Stable Lithium–Sulfur Batteries Ensured by GeS2 and α‐S8 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, GeS2 is utilized, whose (111) lattice plane exactly matches with the (113) lattice of α‐S8, to solve these problems. GeS2 can regulate the interconversion‐deposition behavior of S‐species during the charge process. Soluble LiPSs can be spontaneously adsorbed on the GeS2 surface, then obtain electrons and eventually convert to α‐S8 molecules. More importantly, the α‐S8 molecules will crystallize uniformly along the (111) lattice plane of GeS2 to maintain a stable cathode‐electrolyte interface. Therefore, outstanding charge/discharge LSBs are successfully accomplished.