Rechargeable lithium metal batteries (LMBs) are a highly promising technology for high-energy-density storage systems due to the low electrochemical potential and high theoretical capacity of the lithium metal anode. The electrolyte plays a pivotal role among the critical components of LMBs. However, traditional organic electrolytes pose significant safety risks and shorten the battery life due to their electrochemical instability, volatility, and flammability. Alternatively, ionic liquids (ILs), composed of anions and cations, are room-temperature molten salts characterized by ultra-low volatility, high ionic conductivity, excellent thermal stability, low flammability, and wide electrochemical windows. Based on these properties, liquid IL electrolytes (ILEs) and polymeric IL electrolytes (PILEs) have shown immense potential in enhancing battery cycle stability, energy density, lifespan, and safety. This review aims to comprehensively explore and summarize recent applications of ILEs and PILEs in LMBs, including their use as liquid and solid-state electrolytes, as well as ILs serving as film-forming additives, interfacial wetting agents, and pretreatment reagents. Additionally, the review delves into the solvation structures of Li⁺ ions within different IL-based electrolytes and the resulting interfacial chemical characteristics. Finally, based on literature reports and our previous work, we identify current challenges and propose solutions for the future application of IL-based electrolytes in LMBs.

中文翻译：

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离子液体基电解质中用于可充电锂金属电池的溶剂化和界面化学


由于锂金属负极的低电化学电位和高理论容量，可充电锂金属电池 （LMB） 是一种非常有前途的高能量密度存储系统技术。电解质在 LMB 的关键成分中起着举足轻重的作用。然而，传统的有机电解质由于其电化学不稳定性、挥发性和易燃性，存在重大的安全风险并缩短电池寿命。或者，由阴离子和阳离子组成的离子液体 （IL） 是室温熔盐，其特点是超低挥发性、高离子电导率、优异的热稳定性、低可燃性和宽电化学窗口。基于这些特性，液态 IL 电解质 （ILE） 和聚合物 IL 电解质 （PILE） 在提高电池循环稳定性、能量密度、寿命和安全性方面显示出巨大的潜力。本文旨在全面探讨和总结 ILEs 和 PILEs 在 LMB 中的最新应用，包括它们作为液体和固态电解质的使用，以及 ILs 作为成膜添加剂、界面润湿剂和预处理试剂。此外，该综述深入研究了 Li⁺ 离子在不同 IL 基电解质中的溶剂化结构以及由此产生的界面化学特性。最后，根据文献报道和我们以前的工作，我们确定了当前的挑战并为 IL 基电解质在 LMB 中的未来应用提出了解决方案。