Current status and future directions of all-solid-state batteries with lithium metal anodes, sulfide electrolytes, and layered transition metal oxide cathodes

Highlights: • Progress and challenges of lithium metal anodes, sulfide electrolytes, and layered ternary oxide cathodes in solid-state batteries. • Origins of the failures in lithium metal anodes, Li-electrolyte interface, sulfide electrolytes, electrolyte-cathode interface, and layered metal oxide cathodes. • Summarize the state-of-the art diagnostic tools for investigating interfaces buried under the surface. • Future research directions for the solid-state battery architectures. All-solid-state batteries (ASSBs) offer great promise as a next-generation energy storage technology with higher energy density, wider operating temperature range, and improved safety for electric vehicles. ASSBs employing lithium metal anodes (Li), sulfide-based solid-state electrolytes (SSE), and Ni-rich layered transition metal oxide cathodes (LiMO₂, M = Ni, Mn, Co, Al) are particularly promising due to its superior electrochemical performance compared to other solid-electrolyte systems. However, the battery cycle life at high cathode mass loading and high current is still limited because the failure mechanism is not fully understood. Lithium dendrite growth at the anode or inside a solid electrolyte still represents as a serious risk of cell failure. Interfacial resistance increases attributed to electrolyte decomposition and interfacial void formation at both cathode−electrolyte and anode−electrolyte interfaces lead to gradual capacity fading. In this Review, we present the fundamental challenges and recent scientific understandings of each component in ASSBs. The novel diagnostic tools for these components, especially the interfaces buried under the surface that are often hard for characterization are mainly examined. Finally, we offer a perspective for future research directions. We hope this Review will provide a timely snapshot of state-of-the-art research progress in ASSBs to accelerate the development of ASSBs.