Abstract

Selective extraction of lithium from spent lithium-ion batteries (LIBs) represents a promising solution for efficient lithium recovery. Herein, a water-aerosol-assisted roasting technology is proposed to selectively extract lithium from spent lithium transition metal oxides (LTMOs) cathodes. In an exemplary recycling of spent LiCoO2, the cathode material undergoes a low-temperature (350°C) chlorinating roast process to convert it into metal chlorides, followed by a higher-temperature (500°C) roasting to facilitate the selective pyrolysis of CoCl2. The presence of water-aerosol significantly enhances the selective pyrolysis process of CoCl2, reducing roasting time eightfold compared to conventional air roasting. Subsequent water-leaching effectively extracts 99.1 % of lithium as LiCl, while only 0.2 % of cobalt is extracted, ensuring selective lithium recovery. The resulting high-purity LiCl solution and Co3O4 residue are directly utilizable for producing battery-grade Li2CO3 and LiCoO2, respectively. Regenerated LiCoO2 demonstrates excellent cycling stability, retaining 90.5 % of its capacity after 300 cycles at 1C rate. Moreover, this method is applicable to ternary cathodes (NCM) black mass, offering a sustainable, robust, and cost-effective approach for lithium extraction from spent LIBs.

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