▎ 摘　　要

Properties of ZnS/graphene, such as formation energy of the Li adatom, activation energy for Li diffusion, pseudocapacity-like storage, and density of state (DOS), render ZnS/graphene a suitable anode material for a rechargeable lithium-ion battery. Lithium storage sites, migration paths, electronic conductivity, and storage sequence of lithium ions are clarified. Lithium ions preferentially embed the ZnS/graphene heterostructure interface and the surface of ZnS and then intercalate into the bulk phase of ZnS. In the ZnS bulk, Li ions diffuse by the T-O-T path, and the activation energy diseases with volume expanded. LiS4 and ZnS2 are produced with ZnS lithiation, besides LixZn and Li2S. Moreover, it is proven that the capacity of ZnS/graphene more than the sum of ZnS and graphene originates from the interfacial lithium storage via the pseudocapacity-like storage mechanism. Therefore, further increasing the contact area between ZnS and graphene could promote the capacity by reducing the ZnS particle size.