Atomically dispersed Co/Mn immobilized on O, N dual doped hollow carbon spheres as sulfur host for lithium sulfur batteries

The regulation of the chemical coordination environment in the electrocatalyst can effectively suppress the shuttle effect of sulfur species in lithium-sulfur batteries. However, the mechanism of the atomically dispersed dual metal atom with the coordination of various heteroatoms used as the sulfur cathode catalyst and trapper remains unknown. This study introduces, for the first time, atomically dispersed Co and Mn in-situ immobilized on O, N dual-doped hollow carbon spheres (SACoMn/C-(N, O)) as sulfur host. Experiments combined with density functional theory calculations reveal that the synergy between Co-(N, O) and Mn-(N, O) sites enhances the nucleation/deposition and decomposition capabilities of Li ₂S. This enhancement is attributed to the anchoring-coupling-conversion behavior of sulfur species on the SACoMn/C-(N, O) surface, which effectively restrains the shuttle effect and facilitates the conversion kinetics. Moreover, the cooperation of dual metal atoms with O, N non-metal atoms embedded in the carbon network structure accelerates electric transport and ion diffusion kinetics. The cathode demonstrates a high initial specific capacity of 890 mAh·g ⁻¹ at 1 C and show exceptional long-term cycling durability, with a low capacity degradation of 0.037 % per cycle after 1700 cycles. This research may offer novel insights into the design of dual metal atom-decorated, functionalized carbon materials to improve the conversion reaction in sulfur cathodes.