Stable Lithium–Sulfur Batteries Ensured by GeS ₂ and α‐S ₈ Lattice Matching During the Charge Process

The charge process of lithium–sulfur batteries (LSBs) is a process in which molecular polarity decreases and the volume shrinks gradually, which is the process most likely to cause lithium polysulfides (LiPSs) loss and interfacial collapse. In this work, GeS ₂ is utilized, whose (111) lattice plane exactly matches with the (113) lattice of α‐S ₈ , to solve these problems. GeS ₂ can regulate the interconversion‐deposition behavior of S‐species during the charge process. Soluble LiPSs can be spontaneously adsorbed on the GeS ₂ surface, then obtain electrons and eventually convert to α‐S ₈ molecules. More importantly, the α‐S ₈ molecules will crystallize uniformly along the (111) lattice plane of GeS ₂ to maintain a stable cathode‐electrolyte interface. Therefore, outstanding charge/discharge LSBs are successfully accomplished.