Vacancy-engineered 1T-MoS₂/MnS heterostructures on graphene ribbons enabling high-energy, long-cycle Lithium-ion...

Transition metal sulfides (TMSs) such as MoS₂ are attractive anode candidates due to their high capacity and redox activity. However, the conventional 2H-MoS₂ suffers from low conductivity and severe volume changes, leading to rapid capacity fading. To overcome these drawbacks, we designed vacancy-engineered 1T-MoS₂/MnS heterostructures anchored on graphene ribbons (GRs/MnS-MoS₂). Phase engineering stabilizes the metallic 1T-MoS₂, while sulfur vacancies and heterointerfaces enhance Li⁺ adsorption and charge transfer. The graphene ribbons provide mechanical support and conductivity. Density functional theory and in situ studies confirm that vacancies and heterostructures synergistically improve conductivity, lower resistance, and accelerate Li⁺ kinetics. Furthermore, MnS induces partial Mo⁴⁺ reduction, stabilizing the 1T phase. Electrochemical tests show that GRs/MnS-MoS₂ achieves 1096 mAh g^-1 at 0.1 A g^-1 and 588 mAh g^-1 at 2.0 A g^-1, with excellent cycling stability. Full-cell assemblies with LiNi_0.8Co_0.1Mn_0.1O₂ (NCM811) and LiFePO₄ (LFP) cathodes deliver energy densities of 521.3 and 328.5 Wh kg^-1, respectively. This work provides an effective route for developing advanced TMS-based anodes via phase, vacancy, and interface engineering.