Nickel–Iron Layered Double Hydroxide Hollow Polyhedrons as a Superior Sulfur Host for Lithium–Sulfur Batteries

We have designed and synthesized novel hollow Ni/Fe layered double hydroxide (LDH) polyhedrons as an advanced sulfur host for enhancing the performance of lithium–sulfur (Li–S) batteries. The Ni/Fe LDH host shows multiple advantages. First, the Ni/Fe LDH shells can provide sufficient sulfiphilic sites for chemically bonding with polysulfides. Second, the hollow architecture can provide sufficient inner space for both loading a large amount of sulfur and accommodating its large volumetric expansion. Moreover, once the active material is confined within the host, the shells could easily restrict the outward diffusion of polysulfides, guaranteeing prolonged cycle life even with high sulfur loading. As a result, the S@Ni/Fe LDH cathode has successfully solved the main issues related to sulfur electrodes, and it exhibits significantly improved electrochemical performances with prolonged life over 1000 cycles and excellent rate properties.