Developing Rapid‐Charging Li‐S Batteries via “Target Catalysis” of Cations and Anions Modified Electrocatalyst

The shuttle effect and sluggish sulfur reduction reaction have resulted in significantly low efficiency and poor high current cycling stability in lithium-sulfur batteries, impeding their practical applications. To address these challenges, the introduction of Ni cations into MoS₂ grown on reduced graphene oxide (MoS₂/rGO) induces the formation of impurity energy levels between the conduction and valence bands of MoS₂. Additionally, the introduction of anionic Se expands the interlayer spacing, enhances intrinsic conductivity, and improves ion diffusion rates. Simultaneously introducing anionic and cationic species into the MoS₂/rGO causes the center of the d-band to shift upward, reducing the occupancy of electrons in antibonding orbitals. This modification leads to a rearrangement of the electronic structure of Mo, accelerating the redox reactions of lithium polysulfides. It particularly enhances the binding energy and lowers the conversion energy barrier of Li₂S₄. Consequently, the Li||S coin cell with the Ni-MoSSe/rGO cathode demonstrates an initial capacity of 446 mAh g^-1 at 20 C, with a remarkable capacity retention of ≈96.7% after 200 cycles. Moreover, even under high sulfur loading conditions (6.45 mg cm^-2) and a low electrolyte/sulfur ratio (5.4 µL mg^-2), it maintains a high areal capacity of 6.42 mAh cm^-2.