Recycling Hazardous and Valuable Electrolyte in Spent Lithium-Ion Batteries: Urgency, Progress, Challenge, and Viable Approach

Recycling spent lithium-ion batteries (LIBs) is becoming a hot global issue due to the huge amount of scrap, hazardous, and valuable materials associated with end-of-life LIBs. The electrolyte, accounting for 10-15 wt % of spent LIBs, is the most hazardous substance involved in recycling spent LIBs. Meanwhile, the valuable components, especially Li-based salts, make recycling economically beneficial. However, studies of electrolyte recycling still account for only a small fraction of the number of spent LIB recycling papers. On the other hand, many more studies about electrolyte recycling have been published in Chinese but are not well-known worldwide due to the limitations of language. To build a bridge between Chinese and Western academic achievements on electrolyte treatments, this Review first illustrates the urgency and importance of electrolyte recycling and analyzes the reason for its neglect. Then, we introduce the principles and processes of the electrolyte collection methods including mechanical processing, distillation and freezing, solvent extraction, and supercritical carbon dioxide. We also discuss electrolyte separation and regeneration with an emphasis on methods for recovering lithium salts. We discuss the advantages, disadvantages, and challenges of recycling processes. Moreover, we propose five viable approaches for industrialized applications to efficiently recycle electrolytes that combine different processing steps, ranging from mechanical processing with heat distillation to mechanochemistry and in situ catalysis, and to discharging and supercritical carbon dioxide extraction. We conclude with a discussion of future directions for electrolyte recycling. This Review will contribute to electrolyte recycling more efficiently, environmentally friendly, and economically.