Vacancy‐Engineered ZnS/N‐Doped Carbon on rGO as a Multifunctional Separator Coating for High Stable Lithium‐Sulfur Batteries

Commercialization of lithium‐sulfur (Li‐S) batteries (LSBs) is limited by the shuttle effect, caused by the dissolution and migration of lithium polysulfides (LiPSs) that lead to active material loss and poor cycling stability. To address this challenge, we developed a multifunctional separator consisting of ZnS‐decorated nitrogen‐doped hierarchical porous carbon anchored onto a reduced graphene oxide (rGO) layer coated on a polypropylene separator. The hierarchical micropore‐mesopore structure of the ZIF‐8‐derived carbon provides strong physical adsorption of LiPSs, while vacancy‐rich ZnS nanoparticles offer chemical adsorption and catalytic conversion of polysulfides. In addition, nitrogen‐doped carbon and the rGO framework enhance electronic conductivity and facilitate lithium‐ion transport across the separator. Benefiting from these synergistic effects, the modified separator enables the Li‐S cell to deliver an initial discharge capacity of 1120.2 mAh g −1 at 300 mA g −1 and maintain 75.1% capacity retention with 99.7% coulombic efficiency after 200 cycles, demonstrating significantly improved polysulfide blocking compared with rGO‐coated and bare separators. This work highlights an effective strategy for engineering ZnS/carbon composite separators to achieve highly stable LSBs.