High‐Performance, Long‐Life, Rechargeable Li–CO2 Batteries based on a 3D Holey Graphene Cathode Implanted with Single Iron Atoms

Abstract A highly efficient cathode catalyst for rechargeable Li–CO 2 batteries is successfully synthesized by implanting single iron atoms into 3D porous carbon architectures, consisting of interconnected N,S‐codoped holey graphene (HG) sheets. The unique porous 3D hierarchical architecture of the catalyst with a large surface area and sufficient space within the interconnected HG framework can not only facilitate electron transport and CO 2 /Li + diffusion, but also allow for a high uptake of Li 2 CO 3 to ensure a high capacity. Consequently, the resultant rechargeable Li–CO 2 batteries exhibit a low potential gap of ≈1.17 V at 100 mA g −1 and can be repeatedly charged and discharged for over 200 cycles with a cut‐off capacity of 1000 mAh g −1 at a high current density of 1 A g −1 . Density functional theory calculations are performed and the observed appealing catalytic performance is correlated with the hierarchical structure of the carbon catalyst. This work provides an effective approach to the development of highly efficient cathode catalysts for metal–CO 2 batteries and beyond.