Graphite Recycling from Spent Lithium‐Ion Batteries

Abstract The present work reports on challenges in utilization of spent lithium‐ion batteries (LIBs)—an increasingly important aspect associated with a significantly rising demand for electric vehicles (EVs). In this context, the feasibility of anode recycling in combination with three different electrolyte extraction concepts is investigated. The first method is based on a thermal treatment of graphite without electrolyte recovery. The second method additionally utilizes a subcritical carbon‐dioxide (subcritical CO 2 )‐assisted electrolyte extraction prior to thermal treatment. And the final investigated approach uses supercritical carbon dioxide (scCO 2 ) as extractant, subsequently followed by the thermal treatment. It is demonstrated that the best performance of recycled graphite anodes can be achieved when electrolyte extraction is performed using subcritical CO 2 . Comparative studies reveal that, in the best case, the electrochemical performance of recycled graphite exceeds the benchmark consisting of a newly synthesized graphite anode. As essential efforts towards electrolyte extraction and cathode recycling have been made in the past, the electrochemical behavior of recycled graphite, demonstrating the best performance, is investigated in combination with a recycled LiNi 1/3 Co 1/3 Mn 1/3 O 2 cathode.