High-Safety and Dendrite-Free Lithium Metal Batteries Enabled by Building a Stable Interface in a Nonflammable Medium-Concentration Phosphate Electrolyte

Lithium metal anodes are promising for their high energy density and low working potential. However, high reactivity and dendrite growth of lithium metal lead to serious safety issues. Lithium dendrite may form "dead lithium" or pierce the separator, which will cause low efficiency and short-circuit inside the battery. A nonflammable phosphate-based electrolyte can effectively solve the flammability problem. Also, it shows poor compatibility with lithium metal anodes, resulting in an unstable solid electrolyte interface (SEI), which leads to dendrite growth and poor electrochemical performance. In this study, trimethyl phosphate is used to ensure the safety of lithium metal batteries. By adjusting the concentration of lithium salt and introducing fluoroethylene carbonate, a stable SEI layer is formed on the surface of the lithium metal anode and dendrite growth of the lithium metal anode is inhibited. Lithium metal batteries with a modified electrolyte achieved stable electrochemical plating/stripping, and the full cell has 93.4% capacity left and the coulombic efficiency is nearly 100%. In addition, the modified electrolyte can also enable reversible intercalation and de-intercalation of Li⁺ in the commercial graphite anode. This work may provide an alternative direction for the development of lithium metal batteries with high safety and high energy density.