High-energy and stable lithium-ion batteries are desired for next-generation electric devices and vehicles. To achieve their development, the formation of stable interfaces on high-capacity anodes and high-voltage cathodes is crucial. However, such interphases in certain commercialized Li-ion batteries are not stable. Due to internal stresses during operation, cracks are formed in the interphase and electrodes; the presence of such cracks allows for the formation of Li dendrites and new interphases, resulting in a decay of the energy capacity. In this Review, we highlight electrolyte design strategies to form LiF-rich interphases in different battery systems. In aqueous electrolytes, the hydrophobic LiF can extend the electrochemical stability window of aqueous electrolytes. In organic liquid electrolytes, the highly lithiophobic LiF can suppress Li dendrite formation and growth. Electrolyte design aimed at forming LiF-rich interphases has substantially advanced high-energy aqueous and non-aqueous Li-ion batteries. The electrolyte and interphase design principles discussed here are also applicable to solid-state batteries, as a strategy to achieve long cycle life under low stack pressure, as well as to construct other metal batteries.

下一代电动设备和车辆需要高能且稳定的锂离子电池。为了实现它们的发展，在高容量阳极和高电压阴极上形成稳定的界面至关重要。然而，某些商业化锂离子电池中的这种界面并不稳定。由于运行中的内应力，相间和电极产生裂纹；这种裂纹的存在会导致锂枝晶和新的界面的形成，从而导致能量容量的衰减。在这篇综述中，我们重点介绍了在不同电池系统中形成富含 LiF 的界面的电解质设计策略。在水性电解质中，疏水性LiF可以扩展水性电解质的电化学稳定性窗口。在有机液体电解质中，高度疏锂的LiF可以抑制锂枝晶的形成和生长。旨在形成富含 LiF 的界面的电解质设计极大地推进了高能水系和非水系锂离子电池的发展。这里讨论的电解质和相间设计原理也适用于固态电池，作为在低堆压力下实现长循环寿命的策略，以及构建其他金属电池。