Controlled-Size Hollow Magnesium Sulfide Nanocrystals Anchored on Graphene for Advanced Lithium Storage

Magnesium sulfide (MgS), representative of alkaline-earth metal chalcogenides (AEMCs), is a potential conversion/alloy-type electrode material for lithium ion batteries (LIBs), by virtue of its low potential, high theoretical capacity, and abundant magnesium resource. However, the limited capacity utilization and inferior rate performance still hinder its practical application, and the progress is rather slow due to the challenging fabrication technique for MgS. Herein, we report a series of controlled-size hollow MgS nanocrystals (NCs) homogeneously distributed on graphene (MgS@G), fabricated through a metal hydride framework (MHF) strategy, and its application as advanced electrode material for LIBs. The hollow structure of MgS NCs is mainly attributed to the Kirkendall effect and the escape of hydrogen atoms from metal hydride during sulfuration. The as-synthesized MgS@G demonstrates robust nanoarchitecture and admirable interactions, which ensure a spatially confined lithiation/delithiation process, optimize the dynamics of two-steps conversion/alloying reactions, and induce a synergetic pseudocapacitive storage contribution. As a result, a representative MgS@G composite delivers a largely enhanced capacity of >1208 mAh g-1 at a current density of 100 mA g-1 and a long-term cycle stability at a high current density of 5 A g-1 with a capacity of 838 mAh g-1 over 3000 cycles, indicating well-sustained structural integrity. This work presents an effective route toward the development of high-performance magnesium-based material for energy storage.