An Engineered Separator with N-Doped Graphene Nanosheets for Trapping Polysulfides in Advanced Li-S Batteries

Lithium–sulfur (Li-S) battery technology has attracted significant research interest owing to sulfur’s remarkable theoretical capacity and exceptional energy density potential. Nevertheless, the low conductivity of sulfur and the “shuttle effect” pose challenges to its practical applications. To enhance electrochemical performance, this work developed nitrogen-doped graphene (NG) nanosheets as a separator coating for Li-S battery. As a modification layer for separators, NG acts as a physical barrier that prevents polysulfides from migrating across the separator to reach the anode, thereby mitigating the shuttle effect. Additionally, NG improves the conductivity of the separator and enhances wettability between the separator and electrolyte, facilitating uniform transmission of lithium ions. Notably, NG functionalized separators demonstrate excellent mechanical flexibility, contributing to improved cycle stability for batteries. Furthermore, theoretical calculations indicate a strong interaction between NG and lithium polysulfides (LiPSs), effectively inhibiting polysulfide migration. The Li-S battery utilizing the NG modified separator maintains a capacity retention rate of 51.5% after 100 cycles at 0.1 C with a sulfur loading of 1.47 mg/cm2 and exhibits a capacity decay rate of only 0.092% after 500 cycles at a discharge rate of 1 C. This work highlights the potential advantages of employing NG as a separator coating layer in enhancing the electrochemical performance of the Li-S battery.