Ultrahigh‐Rate Lithium Storage in MoS ₂ Enabled by Isotropic Ion Transport and Fe‐Atomic Site Conversion

ABSTRACT The high‐rate performance of MoS 2 anodes in lithium‐ion batteries (LIBs) is constrained by their intrinsic anisotropic ion diffusion behavior within interlayers. Herein, we present a microwave‐induced local hotspot strategy achieved through atomic Fe doping in the MoS 2 lattice, enabling the synthesis of single‐layered MoS 2 and realizing isotropic ion transport. Additionally, Fe atoms can be converted into finer Fe nanoparticles (∼2 nm) in single‐layered MoS 2 than in few‐layered ones, which can trigger stronger spin‐polarized surface capacitance effect demonstrated by in situ magnetometry. Importantly, the Fe nanoparticles can catalyze the formation of a stable LiF‐rich solid electrolyte interphase, as confirmed by X‐ray photoelectron spectroscopy and ab initio molecular dynamics simulations. These combined advantages equip the MoS 2 with ultrahigh‐rate lithium storage (870.1 mAh g −1 ) up to 50 A g −1 (∼75 C) in half cells. Notably, 1.6 Ah pouch cells utilizing the MoS 2 anode deliver an unprecedented fast‐charging capability (81.3% retention) at 3 C. This study develops an ultrahigh‐rate MoS 2 ‐based anode and elucidates its ion transport enhancement mechanism, laying a theoretical foundation for the development of fast‐charging LIBs.