The electrode/electrolyte interface plays a critical role in stabilizing the cycling performance and prolonging the service life of rechargeable batteries to meet the sustainable energy requirements of the mobile society. The understanding of interfaces is still at the preliminary stage due to the limited research techniques and variable properties with time and potential. Herein, the latest developments focused on the interfaces in rechargeable systems including the cathode electrolyte interphase (CEI) and solid electrolyte interphase (SEI) are reviewed. The possible formation mechanisms of the electrode/electrolyte interface are discussed, followed by the introduction of two key influencing factors, specific adsorption and solvated coordinate structure, which will dominate the formation of the interface. Finally, the structure and chemical composition of the interface as well as the possible transport mechanism of lithium ions in the interface and the strategies to regulate the pathway through the interface are presented in detail. This work sheds light on the fundamental understanding of the interface and provides rational scientific principles in designing the electrode/electrolyte interface and inspires the rational design of long‐term cycling rechargeable batteries.

中文翻译：

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走向可充电电池中的关键电极/电解质界面

电极/电解质界面在稳定循环性能和延长可充电电池的使用寿命以满足移动社会对可持续能源的需求方面起着至关重要的作用。由于有限的研究技术以及随时间和潜力的可变属性，对界面的理解仍处于初步阶段。在此，回顾了集中在可再充电系统中的接口的最新发展，包括阴极电解质中间相（CEI）和固体电解质中间相（SEI）。讨论了电极/电解质界面的可能形成机理，然后介绍了两个关键的影响因素，特定的吸附和溶剂化的配位结构，它们将主导界面的形成。最后，详细介绍了界面的结构和化学成分，以及界面中锂离子的可能迁移机理，以及调节通过界面的途径的策略。这项工作阐明了对界面的基本理解，并为设计电极/电解质界面提供了合理的科学原理，并激发了长期循环充电电池的合理设计。