Lithium-ion batteries (LIBs) have become a widespread technology for electrochemical energy storage in the current era of digitalization and transport electrification, being used as electric stationary storage as well as for powering electric vehicles, e-bikes and portable electronic devices such as smartphones and laptops. However, LIBs contain valuable materials, such as cobalt, nickel, lithium and graphite, whose supply has become critical to meet the increasing demand of batteries. Therefore, proper recycling processes are required in order to recover these materials from spent batteries and re-use them to produce new batteries in a sustainable cycle.
This contribution provides an extensive survey of the main recycling routes available today, focusing specifically on pyrometallurgical and hydrometallurgical processes based in Europe, North America and Asia. Attention is also devoted to the recycling behaviour of individuals and companies and to the possible ways to increase their recycling rate. The comparison of different processes allows for the ranking of best practices as well as the drawbacks of different process units, with identification of which materials can be recovered, their recovery rate, and an assessment of the overall recycling efficiency of the process for different battery sizes (small and large, for portable electronics and electric vehicles, respectively). The analysis reveals that pyrometallurgical processes can flexibly treat different LIB chemistries but, since the electrolyte and graphite are burnt in the process, the global recycling efficiency cannot compete with hydrometallurgical processes, especially for small format batteries. Nevertheless, hydrometallurgical processes typically require preliminary mechanical separation treatments to separate the black mass, which contains valuable electrodic materials, as well as complex precipitation steps, which eventually reduce the material recovery rate and the applicability to diverse LIB chemistries. Finally, the study reports an analysis of the electrochemical performance of a battery made with recycled materials, showing that even if recycled cathodic materials had a lower gravimetric capacity and solid-state diffusivity, the performance of a recycled battery could be compensated by simple minor changes to the cell design which would ultimately decrease the specific energy density by a few percent compared to a LIB made with virgin materials.