Immobilizing Polysulfide by In Situ Topochemical Oxidation Derivative TiC@Carbon‐Included TiO₂ Core–Shell Sulfur Hosts for Advanced Lithium–Sulfur Batteries

Abstract

The performance of lithium-sulfur (Li-S) batteries is greatly hindered by the notorious shuttle effect of lithium polysulfides (LiPSs). To address this issue, in situ topochemical oxidation derivative TiC@carbon-included TiO₂ (TiC@C-TiO₂ ) core-shell composite is designed and proposed as a multifunctional sulfur host, which integrates the merits of conductive TiC core to facilitate the redox reaction kinetics of sulfur species, and porous C-TiO₂ shell to suppress the dissolution and shuttling of LiPSs through chemisorption. A unique dual chemical mediation mechanism is demonstrated for the proposed TiC@C-TiO₂ composite that synergistically entraps LiPSs through thiosulfate/polythionate conversion coupled with strong polar-polar interaction. The morphological characterization reveals that the TiC@C-TiO₂ -based cathode can well regulate the distribution of electrode materials to retard their accumulation inside the electrode, ensuring effective contact between the active materials and electrolyte. Based on its unique function and structure, the cathode delivers an improved capacity of 1256 mAh g^-1 at 0.2C, a remarkable rate capability of 643 mAh g^-1 , and an ultralow capacity decay rate of 0.065% per cycle at 2C over 900 cycles. This work not only demonstrates a dual chemical mediation mechanism to immobilize LiPSs, but also provides a universal strategy to construct multifunctional sulfur hosts for advanced Li-S batteries.