In Situ Anchoring Ultrafine ZnS Nanodots on 2D MXene Nanosheets for Accelerating Polysulfide Redox and Regulating Li Plating

Abstract Lithium−sulfur (Li−S) battery is a promising energy storage system due to its cost effectiveness and high energy density. However, formation of Li dendrites from Li metal anode and shuttle effect of lithium polysulfides (LiPSs) from S cathode impede its practical application. Herein, ultrafine ZnS nanodots are uniformly grown on 2D MXene nanosheets by a low‐temperature (60 °C) hydrothermal method for the first time. Distinctively, the ZnS nanodot‐decorated MXene nanosheets (ZnS/MXene) can be easily filtered to be a flexible and freestanding film in several minutes. The ZnS/MXene film can be used as a current collector for Li‐metal anode to promote uniform Li deposition due to the superior lithiophilicity of ZnS nanodots. ZnS/MXene powders obtained by freeze drying can be used as separator decorator to address the shuttle effect of LiPSs due to their excellent adsorbability. Theoretical calculation proves that the existence of ZnS nanodots on MXene can obviously improve the adsorption ability of ZnS/MXene with Li+ and LiPSs. Li−S full cells with composite Li‐metal anode and modified separator exhibit remarkable rate and cycling performance. Other transition metal sulfides (CdS, CuS, etc.) can be also grown on 2D MXene nanosheets by the low‐temperature hydrothermal strategy.