Benign Recycling of Spent Batteries towards All‐Solid‐State Lithium Batteries

Lithium-ion batteries (LIBs) are one of the most significant energy storage devices applied in power supply facilities. However, a huge number of spent LIBs would bring harmful resource waste and environmental hazards. In this study, a benign hydrometallurgical method using phytic acid as precipitant is proposed to recover useful metallic Mn ions from spent LiMn2 O4 batteries. Besides Mn-based cathodes, this recovery process is also applicable for other commercial batteries. More importantly, for the first time, the as-obtained manganous complex is employed as a nanofiller in a polyethylene oxide matrix to largely improve Li+ conductivity and transference number. As a result, when applied in all-solid-state lithium batteries, high capacity and outstanding cyclic stability are achieved with capacity retention of 86.4 % after 60 cycles at 0.1 C. The recovery of spent lithium batteries not only has benefits for the environment and resources, but also shows great potential application in all-solid-state lithium batteries, which opens up a costless and efficient circulation pathway for clean and reliable energy storage systems.