Restrained interfacial resistance Co5.47N@C derived from metal-organic frameworks for advanced Li-CO2 batteries cathodes

Lithium-carbon dioxide (Li-CO2) batteries are novel high energy density energy storage devices that can simultaneously enrich and convert CO2, but their widespread implementation is hindered by the continuous accumulation of lithium carbonate at the cathode. Herein, we developed non-precious metal cobalt-based nitride matrix composite Co5.47N@C based on metal-organic frameworks precursor for the catalytic cathode of advanced Li-CO2 batteries. The highly stable Co5.47N achieves favorable adsorption and catalysis of CO2 molecules by virtue of the excellent electronic structure on the surface, while the nanoscale high dispersion also effectively promotes interfacial electron transfer. As expected, the assembled Li-CO2 battery exhibits excellent electrochemical performance in the discharge capacity of 10,000 mAh g(-1) and a cycling capability of about 400 h. Further density functional theory (DFT) calculations explored the relationship between electronic structure and electrochemical activity. This work promotes the development of catalytic materials for Li-CO2 batteries cathode.