Abstract Owing to the use of solid electrolytes instead of flammable and potentially toxic organic liquid electrolytes, all solid-state lithium batteries (ASSLBs) are considered to have substantial advantages over conventional liquid electrolyte based lithium ion batteries(LIBs) in terms of safety, energy density, battery packaging, and operable temperature range. However, the electrochemistry and the operation mechanism of ASSLBs differ considerably from conventional LIBs. Consequently, the failure mechanisms of ASSLBs, which are not well understood, require particular attention. To improve the performance and realize practical applications of ASSLBs, it is crucial to unravel the dynamic evolution of electrodes, solid electrolytes, and their interfaces and interphases during cycling of ASSLBs. In situ transmission electron microscopy (TEM) provides a powerful approach for the fundamental investigation of structural and chemical changes during operation of ASSLBs with high spatio-temporal resolution. Herein, recent progress in in situ TEM studies of ASSLBs are reviewed with a specific focus on real-time observations of reaction and degradation occurring in electrodes, solid electrolytes, and their interfaces. Novel electro-chemo-mechanical coupling phenomena are revealed and mechanistic insights are highlighted. This review covers a broad range of electrode and electrolyte materials applied in ASSLBs, demonstrates the general applicability of in situ TEM for elucidating the fundamental mechanisms and providing the design guidance for the development of high-performance ASSLBs. Finally, challenges and opportunities for in situ TEM studies of ASSLBs are discussed.

中文翻译：

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通过原位透射电子显微镜了解所有固态锂电池

摘要 由于使用固体电解质代替易燃且具有潜在毒性的有机液体电解质，全固态锂电池（ASSLBs）被认为在安全、能量和能量方面优于传统的液体电解质基锂离子电池（LIBs）。密度、电池封装和工作温度范围。然而，ASSLBs 的电化学和运行机制与传统的 LIBs 有很大不同。因此，ASSLB 的故障机制尚不清楚，需要特别注意。为了提高 ASSLBs 的性能并实现其实际应用，解开 ASSLBs 循环过程中电极、固体电解质及其界面和界面的动态演变至关重要。原位透射电子显微镜 (TEM) 为在具有高时空分辨率的 ASSLB 操作过程中进行结构和化学变化的基础研究提供了一种强有力的方法。在此，综述了 ASSLB 原位 TEM 研究的最新进展，特别关注电极、固体电解质及其界面中发生的反应和降解的实时观察。揭示了新的电化学机械耦合现象，并突出了机械见解。这篇综述涵盖了广泛应用于 ASSLB 的电极和电解质材料，展示了原位 TEM 的普遍适用性，用于阐明基本机制并为高性能 ASSLB 的开发提供设计指导。最后，