In the frame of global demand for electrical storage based on lithium-ion batteries (LIBs), their recycling with a focus on the circular economy is a critical topic. In terms of political incentives, the European legislative is currently under revision. Most industrial recycling processes target valuable battery components, such as nickel and cobalt, but do not focus on lithium recovery. Especially in the context of reduced cobalt shares in the battery cathodes, it is important to investigate environmentally friendly and economic and robust recycling processes to ensure lithium mobilization. In this study, the method early-stage lithium recovery (“ESLR”) is studied in detail. Its concept comprises the shifting of lithium recovery to the beginning of the chemo-metallurgical part of the recycling process chain in comparison to the state-of-the-art. In detail, full NCM (Lithium Nickel Manganese Cobalt Oxide)-based electric vehicle cells are thermally treated to recover heat-treated black mass. Then, the heat-treated black mass is subjected to an H2O-leaching step to examine the share of water-soluble lithium phases. This is compared to a carbonation treatment with supercritical CO2, where a higher extent of lithium from the heat-treated black mass can be transferred to an aqueous solution than just by H2O-leaching. Key influencing factors on the lithium yield are the filter cake purification, the lithium separation method, the solid/liquid ratio, the pyrolysis temperature and atmosphere, and the setup of autoclave carbonation, which can be performed in an H2O-environment or in a dry autoclave environment. The carbonation treatments in this study are reached by an autoclave reactor working with CO2 in a supercritical state. This enables selective leaching of lithium in H2O followed by a subsequent thermally induced precipitation as lithium carbonate. In this approach, treatment with supercritical CO2 in an autoclave reactor leads to lithium yields of up to 79%.

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