LAUSR

Abstract Design of efficient catalysts for electrochemical reduction of carbon dioxide (CO2) with high selectivity and activity is of great challenge, but significant for managing the global carbon balance. Herein, a series of three-dimensional (3D) single-atom metals anchored on graphene networks (3D SAM-G) with open-pore structure were successfully mass-produced via a facile in-situ calcination technique assisted by NaCl template. As-obtained 3D SANi-G electrode delivers excellent CO Faradaic efficiency (FE) of >96% in the potential range of -0.6 to -0.9 V versus reversible hydrogen electrode (RHE) and a high current density of 66.27 mA cm-2 at -1.0 V versus RHE, outperforming most of the previously reported catalysts tested in H-type cells. Simulations indicate that enhanced mass transport within the 3D open-pore structure effectively increases the catalytically active sites, which in turn leads to simultaneous enhancement on selectivity and activity of 3D SANi-G toward CO2 electroreduction. The cost-effective synthesis approach together with the microstructure design concept inspires new insights for the development of efficient electrocatalysts.