Atomically dispersed Co-N₄C₂ catalytic sites for wide-temperature Na-Se batteries

Sodium-selenium (Na-Se) batteries have been widely regarded as promising large-scale energy storage systems owing to the high volumetric energy density of 2530 W h L⁻¹ and natural abundance of the element sodium. However, critical drawbacks including sluggish redox kinetics, severe volume variation and shuttle effect seriously deteriorate the electrochemical performance. Herein, we propose a precompetitive coordination strategy for over-coordinated single-atom catalyst, and subsequently synthesize the six-coordinated Co electrocatalyst supported carbon nanofibers (Co-N₄C₂) for solid-state conversion in wide-temperature Na-Se batteries. The Co-N₄C₂ catalyst can not only boost the redox kinetics of solid-phase Na₂Se₂/Na₂Se, but also accelerate the electroreduction of ethylene carbonate to construct robust cathode electrolyte interphase, thereby inhibiting the irreversible phase transformation of active Se species. Furthermore, for the first time, the components of the cathode electrolyte interphase as sodium ethylene mono-carbonate are identified. Consequently, the as-synthesized free-standing Se@Co-N₄C₂ cathode with high Se-loading realizes high capacity, cycling stability and rate capability at both room temperature (20.0/40.0 ℃) and low temperature (− 11.7 ℃).