Double‐Shelled C@MoS2 Structures Preloaded with Sulfur: An Additive Reservoir for Stable Lithium Metal Anodes

The growth of Li dendrites hinders the practical application of lithium metal anodes (LMAs). In this work, a hollow nanostructure, based on hierarchical MoS2 coated hollow carbon particles preloaded with sulfur (C@MoS2/S), was designed to modify the LMA. The C@MoS2 hollow nanostructures serve as a good scaffold for repeated Li plating/stripping. More importantly, the encapsulated sulfur could gradually release lithium polysulfides during the Li plating/stripping, acting as an effective additive to promote the formation of a mosaic solid electrolyte interphase layer embedded with crystalline hybrid lithium‐based components. These two factors together effectively suppress the growth of Li dendrites. The as‐modified LMA shows a high Coulombic efficiency of 98 % over 500 cycles at the current density of 1 mA cm−2. When matched with a LiFePO4 cathode, the assembled full cell displays a highly improved cycle life of 300 cycles, implying the feasibility of the proposed LMA. Functional microcapsules for stable lithium metal anodes (LMAs) have been designed based on double‐shelled C@MoS2 nanostructures preloaded with sulfur. The as‐prepared C@MoS2/S structures can provide a long‐term supply of polysulfides, which serve as an effective additive for improving the stability of the solid electrolyte interphase on the LMA, thus prolonging the cycle life.