Molecular Dynamics Simulation of Solvation NanoStructure in Carbonate-Based Electrolyte of Lithium–Sulfur Battery

Lithium–sulfur (Li–S) batteries are widely regarded as the most promising batteries for the future due to their higher specific capacity and lower prices. Various strategies are utilized to alleviate the shortcomings of Li–S batteries failing to reach theoretical capacity. However, basic research at the molecular level continues to be lacking. Therefore, we use molecular dynamics to study the details of the solvated structure of Li–S batteries electrolyte and the nature of the transport process, revealing the relationship between the solvated structure of the electrolyte of LiPF6 and the organic solvent ethylene carbonate/dimethyl carbonate (EC/DMC). The electrolyte of Li2S4 was first simulated in a pure solvent environment. Then the LiPF6 salt was added to the model to simulate a typical electrolyte for a working Li–S battery. Regarding the rationality of the solvent system, various reference systems such as density, dielectric constant, viscosity and diffusion coefficient of the solvent were used for verification. And the detailed composition of the first solvation shell of the polysulfate ion and the coordination number of the ions are discussed. These results provide new insights into the use of EC/DMC electrolytes in Li–S batteries, while at the same time providing a basis for efficient future predictions of electrolyte structure and transport in complex electrode confinements.