A review of direct recycling methods for spent lithium-ion batteries

The increasing demand for lithium-ion batteries (LIBs) in new energy storage systems and electric vehicles implies a surge in both the shipment and scrapping of LIBs. LIBs contain a lot of harmful substances, and improper disposal can cause severe environment damage. Developing efficient recycling technology has become the key to the sustainable growth of the LIBs industry. At present, the extraction of high-value materials from spent LIBs using pyrometallurgical and hydrometallurgical processes is most usual. However, they consume a lot of energy and lead to secondary environmental pollution, which is not consistent with the the idea of creating a green circular economy. Direct recycling has been suggested as a possible alternative method of dealing with the spent LIBs under non-destructive conditions in the further. Compared with traditional metallurgical technologies, direct regeneration significantly reduces the consumption of energy and chemical reagents, and has a high selectivity for certain metal ions, which is environmentally friendly. However, direct cycling is still in its infancy with many scientific and technological barriers. In this review, we first consider the necessity of recycling spent LIBs, and then summarize the failure mechanisms of degraded cathode materials in order to choose a corresponding regeneration method. The direct cycling technologies, including hydrothermal, solid-state, eutectic medium and electrochemical regeneration are introduced separately from the perspective of the experimental process, operating parameters, regeneration principles, advantages, and effects. Furthermore, the current problems and potential future research on the direct cycling of spent LIBs are also discussed.