Spongy Silicon‐Doped MoS2 via Long‐Chain Molecule Induction and Mesopore Confinement for Ultra‐Stable Lithium‐Ion Storage

Abstract Layered transition metal dichalcogenides (LTMDs), such as MoS 2 , are promising anode materials for high‐energy‐density lithium‐ion batteries (LIBs) due to their high specific capacities. However, their practical applications are hindered by poor cycling stability resulting from the instable structure during charge/discharge and inherently low electronic conductivity. To tackle these issues, herein, this study presents the design and synthesis of spongy silicon‐doped MoS 2 induced by the long‐chain molecules in mesopores. The material consists of few‐layered nanofragments with high porosity, resulting in abundant edge sites and sulfur vacancies. These structural features can promote Li + transport and accommodate electrode volume changes during charge/discharge. Electrochemical and theoretical analyses reveal that silicon doping enhances the electronic conductivity of MoS 2 , while the nanostructure design enables reversible Li⁺ diffusion along the edges, distinct from Li + storage in the interlayers of conventional MoS 2 anodes. Notably, the material delivers a high reversible capacity of 767.9 mAh g −1 at 0.1 A g −1 and exhibits remarkable rate capability. Moreover, it demonstrates superior cycling stability with over 83% capacity retention even after 1000 cycles at 1.0 A g −1 , outperforming most existing MoS 2 ‐based anode materials. This work paves a new way for designing high‐performance LTMD‐based anodes for LIBs and beyond.