A Review on Regulating Li⁺ Solvation Structures in Carbonate Electrolytes for Lithium Metal Batteries

Lithium metal batteries (LMBs) are considered promising candidates for next-generation battery systems due to their high energy density. However, commercialized carbonate electrolytes cannot be used in LMBs due to their poor compatibility with lithium metal anodes. While increasing cut-off voltage is an effective way to boost the energy density of LMBs, conventional ethylene carbonate-based electrolytes undergo a number of side reactions at high voltages. It is therefore critical to upgrade conventional carbonate electrolytes, the performance of which is highly influenced by the solvation structure of lithium ions (Li⁺ ). This review provides a comprehensive overview of the strategies to regulate the solvation structure of Li⁺ in carbonate electrolytes for LMBs by better understanding the science behind the Li⁺ solvation structure and Li⁺ behavior. Different strategies are systematically compared to help select better electrolytes for specific applications. The remaining scientific and technical problems are pointed out, and directions for future research on carbonate electrolytes for LMBs are proposed.