The lithium‐carbon dioxide (Li‐CO2) battery as a novel metal‐air battery has a high specific energy density and unique CO2 conversion ability. However, its further development is limited by incomplete product decomposition resulting in poor cycling and rate performance. In this work, Cu‐tetra(4‐carboxyphenyl) porphyrin (Cu‐TCPP) nanosheets are prepared through the solvothermal method successfully. An efficient Li‐CO2 battery with Cu‐TCPP as catalyst achieves a high discharge capacity of 20393 mAh g−1 at 100 mA g−1, a long‐life cycle of 123 at 500 mA g−1, and a lower overpotential of 1.8 V at 2000 mA g−1. Density functional theory calculation reveals that Cu‐TCPP has higher adsorption energy of CO2 and Li2CO3 compared with TCPP, and a large number of electrons gather near the Cu‐N4 active sites in Cu‐TCPP. Therefore, the excellent CO2 capture ability of the porphyrin ligand and the synergic catalytic effect of Cu atom in Cu‐TCPP promote the thermodynamics and kinetics of CO2 reduction and evolution processes.
scite is a Brooklyn-based organization that helps researchers better discover and understand research articles through Smart Citations–citations that display the context of the citation and describe whether the article provides supporting or contrasting evidence. scite is used by students and researchers from around the world and is funded in part by the National Science Foundation and the National Institute on Drug Abuse of the National Institutes of Health.