The global market of lithium-ion batteries (LIB) has been growing in recent years, mainly owed to electromobility. The global LIB market is forecasted to amount to $129.3 billion in 2027. Considering the global reserves needed to produce these batteries and their limited lifetime, efficient recycling processes for secondary sources are mandatory. A selective process for Li recycling from LIB black mass is described. Depending on the process parameters Li was recovered almost quantitatively by the COOL-Process making use of the selective leaching properties of supercritical CO2/water. Optimization of this direct carbonization process was carried out by a design of experiments (DOE) using a 33 Box-Behnken design. Optimal reaction conditions were 230 °C, 4 h, and a water:black mass ratio of 90 mL/g, yielding 98.6 ± 0.19 wt.% Li. Almost quantitative yield (99.05 ± 0.64 wt.%), yet at the expense of higher energy consumption, was obtained with 230 °C, 4 h, and a water:black mass ratio of 120 mL/g. Mainly Li and Al were mobilized, which allows for selectively precipitating Li2CO3 in battery grade-quality (>99.8 wt.%) without the need for further refining. Valuable metals, such as Co, Cu, Fe, Ni, and Mn, remained in the solid residue (97.7 wt.%), from where they are recovered by established processes. Housing materials were separated mechanically, thus recycling LIB without residues. This holistic zero waste-approach allows for recovering the critical raw material Li from both primary and secondary sources.
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