<p>The widespread deployment of lithium-ion batteries has precipitated critical challenges in resource recovery and environmental management due to the escalating volume of battery waste. This study introduces a novel deep eutectic solvent system, utilizing a choline chloride–malonic acid (1:1) formulation, for the effective extraction of valuable metals from spent LiNi<sub>x</sub>Co<sub>y</sub>Mn<sub>z</sub>O<sub>2</sub> batteries. We conducted a comprehensive analysis of the leaching kinetics under pressurized conditions. Our findings reveal that under optimal conditions—specifically, a temperature of 120&#xa0;°C, a duration of 6&#xa0;h, and a liquid–solid ratio of 20:1—the leaching efficiencies for Li, Co, Ni, and Mn surpass 95%, nearing total extraction. The leaching kinetics for Co, Li, Mn, and Ni adhere to the “shrinking unreacted core model,” predominantly governed by mixing dynamics. The application of pressure expedites the disintegration of the cathode material’s crystal structure, thereby accelerating the liberation of metal ions. Additionally, pressurized leaching amplifies the coordination capacity of chloride ions and malonate ions (C<sub>3</sub>H<sub>2</sub>O<sub>4</sub><sup>2</sup>⁻) within the system, fostering the formation of more stable complexes with transition metal ions and propelling the dissolution equilibrium toward completion. Moreover, the pressurized environment induces lattice expansion in NCM materials, reducing the energy barriers for the migration of Li⁺ and transition metal ions, thus facilitating their release from the lattice and enhancing the reaction kinetics. In comparison to conventional atmospheric pressure hydrometallurgical methods, the pressurized leaching process markedly reduces leaching time, lowers the requisite reaction temperature, and mitigates secondary pollution, presenting a more sustainable and efficient approach to battery recycling.</p> Graphical Abstract <p></p>

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Recovery of Li, Ni, Co, and Mn from Cathode Mass of Spent Lithium-Ion Batteries by Deep Eutectic Solvent-Based Pressurized Leaching

  • Yunjie Bao,
  • Dianchun Ju,
  • Leyan Jiang,
  • Ruihan Liu,
  • Xuefeng Yin,
  • Jiayong Qiu,
  • Weitong Du,
  • Zhuo Chen

摘要

The widespread deployment of lithium-ion batteries has precipitated critical challenges in resource recovery and environmental management due to the escalating volume of battery waste. This study introduces a novel deep eutectic solvent system, utilizing a choline chloride–malonic acid (1:1) formulation, for the effective extraction of valuable metals from spent LiNixCoyMnzO2 batteries. We conducted a comprehensive analysis of the leaching kinetics under pressurized conditions. Our findings reveal that under optimal conditions—specifically, a temperature of 120 °C, a duration of 6 h, and a liquid–solid ratio of 20:1—the leaching efficiencies for Li, Co, Ni, and Mn surpass 95%, nearing total extraction. The leaching kinetics for Co, Li, Mn, and Ni adhere to the “shrinking unreacted core model,” predominantly governed by mixing dynamics. The application of pressure expedites the disintegration of the cathode material’s crystal structure, thereby accelerating the liberation of metal ions. Additionally, pressurized leaching amplifies the coordination capacity of chloride ions and malonate ions (C3H2O42⁻) within the system, fostering the formation of more stable complexes with transition metal ions and propelling the dissolution equilibrium toward completion. Moreover, the pressurized environment induces lattice expansion in NCM materials, reducing the energy barriers for the migration of Li⁺ and transition metal ions, thus facilitating their release from the lattice and enhancing the reaction kinetics. In comparison to conventional atmospheric pressure hydrometallurgical methods, the pressurized leaching process markedly reduces leaching time, lowers the requisite reaction temperature, and mitigates secondary pollution, presenting a more sustainable and efficient approach to battery recycling.

Graphical Abstract