Finally, the remaining issues and future opportunities of ASSLMBs for next-generation high-energy storages are prospected. The approaches based on nanostructured materials and nanotechnology advances of great promise to improve the overall performances of ASSLMBs are discussed in detail. The strategies to address the large interfacial impedances between SSE and Li metal anode attributed to low ionic conductivity and poor instability of SEI, and degraded physical contact are also overviewed. The fundamental understanding and characterizations on the lithium nucleation, dendrite growth, and formation of solid electrolyte interphase (SEI) during Li electrochemical deposition is discussed systematically. In this chapter, we first highlight the critical scientific challenges as well as technological progresses for the currently studied SSEs including organic polymers, inorganic electrolytes, and the composites. However, the problems including sluggish ion transport in SSEs and the interfacial incompatibility of SSEs with electrodes significantly limit the overall performances of ASSLMBs. In addition, SSEs could in principle suppress the lithium dendrite growth and enable the utilization of lithium metal anode that is regarded as a “holy grail” of lithium batteries, in all-solid-state lithium metal batteries (ASSLMBs). Replacing flammable organic liquid electrolytes by solid-state electrolytes (SSEs) provides a fundamental solution to safety issue for lithium-ion batteries (LIBs), driven by the increasing demand of high energy density, stable cycling performance, low cost, and abuse tolerance for energy storage systems in the widespread applications of electric vehicles (EVs) and smart grids.

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