<p>With the advent of large-scale lithium-ion battery retirement , efficient recycling of key materials for batteries has significant economic and environmental significance. The layered structure of the graphite anode in spent lithium-ion batteries remains largely unchanged. If its internal impurities can be removed by acid leaching, the high-temperature graphitization step can be omitted to enable recycling. After Na<sub>2</sub>CO<sub>3</sub> roasting at 1000℃,the leaching ratios of Co, Ni, Mn, and Li reached 98.57, 99.93, 98.72, and 99.37%, respectively, under the conditions of 2.5&#xa0;mol·L<sup>-1</sup> H<sub>2</sub>SO<sub>4</sub>, H<sub>2</sub>O<sub>2</sub> content of 6%, 90℃, and a solid-to-liquid ratio of 1:20. Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), and electrochemical performance tests showed that the graphite ordering degree of the sample was significantly enhanced at 1600℃. The graphite layered structure was clear, and the surface impurities were obviously reduced. The discharge-specific capacity of the 1600℃ sample could reach 330&#xa0;mAh·g<sup>-1</sup> at 0.1&#xa0;C, and its first-time coulombic efficiency was 73.51%. The H<sub>2</sub>SO<sub>4</sub> + H<sub>2</sub>O<sub>2</sub> acid leaching process can omit the high-temperature graphitization steps and significantly reduce energy consumption and carbon emissions, thus providing a novel strategy for waste graphite recovery.</p>

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Research on the Deep Removal of Impurities and Repair Process of Graphite Anode of Spent Lithium-Ion Batteries

  • Bohan Geng,
  • Xin Li,
  • Jingbao Lian,
  • Jiao He,
  • Xue Zhang

摘要

With the advent of large-scale lithium-ion battery retirement , efficient recycling of key materials for batteries has significant economic and environmental significance. The layered structure of the graphite anode in spent lithium-ion batteries remains largely unchanged. If its internal impurities can be removed by acid leaching, the high-temperature graphitization step can be omitted to enable recycling. After Na2CO3 roasting at 1000℃,the leaching ratios of Co, Ni, Mn, and Li reached 98.57, 99.93, 98.72, and 99.37%, respectively, under the conditions of 2.5 mol·L-1 H2SO4, H2O2 content of 6%, 90℃, and a solid-to-liquid ratio of 1:20. Raman spectroscopy, field emission scanning electron microscopy (FE-SEM), and electrochemical performance tests showed that the graphite ordering degree of the sample was significantly enhanced at 1600℃. The graphite layered structure was clear, and the surface impurities were obviously reduced. The discharge-specific capacity of the 1600℃ sample could reach 330 mAh·g-1 at 0.1 C, and its first-time coulombic efficiency was 73.51%. The H2SO4 + H2O2 acid leaching process can omit the high-temperature graphitization steps and significantly reduce energy consumption and carbon emissions, thus providing a novel strategy for waste graphite recovery.