Sorting, characterisation, environmentally friendly recycling and re-use of components from End-of-Life 18650 Li ion batteries

The rapid growth in demand for lithium-ion batteries (LIBs) is leading to increasing challenges in: (i) the management of end-of-life (EoL) systems of electric vehicles (EVs) and industrial applications with huge variety in chemistry and design; (ii) the supply of critical raw materials (CRMs), especially Lithium, Cobalt and Nickel, whose ores are known to be conflict resources, and currently under the spotlight in the recycling field. The above-mentioned challenges can be addressed by collecting and recycling spent LIBs through economically and environmentally sustainable processes and enabling the transition to a circular economy vision based on the use of secondary raw materials. These processes involve not only the metallurgic approaches to recover the critical metals, but also the pre-treatment approaches in LIBs recycling that are crucial to enhance the recovery efficiency of other valuable materials (e.g., graphite, fluorinated compounds, binders, electrolyte), and to reduce the energy consumption in the subsequent metallurgic processes. Here, some pre-treatment processes, from the disassembling, opening, and sorting to the component separation, collection, and recovery, are described for the EoL 18650-type commercial Li-ion batteries (4400 mAh) harvested from a laptop module. Additionally, a closed loop of eco-friendly recycling to fully recover the composite cathode (both cathode active material, CAM, and binder) is presented. In the case of CAM, two different processes were explored: (i) soft-solvometallurgy via green solvents based on deep eutectic solvents (DESs); (ii) direct recycling. The recovered materials were used to prepare a new composite cathode that was assembled in a new cell using the recovered separator and characterized to evaluate the effective feasibility of the whole recycling process.