Dual confinement of polysulfides in boron-doped porous carbon sphere/graphene hybrid for advanced Li-S batteries

A hybrid structure consisting of boron-doped porous carbon spheres and graphene (BPCS-G) has been designed and synthesized toward solving the polysulfide-shuttle problem, which is the most critical issue of current Li-S batteries. The proposed hybrid structure showing high surface area (870 m²·g⁻¹) and high B-dopant content (6.51 wt.%) simultaneously offers both physical confinement and chemical absorption of polysulfides. On one hand, the abundant-pore structure ensures high sulfur loading, facilitates fast charge transfer, and restrains polysulfide migration during cycling. On the other hand, our density functional theory calculations demonstrate that the B dopant is capable of chemically binding polysulfides. As a consequence of such dual polysulfide confinement, the BPCS-G/S cathode prepared with 70 wt.% sulfur loading presents a high reversible capacity of 1,174 mAh·g⁻¹ at 0.02 C, a high rate capacity of 396 mAh·g⁻¹ at 5 C, and good cyclability over 500 cycles with only 0.05% capacity decay per cycle. The present work provides an efficient and cost-effective platform for the scalable synthesis of high-performance carbon-based materials for advanced Li-S batteries. [Figure not available: see fulltext.].