MoS ₅ ‐Based Cathodes With Integrated Electronic and Ionic Pathways for All‐Solid‐State Lithium Batteries

To achieve high‐performance all‐solid‐state lithium batteries (ASSLBs), it is imperative to develop cathode materials featuring simultaneous high electronic/ionic conductivities and excellent interfacial stability. MoS ₅ possesses a high specific capacity, but its low intrinsic electronic conductivity and inferior solid–solid contact with solid electrolyte severely limit its electrochemical performance. In this work, an integrated electronic and ionic conductive network is developed, where MoS ₅ particles are in situ anchored on single‐walled carbon nanotubes (SWCNTs) and further uniformly coated with Li ₇ P ₃ S ₁₁ solid electrolyte to form MoS ₅ ‐10%SWCNT@15%Li ₇ P ₃ S ₁₁ composite. The ionic and electronic conductivities of the composite are 6.13 × 10 ⁻⁴ S cm ⁻¹ and 3.87 × 10 ⁻² S cm ⁻¹ , respectively, which are approximately 2 and 5 orders of magnitude compared to those of pristine MoS ₅ with 1.40 × 10 ⁻⁶ S cm ⁻¹ and 8.80 × 10 ⁻⁷ S cm ⁻¹ . Consequently, the ASSLB employing the MoS ₅ ‐10%SWCNT@15%Li ₇ P ₃ S ₁₁ composite cathode delivers a high initial discharge capacity of 1089.2 mAh g ⁻¹ with a high initial Coulombic efficiency of 92.4% at 0.1 A g ⁻¹ . After 500 cycles at 0.5 A g ⁻¹ , it retains a reversible specific capacity of 798.02 mAh g ⁻¹ with a capacity retention of 73.6%. These findings demonstrate that the MoS ₅ ‐10%SWCNT@15%Li ₇ P ₃ S ₁₁ nanocomposite is a promising cathode material for ASSLBs.