Graphite Recycling from Spent Lithium-Ion Batteries

• Published in: ChemSusChem 2016-12, Vol.9 (24), p.3473-3484
• Main Authors: Rothermel, Sergej, Evertz, Marco, Kasnatscheew, Johannes, Qi, Xin, Grützke, Martin, Winter, Martin, Nowak, Sascha
• Format: Article
• Language: English
• Subjects: Anodes; Carbon dioxide; Carbon Dioxide - chemistry; Electric Power Supplies; Electrochemistry; electrolyte extraction; Electrolytes; Extraction; Graphite; Graphite - chemistry; Heat treatment; Lithium; Lithium - chemistry; Lithium-ion batteries; lithium-ion battery; Rechargeable batteries; Recycling; Temperature
• ISSN: 1864-5631; 1864-564X
• DOI: 10.1002/cssc.201601062

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 CO2)‐assisted electrolyte extraction prior to thermal treatment. And the final investigated approach uses supercritical carbon dioxide (scCO2) 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 CO2. 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 LiNi1/3Co1/3Mn1/3O2 cathode. Old beats new: To address the growing need for utilization of spent lithium‐ion batteries, the feasibility of anode recycling in combination with three different electrolyte extraction concepts is investigated. It is demonstrated that the best performance of recycled graphite anodes can be achieved when electrolyte extraction is performed using subcritical carbon dioxide. In the best case, the electrochemical performance of recycled graphite exceeds the newly synthesized graphite anode benchmark.