A Competitive Solvation of Ternary Eutectic Electrolytes Tailoring the Electrode/Electrolyte Interphase for Lithium...

The development of electrolytes with high safety, high ionic conductivity, and the ability to inhibit lithium dendrites growth is crucial for the fabrication of high-energy-density lithium metal batteries. In this study, a ternary eutectic electrolyte is designed with LiTFSI (TFSI = bis(trifluoromethanesulfonyl)imide), butyrolactam (BL), and succinonitrile (SN). This electrolyte exhibits a high ion conductivity, nonflammability, and a wide electrochemical window. The competitive solvation effect among SN, BL, and Li⁺ reduces the viscosity and improves the stability of the eutectic electrolyte. The preferential coordination of BL toward Li⁺ facilitates the formation of stable solid electrolyte interphase films, leading to homogeneous and dendrite-free Li plating. As expected, the LiFePO₄/Li cell with this ternary eutectic electrolyte delivers a high capacity retention of 90% after 500 cycles at 2 C and an average Coulombic efficiency of 99.8%. Moreover, Ni-rich LiNi_0.8Co_0.1Al_0.1O₂/Li and LiNi_0.8Co_0.1Mn_0.1O₂/Li cells based on the modified ternary eutectic electrolyte achieve an outstanding cycling performance. This study provides insights for understanding and designing better electrolytes for lithium metal batteries and analogous sodium/potassium metal batteries.