Targeted Synergy between Adjacent Co Atoms on Graphene Oxide as an Efficient New Electrocatalyst for Li–CO2 Batteries

Abstract Li–CO 2 batteries are an attractive technology for converting CO 2 into energy. However, the decomposition of insulating Li 2 CO 3 on the cathode during discharge is a barrier to practical application. Here, it is demonstrated that a high loading of single Co atoms (≈5.3%) anchored on graphene oxide (adjacent Co/GO) acts as an efficient and durable electrocatalyst for Li–CO 2 batteries. This targeted dispersion of atomic Co provides catalytically adjacent active sites to decompose Li 2 CO 3 . The adjacent Co/GO exhibits a highly significant sustained discharge capacity of 17 358 mA h g −1 at 100 mA g −1 for >100 cycles. Density functional theory simulations confirm that the adjacent Co electrocatalyst possesses the best performance toward the decomposition of Li 2 CO 3 and maintains metallic‐like nature after the adsorption of Li 2 CO 3 .