Enlarged Interlayer Spacing of Marigold-Shaped 1T-MoS₂ with Sulfur Vacancies via Oxygen-Assisted Phosphorus Embedding for Rechargeable Zinc-Ion Batteries

Structural unsteadiness and sluggish diffusion of divalent zinc cations in cathodes during cycling severely limit further applications of MoS₂ for rechargeable aqueous zinc-ion batteries (ZIBs). To circumvent these hurdles, herein, phosphorus (P) atom embedded three-dimensional marigold-shaped 1T MoS₂ structures combined with the design of S vacancies (Sv) are synthesized via the oxygen-assisted solvent heat method. The oxygen-assisted method is utilized to aid the P-embedding into the MoS₂ crystal, which can expand the interlayer spacing of P-MoS₂ and strengthen Zn²⁺ intercalation/deintercalation. Meanwhile, the three-dimensional marigold-shaped structure with 1T phase retains the internal free space, can adapt to the volume change during charge and discharge, and improve the overall conductivity. Moreover, Sv is not only conducive to the formation of rich active sites to diffuse electrons and Zn²⁺ but also improves the storage capacity of Zn²⁺. The electrochemical results show that P-MoS₂ can reach a high specific capacity of 249 mAh g^-1 at 0.1 A g^-1. The capacity remains at 102 mAh g^-1 after 3260 cycles at a current of 0.5 A g^-1, showing excellent electrochemical performance for Zn²⁺ ion storage. This research provides a more efficient method of P atom embedded MoS₂-based electrodes and will heighten our comprehension of developing cathodes for the ZIBs.