Atomic investigation on structural rearrangement of MoS2/graphene heterostructure upon electrochemical lithiation and delithiation

Abstract MoS2/graphene composite is a promising anode candidate with high rate capability and high capacity. In this work, first principles simulations are applied to study structural rearrangement of the MoS2/graphene heterointerface upon lithiation and delithiation. The atomic structures of MoS2/graphene after lithiation and delithiation processes indicates that the lithiated configuration cannot be restore to the original structure under delithiation. Both the length of Li–S bond and the distribution of Mo–Mo distance correspond to the permanent structural change of MoS2. The rearrangement in atomic configuration will influence the next lithiation process and result in irreversible lithium loss.