Tailoring Heterogeneous Antiphase Boundaries in Multi‐Shelled Structure to Boost Na ⁺ Diffusion Kinetics for High‐Rate Sodium–Ion Batteries

ABSTRACT MoS 2 is a promising anode of sodium–ion batteries (SIBs), owing to high theoretical capacity and environmental benignity. However, its sluggish Na + diffusion kinetics severely impair rate capability and cycling stability. In this study, we rationally designed MoS 2 /Fe x Mo 2 S 4 hollow multi‐shelled structure (HoMS). Wherein, the precise regulation of Mo/Fe molar ratio induces the formation of unique alternating antiphase boundaries (APBs) at the heterointerfaces reported for the first time arising from the lattice mismatch of (002) crystal planes between MoS 2 and Fe x Mo 2 S 4 . These APBs provide excess diffusion channels for Na + in lattice, accompanying unique structure of HoMS to achieve 3D Na + diffusion path. Additionally, the electron conductivity is promoted due to the construction of a built‐in electric field, thus facilitating fast reversible electrochemical reaction for high rate capability. Meanwhile, the void space in HoMS with APBs buffers volume change during cycling, enhancing cycling stability. Particularly, the MoS 2 /Fe x Mo 2 S 4 hollow double‐shelled sphere exhibits a high specific capacity of 743.6 mAh g −1 at 0.2 A g −1 , and a capacity of 226.4 mAh g −1 is still retained at 10 A g −1 , demonstrating excellent rate capability. This work provides an inspiration for constructing hollow multi‐shelled structure anode materials with abundant APBs lattice mismatch for fast and reversible electrochemical reactions.