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<p>This study proposes a sustainable and selective hydrometallurgical route for the recovery of lithium (Li) and cobalt (Co) from spent lithium-ion batteries (LIBs), integrating sodium sulfite-assisted sulfation roasting with water and organic acid leaching. The sulfation roasting process at 600&#xa0;°C facilitated the transformation of LiCoO<sub>2</sub> into soluble LiNaSO<sub>4</sub> while preserving cobalt predominantly in oxide form. Subsequent water leaching at 50&#xa0;°C selectively dissolved lithium (up to 74.4%), leaving cobalt in the residue. To achieve complete metal recovery, oxalic acid—a biodegradable and environmentally benign organic acid—was used as a leaching agent. Under optimized conditions (1&#xa0;mol·L<sup>− 1</sup> oxalic acid, 90&#xa0;°C, 90&#xa0;min, S/L ratio 1/160), leaching efficiencies reached 99.96% for Li and 99.15% for Co. Notably, cobalt was recovered directly as a cobalt oxalate precipitate, while lithium remained in solution, eliminating the need for additional separation steps. In the water-leaching stage, lithium selectively dissolves while cobalt largely remains in oxide form. In the separate oxalic-acid leaching stage, both metals dissolve; however, cobalt immediately precipitates as cobalt oxalate whereas lithium remains soluble. Thus, although the two leaching approaches are independent processes, each exhibits a distinct Li/Co separation behavior. Kinetic modeling revealed that nucleation and growth mechanisms, best described by the Avrami equation, governed the leaching behavior. This combined pyro-hydrometallurgical process offers a high-efficiency, low-impact solution for critical metal recovery from LIB waste and represents a viable alternative to conventional mineral acid-based methods.</p>

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Environmentally Friendly Separation of Lithium and Cobalt from Spent Li-ion Batteries Using Water and Organic Acid Leaching

  • 期刊论文

  • 出版模式：

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  • 发表日期：

    2026年2月12日

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  • Figen Algul,
  • Ahmet Alp

摘要

This study proposes a sustainable and selective hydrometallurgical route for the recovery of lithium (Li) and cobalt (Co) from spent lithium-ion batteries (LIBs), integrating sodium sulfite-assisted sulfation roasting with water and organic acid leaching. The sulfation roasting process at 600 °C facilitated the transformation of LiCoO2 into soluble LiNaSO4 while preserving cobalt predominantly in oxide form. Subsequent water leaching at 50 °C selectively dissolved lithium (up to 74.4%), leaving cobalt in the residue. To achieve complete metal recovery, oxalic acid—a biodegradable and environmentally benign organic acid—was used as a leaching agent. Under optimized conditions (1 mol·L− 1 oxalic acid, 90 °C, 90 min, S/L ratio 1/160), leaching efficiencies reached 99.96% for Li and 99.15% for Co. Notably, cobalt was recovered directly as a cobalt oxalate precipitate, while lithium remained in solution, eliminating the need for additional separation steps. In the water-leaching stage, lithium selectively dissolves while cobalt largely remains in oxide form. In the separate oxalic-acid leaching stage, both metals dissolve; however, cobalt immediately precipitates as cobalt oxalate whereas lithium remains soluble. Thus, although the two leaching approaches are independent processes, each exhibits a distinct Li/Co separation behavior. Kinetic modeling revealed that nucleation and growth mechanisms, best described by the Avrami equation, governed the leaching behavior. This combined pyro-hydrometallurgical process offers a high-efficiency, low-impact solution for critical metal recovery from LIB waste and represents a viable alternative to conventional mineral acid-based methods.