For the resurgence and commercialization of lithium-metal batteries (LMBs), functional electrolytes play an important role in mitigating critical challenges, such as dendritic growth on the lithium (Li) anode, capacity degradation at the cathode, and the decomposition of the electrolyte. Modifying electrolyte additives promises a practical, accessible, and cost-competitive approach to fine control the critical electrode interface reactions including Li deposition and solid electrolyte interphase/cathode electrolyte interphase (SEI/CEI) formation. Here, we summarize the state-of-the-art electrolyte additives and their mechanism in inducing the Li deposition and SEI/CEI film formation. Based on our previous work, we prospectively propose rational designing strategies of electrolyte formula, i.e., compound electrolytes, via combining film-forming additives and leveling additives, to comprehensively and continuously tuning the film formation, film properties, and Li deposition layer throughout the long-term cycling. We hope the proposed design strategies could promote the advancement of electrolyte engineering in the commercialization of high-energy LMBs.



