Graphene/C₂N lateral heterostructures as promising anode materials for lithium-ion batteries

Two-dimensional (2D) heterostructures have been proposed as potential anode materials for lithium-ion batteries due to their large surface areas and excellent electronic properties. In this study, we employ first-principles calculations to investigate the structural stability, electronic properties, and ion diffusion behaviors of 2D graphene/C2N lateral heterostructures. Three species of (5, 26), (11, 26), and (17, 26) heterostructures are chosen to explore the effects of graphene components on electronic properties. The results show that graphene/C2N lateral heterostructures exhibit good dynamic stability due to a small lattice mismatch and strong chemical interaction at the heterojunction interface. By introducing zero-gap graphene, these heterostructures acquire good electronic conductivity with small direct band gaps. The component ratio of graphene can significantly tune the band gap, showing a monotonic decrease as the ratio increases. Moreover, the introduction of C2N components can greatly improve the lithium capacities of heterostructures. Small diffusion energy barriers (0.257-0.273 eV) and a low average operating voltage of 0.758 V are observed in graphene/C2N heterostructures. The effects of graphene components and valence states on Li migration are discussed. Our results demonstrate that the graphene/C2N lateral heterostructure can effectively combine the advantages of graphene and the C2N monolayer, showing great promise as an anode material for lithium-ion batteries.