Fabrication of long-life quasi-solid-state Na-CO2 battery by formation of Na2C2O4 discharge product

Rechargeable Na-CO2 batteries are promising energy-storage devices due to their high energy density, environmental friendliness, and cost effectiveness. However, the insulating nature and irreversibility of the Na2CO3 discharge product cause large polarization and poor cyclicity. Here, we report a reversible quasi-solid-state Na-CO2 battery that is constructed by the synergistic action of a Co-encapsulated N-doped carbon framework catalyst and gel electrolyte to ensure the formation of a highly reversible Na2C2O4 discharge product. Experiments and density functional theory calculations indicate that the electron-agglomeration effect of Co nanoparticles enhances CO2 adsorption and lowers energy barrier, as well as promotes Na2C2O4 generation. A gel electrolyte containing an imidazole organic cation is used to inhibit the decomposition of the thermodynamically unstable Na2C2O4. The fabricated Na-CO2 battery exhibits a high discharge capacity of 3,094 mAh g−1, a high-rate performance of 1,777 mAh g−1 at a current density of 0.5 mA cm−2, and excellent cycling performance of 366 cycles (2,200 h).