Perception of insight in the formation of solid electrolyte interphase

Abstract

While the solid electrolyte interphase (SEI) film in carbonate-based lithium-ion batteries (LIBs) has been extensively studied, less is known about the formation of SEI due to the complexity and instability of interfacial chemical reactions between Li+ and solvent. This study presents new insights into the formation mechanism of SEI film on graphite anode in ethylene carbonate (EC) and dimethyl carbonate (DMC) co-solvent-based electrolytes. The potential-resolved in-situ electrochemical impedance spectroscopy technology and density functional theory calculations combined with multi-sweep cyclic voltammetry are utilized to confirm that EC prefers to solvate with Li+. Then, a large amount of Li+-EC and a small amount of Li+-DMC solvent molecules undergo solvent migration process and de-solvation at the electrode/electrolyte interface. It was found that Li+-DMC is preferentially de-solvation and reduced to form an unstable SEI film, while Li+-EC inhibits the reduction of DMC and turns the reduction process to be diffusion-controlled. This work provides a fresh perspective on the formation of SEI film by Li+-solvent interaction, which could guide the construction of a stable interface by regulating the Li+-solvation kinetic for high-performance LIBs.