Dual-Functional MgO Nanocrystals Satisfying Both Polysulfides and Li Regulation toward Advanced Lithium-Sulfur Full...

Lithium-sulfur battery (LSB) is regarded as a preferential option for next-generation energy-storage system, but the lithium polysulfides (LiPSs) shuttling effect and the uncontrollable growth of dendritic Li in the anode impede its commercial viability. To address both of the issues simultaneously, a well-designed hybrid of MgO ultrafine nanocrystals dispersed on graphene-supported carbon nanosheets (MCG) is developed via a facile self-template strategy as dual-functional host for both sulfur and lithium. Relying on the coordination of strong LiPS-capturing capability, the shuttling effect is inhibited. Furthermore, the lithiophilic configuration with high specific surface area induce homogenous Li deposition, thus preventing the formation of disordered lithium dendrite. Integrating all these advantages, a full cell based on S@MCG cathode and Li@MCG@Cu anode exhibits a stable capacity at 0.5 C for 150 cycles with a low capacity fading rate. Furthermore, the full cell achieves a high capacity retention of 85.5% at a high S areal loading of 3.82 mg cm^-2 under the condition of a low electrolyte/sulfur ratio (E/S) of 6.5 µL mg^-1 and negative/positive capacity ratio (N/P) of 3. This strategy satisfying both cathode and anode host provides a viable approach to realize high-energy-density and dendrite-free LSBs.