Atomic Insights of Structural, Electronic Properties of B, N, P, S, Si-doped Fullerenes and Lithium Ion Migration with DFT-D Method

Context: Battery interface research can effectively guide battery design and material selection to improve battery performance. However, current electrode material interface studies still have significant limitations. In this paper, by employing DFT-D method, the influences of doping elements (boron, nitrogen, phosphorus, sulfur, and silicon) on the properties of C fullerene, such as structural stability, electronic properties, and the adsorption and migration of lithium ion, are comprehensively investigated. It is demonstrated that doping can bolster the fullerene molecule's structural integrity and enhance charge transfer comparing with C, thereby augmenting the material's electrical conductivity. Among the five doping elements, B-doping exhibits the most favorable adsorption energies, indicating a strong lithium binding affinity. This observation is supported with energy barrier of lithium ion migration. B-doping leads to an elevated barrier (0.37 eV) comparing with pristine C (0.19 eV), whereas Si-doping significantly reduced barrier (0.038 eV) indicates enhanced lithium-ion mobility. These findings solid the efficacy of doping as a strategy to enhance the performance of fullerene electrodes.

Method: All DFT calculations were performed using the VASP software package. The chosen computational technique was a combination of the generalized approximate gradient function PBE with the dispersion correction (DFT-D3) developed by Grimme. The results of the calculations were analyzed with the help of VASPKIT.