<p>With the accelerating global transition toward carbon neutrality, renewable energy technologies such as solar and wind power have rapidly developed, driving an urgent demand for efficient, low-cost, and large-scale energy storage systems. Lithium-ion batteries (LIBs) have become the dominant choice for portable electronics and electric vehicles due to their high energy density and long cycle life. However, further performance improvements are required to meet future grid-scale storage and high-energy applications. Silicon has attracted significant attention as an anode material because of its ultrahigh theoretical capacity (≈4200 mAh·g<sup>−1</sup>) and low operating potential, offering great potential to enhance the energy density of LIBs. Nevertheless, severe volume expansion during lithiation and poor intrinsic conductivity remain key challenges. Utilizing silicon waste as an anode precursor not only provides a low-cost material source but also aligns with the goals of sustainable resource utilization and the circular economy. Unlike previous approaches that primarily focused on purified silicon powders or laboratory-synthesized nanoparticles, the present study applies a simple H<sub>2</sub>O<sub>2</sub>-assisted wet ball-milling oxidation directly to industrial silicon waste, and systematically investigates the influence of the H<sub>2</sub>O<sub>2</sub>/Si ratio on oxide-shell formation, Fe-Si phase evolution, and electrochemical behavior. The addition of an optimal proportion of H<sub>2</sub>O<sub>2</sub> for oxidation modification can facilitate the formation of a silica-oxygen structure on the silicon waste particles. Additionally, the Fe and Si form the FeSi<sub><i>x</i></sub> phase with an oxidation layer on the surface acting as a buffer to mitigate silicon's volume expansion during cycling. H<sub>2</sub>O<sub>2</sub> modification enhances the structural stability of silicon waste by forming SiO<sub><i>x</i></sub>, where the Si–O bond exhibits greater strength and mechanical stability than the Si–Si bond, thereby mitigating the stress caused by volume expansion of silicon. The material exhibited an initial Coulombic efficiency of 58.4%, an initial charge-specific capacity of 993 mAh·g<sup>−1</sup>, and a capacity retention of 77.1% (652.4 mAh·g<sup>−1</sup>) after 300 cycles.</p>

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Oxidation modification of silicon waste for LIB anode material

  • Hehang Sun,
  • Bowen Li,
  • Hui Tian,
  • Jiao Hou,
  • Xinwei Wang,
  • Jiandong Wu,
  • Yajuan Fen,
  • Beiping Wang,
  • Chunping Hou

摘要

With the accelerating global transition toward carbon neutrality, renewable energy technologies such as solar and wind power have rapidly developed, driving an urgent demand for efficient, low-cost, and large-scale energy storage systems. Lithium-ion batteries (LIBs) have become the dominant choice for portable electronics and electric vehicles due to their high energy density and long cycle life. However, further performance improvements are required to meet future grid-scale storage and high-energy applications. Silicon has attracted significant attention as an anode material because of its ultrahigh theoretical capacity (≈4200 mAh·g−1) and low operating potential, offering great potential to enhance the energy density of LIBs. Nevertheless, severe volume expansion during lithiation and poor intrinsic conductivity remain key challenges. Utilizing silicon waste as an anode precursor not only provides a low-cost material source but also aligns with the goals of sustainable resource utilization and the circular economy. Unlike previous approaches that primarily focused on purified silicon powders or laboratory-synthesized nanoparticles, the present study applies a simple H2O2-assisted wet ball-milling oxidation directly to industrial silicon waste, and systematically investigates the influence of the H2O2/Si ratio on oxide-shell formation, Fe-Si phase evolution, and electrochemical behavior. The addition of an optimal proportion of H2O2 for oxidation modification can facilitate the formation of a silica-oxygen structure on the silicon waste particles. Additionally, the Fe and Si form the FeSix phase with an oxidation layer on the surface acting as a buffer to mitigate silicon's volume expansion during cycling. H2O2 modification enhances the structural stability of silicon waste by forming SiOx, where the Si–O bond exhibits greater strength and mechanical stability than the Si–Si bond, thereby mitigating the stress caused by volume expansion of silicon. The material exhibited an initial Coulombic efficiency of 58.4%, an initial charge-specific capacity of 993 mAh·g−1, and a capacity retention of 77.1% (652.4 mAh·g−1) after 300 cycles.