Interfacial Layers to Enable Recyclability of All-Solid-State Lithium Batteries

All-solid-state batteries provide opportunities for safe and robust energy storage solutions. An emerging issue is the final disposal of spent batteries due to the required production scale, limited lifetime, and lack of recycling methods. Here, we propose an architectural design for recyclable all-solid-state lithium batteries based on interfacial layers at the electrodes. Flexible lithium bis(fluorosulfonyl)imide doped polypropylene carbonate (PPC-LiFSI) interfacial layers improve physical contacts at Li metal and Li₇La₃Zr₂O₁₂ (LLZO)-based composite electrolytes interfaces and serve as sacrificial layers to enable clean separation and direct recycling. Recovered components demonstrate the preservation of electrochemical properties through direct reintegration into batteries. Fully recovered full cells with Li-metal and LTO anodes show 92.5% and 93.8% of original discharge capacity at 0.05 C and room temperature. We demonstrate an approach for the design of recyclable all-solid-state lithium batteries to fulfill long-term goals for sustainable energy storage devices.