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<p>The massive use of lithium-ion batteries has made their recycling a significant challenge in the new era. In this study, we propose an environmentally friendly electrochemical method for the direct recovery of degraded LiCoO<sub>2</sub> (LCO) cathode materials from spent lithium-ion batteries (LIBs), utilizing deep eutectic solvent-based electrolyte. Spent lithium-ion batteries are first pretreated by discharge, manual disassembly, and calcination to obtain degraded LCO. Electrochemical relithiation is then performed by applying a constant current density to the deep eutectic solvent-based electrolyte, which induces the insertion of Li<sup>+</sup> into the defect sites of the degraded LCO. After annealing at 700&#xa0;°C for 2&#xa0;h, surface impurities are removed, the crystal structure is restored, and regenerated LCO is obtained. Integrated characterization techniques such as ICP, XRD, SEM, XPS and cycling test confirmed the recovery of the Li/Co molar ratio (from 0.61:1 to 0.90:1), the recovery of lattice parameters (c-lattice constant from 14.185 Å to 14.081 Å), and the increase of battery capacity (from 130.3 mAh/g to 140.0 mAh/g). This electrochemical method provides a low-energy, short-process, and high-efficiency alternative to traditional indirect recycling technologies (physical separation, pyrometallurgy, and hydrometallurgy), offering not only a solution to resource sustainability but also a more environmentally friendly strategy for lithium battery recycling technology.</p>

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Direct recycling of LiCoO2 materials from lithium battery cathodes using electrochemical methods with deep eutectic solvent

  • 期刊论文

  • 发表日期：

    2025年11月19日

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  • Tianqi Jin,
  • Yechen Zhou,
  • Yejiao Xu,
  • Luanxia Chen,
  • Zhen Zhang,
  • Kaiyuan Peng

摘要

The massive use of lithium-ion batteries has made their recycling a significant challenge in the new era. In this study, we propose an environmentally friendly electrochemical method for the direct recovery of degraded LiCoO2 (LCO) cathode materials from spent lithium-ion batteries (LIBs), utilizing deep eutectic solvent-based electrolyte. Spent lithium-ion batteries are first pretreated by discharge, manual disassembly, and calcination to obtain degraded LCO. Electrochemical relithiation is then performed by applying a constant current density to the deep eutectic solvent-based electrolyte, which induces the insertion of Li+ into the defect sites of the degraded LCO. After annealing at 700 °C for 2 h, surface impurities are removed, the crystal structure is restored, and regenerated LCO is obtained. Integrated characterization techniques such as ICP, XRD, SEM, XPS and cycling test confirmed the recovery of the Li/Co molar ratio (from 0.61:1 to 0.90:1), the recovery of lattice parameters (c-lattice constant from 14.185 Å to 14.081 Å), and the increase of battery capacity (from 130.3 mAh/g to 140.0 mAh/g). This electrochemical method provides a low-energy, short-process, and high-efficiency alternative to traditional indirect recycling technologies (physical separation, pyrometallurgy, and hydrometallurgy), offering not only a solution to resource sustainability but also a more environmentally friendly strategy for lithium battery recycling technology.