The amount of spent lithium-ion batteries has grown dramatically in recent years, and the development of a recycling process for spent lithium-ion batteries is necessary and urgent from the viewpoints of environmental protection and resource savings. The hydrometallurgical process is considered to be the most suitable method for the recycling of spent lithium-ion batteries. The current status of hydrometallurgical recycling technologies of spent lithium-ion batteries is reviewed in this paper. A series of hydrometallurgical procedures including pretreatment of the spent lithium-ion batteries, leaching process and separation of valuable metals from leaching solution are introduced in detail, and their advantages and problems are analyzed. Finally, the prospects and direction of the recycling of spent lithium-ion batteries are put forward. It is pointed out that a more flexible and universal process is required for the recovery of different types of spent lithium-ion batteries. Besides cathode active materials, the other components of spent lithium-ion batteries including electrolyte and anode materials also need to be recovered due to their potential environmental hazards.

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It is a challenge to recover lithium from the leaching solution of spent lithium-ion batteries, and crown ethers are potential extractants due to their selectivity to alkali metal ions. The theoretical calculations for the selectivity of crown ethers with different structures to Li ions in aqueous solutions were carried out based on the density functional theory. The calculated results of geometries, binding energies, and thermodynamic parameters show that 15C5 has the strongest selectivity to Li ions in the three crown ethers of 12C4, 15C5, and 18C6. B15C5 has a smaller binding energy but more negative free energy than 15C5 when combined with Li + , leading to that the lithium ions in aqueous solutions will combine with B15C5 rather than 15C5. The exchange reactions between B15C5 and hydrated Li + , Co 2+ , and Ni 2+ were analyzed and the results show that B15C5 is more likely to capture Li + from the hydrated ions in an aqueous solution containing Li + , Co 2+ , and Ni 2+. This study indicates that it is feasible to extract Li ions selectively using B15C5 as an extractant from the leaching solution of spent lithium-ion batteries.

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