High‐Capacity and Long‐Life Rechargeable Li–CO 2 Batteries Based on N‐Doped Carbon Cathode With High‐Loaded Single Ni Atoms

As a novel type of battery for energy devices, Li–CO 2 batteries have a slow kinetic reaction during carbon dioxide reduction and evolution, which leads to problems such as high battery polarization potential, poor cycling performance, and a short lifetime. Therefore, it is important to explore electrocatalysts with high activity and stability. In this study, a novel high‐loaded single‐atom catalyst was prepared by uniformly anchoring single‐atom Ni/Co on N‐doped carbon (NiNC/CoNC). Compared with previous reports, the doping amount of Ni is as high as 10 wt%. The Li–CO 2 battery assembled using NiNC achieves a high discharge capacity of 51,125 mAh g −1 at 100 mA g −1 current density and displays a low overpotential of 1.63 V after 268 stable cycles (more than 2600 h) at 200 mA g −1 current density. The X‐ray absorption fine structure analysis of NiNC reveals the presence of Ni and NiN 4 sites. Combined with density functional theory calculations, it is found that NiNC adsorbs CO 2 reactive species more strongly. Moreover, the electronic synergism of the NiN 4 sites can weaken the decomposition barrier of the discharge product Li 2 CO 3 and accelerate the reaction kinetic process, thereby enhancing the electrocatalytic activities of CO 2 electroreduction and CO 2 reduction reaction.