Facile synthesis and first-principles study of nitrogen and sulfur dual-doped porous graphene aerogels/natural graphite as anode materials for Li-ion batteries

•A simple and scalable method was used to prepare nitrogen-sulfur co-doped graphene aerogels.•The adsorption and electronic properties of the N/S co-doping system were systematically studied.•Theoretical and experimental methods were used to verify the effect of doping graphene on the original anode materials. In order to prepare anode materials with a high specific capacity, super rate performance and relatively good stability, the N, S dual-doped porous graphene aerogels/natural graphite composites (denoted as N, S-pGA/NG) were designed via annealing incorporation with hydrothermal method in this paper. Commercial graphite anode materials were modified by adding a small amount of N/S dual-doped Porous graphene aerogels to make them have excellent electrochemical properties. At the same time, in order to further explain the internal mechanism of nitrogen and sulfur atoms doped graphene to improve the properties of natural graphite anode electrodes, we used density functional theory to calculate the adsorption energy, static charge and density of states, which proved that the this optimization’s mechanism may lie in the effect of nitrogen and sulfur co-doping on the adsorption behavior of lithium atoms. Therefore, the N, S-pGA/NG exhibited high capacities (531 mAh g−1 at 0.1 C), improved rate performance (277 mAh g−1 at 2 C), and good cycling stability.