4 during CO2 electroreduction. Chemical kinetic simulation demonstrates that the nanocavities could enrich the adsorbed CO surface concentration (θCOad), while the higher k helps to lower the C-C coupling barrier for CO intermediates, thus favoring the formation of C2H4. The commercial Cu foil treated with cyclic voltammetry is used to match this model, displaying a remarkable C2H4/CH4 ratio of 4.11, which is 18 times larger than that on the pristine Cu foil. This work offers a handy strategy for surface modification and provides new insights into the C-C coupling and the C2H4 selectivity in terms of mass transfer flux and energy barrier.