Multi-Shell Copper Catalysts for Selective Electroreduction of CO2 to Multicarbon Chemicals

Electrocatalytic CO2 reduction (CO2R) coupled with renewable electricity has been considered as a promising route for the sustainability transition of energy and chemical industries. However, the unsatisfactory yield of desired products, particularly multicarbon (C2+) products, has hindered the implementation of this technology. This work describes a strategy to enhance the yield of C2+ product formation in CO2R by utilizing spatial confinement effects. The finite element simulation results suggest that increasing the number of shells in the catalyst wil lead to a high local concentration of *CO and promotes the formation of C2+ products. Inspired by this, Cu nanoparticles are synthesized with desired hollow multi-shell structures. The CO2 reduction results confirm that as the number of shells increase, the hollow multi-shell copper catalysts exhibit improved selectivity toward C2+ products. Specifically, the Cu catalyst with 4.4-shell achieved a high selectivity of over 80% toward C2+ at a current density of 900 mA cm(-2). Evidence from in situ attenuated total reflection surface-enhanced infrared absorption spectroscopy unveils that the multi-shell Cu catalyst exhibits an enhanced *COatop coverage and the stronger interaction with *COatop compared to commercial Cu, confirming the simulation results. Overall, the work promises an effective approach for boosting CO2R selectivity toward value-added chemicals.