First‐Principles Study on Introducing Fluorine Doping and Sulfur Vacancy into MoS2 for Advanced Lithium Storage

Abstract MoS 2 , a potential anode material for lithium ion batteries (LIBs), boasts high specific capacity, a unique layered structure, and large interlayer spacing, but struggles with poor conductivity and volume effect. Starting from improving the intrinsic electronic conductivity of MoS 2 , this study innovatively introduces F‐doping and sulfur vacancies into MoS 2 crystals to form F‐MoS 2‐x crystals, and investigates its structural features and LIBs applications through first‐principle calculations. The rationality and stability of F‐MoS 2−x are calculated by phonon spectra. The density of states calculations reveals that F‐doping and sulfur vacancies effectively alter MoS 2 's electronic state, reducing its intrinsic band‐gap and confirming F‐MoS 2‐x 's superior electronic conductivity theoretically. They also significantly decrease lithium‐ion diffusion resistance on F‐MoS 2‐x 's surface, potentially enabling high‐rate performance. Besides, the calculation of adsorption energy and differential charge density reveals strong adsorption between F‐MoS 2‐x and lithium ions, which favors long‐term cycle stability. Notably, with each F‐MoS 2‐x molecule storing up to 4.5 Li, corresponding to a theoretical capacity of 769 mAh g −1 , higher than MoS 2 's 670 mAh g −1 . This study provides a meaningful reference value for the modification of MoS 2 .