Electrostatic Interaction Tailored Anion-Rich Solvation Sheath Stabilizing High-Voltage Lithium Metal Batteries.

Through tailoring interfacial chemistry, electrolyte engineering is a facile yet effective strategy for high-performance lithium (Li) metal batteries, where the solvation structure is critical for interfacial chemistry. Herein, the effect of electrostatic interaction on regulating an anion-rich solvation is firstly proposed. The moderate electrostatic interaction between anion and solvent promotes anion to enter the solvation sheath, inducing stable solid electrolyte interphase with fast Li transport kinetics on the anode. This as-designed electrolyte exhibits excellent compatibility with Li metal anode (a Li deposition/stripping Coulombic efficiency of 99.3%) and high-voltage LiCoO cathode. Consequently, the 50 μm-thin Li||high-loading LiCoO cells achieve significantly improved cycling performance under stringent conditions of high voltage over 4.5 V, lean electrolyte, and wide temperature range (- 20 to 60 °C). This work inspires a groundbreaking strategy to manipulate the solvation structure through regulating the interactions of solvent and anion for high-performance Li metal batteries.