Recycling and Reuse of Mn-Based Spinel Electrode from Spent Lithium-Ion Batteries

Abstract

In this paper, we introduce an environmentally friendly approach to recycle used batteries and recover highly valuable manganese-based cathode materials. This study demonstrates the feasibility of fast plasma pyrolysis to recover LiMn2O4 electrode materials (e.g., lithium manganese oxide, LMO) and demonstrate their reuse in newly assembled Li-ion cells. The electrochemical performance of as-recycled cathodes shows an initial discharge capacity of 72 mAh/g and is stable for 100 cycles at 0.1 C. After adding 20 mole % of excess LiOH, the recycled LMO after relithiation at 660 °C can deliver an initial discharge capacity of 96 mAh/g and retain a decent discharge capacity of 88 mAh/g after 50 cycles at a 0.2 C rate. Without relithiation, the as-recycled LMO cathode after heating at 1000 °C delivers the best electrochemical cycling performance, including an initial discharge capacity of 94 mAh/g and 50th cycle capacity of 91 mAh/g at a 0.2 C rate. This study highlights a feasible approach for recycling electrode materials in spent LIBs. Recycling of lithium-ion batteries and especially electrode materials is crucial for the sustained growth of the lithium-ion battery industry and reduced environmental issues.