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<p>Direct regeneration is considered a sustainable solution to the issue of resource recycling and the environmental pollution caused by discarded lithium-ion batteries (LIBs). However, the direct regeneration of spent LiFePO<sub>4</sub> cathode materials still faces a formidable challenge that the irregular strains induced by the irreversible FePO<sub>4</sub> phase after several charge and discharge cycles hinder the regenerative replenishment of Li<sup>+</sup>. This work proposes a lattice stress modulation strategy that reduces FePO<sub>4</sub> phase into Fe<sub>2</sub>P<sub>2</sub>O<sub>7</sub> phase (reduction of unit cell volume from 271.7 to 122.6 Å<sup>3</sup>), which releases the residual stress, paving continuous transport channels for Li<sup>+</sup>. In addition, the phase transformation reconstructs the FeO<sub>6</sub> octahedra, significantly decreasing the migration energy barrier of ions within the lattice. Ultimately, the steric effect is synergistically weakened, facilitating the replenishment of Li<sup>+</sup> and the elimination of Li-Fe anti-site defects. The regenerated LiFePO<sub>4</sub> cathodes outperform commercial cathodes (80.2% capacity retention after 1000 cycles at 2 C). This work establishes fundamental principles for the pretreatment stage of the direct regeneration process and provides a paradigm shifting solution for sustainable LIBs recycling technology.</p>

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Elimination of lattice strain to reconstruct ion transport channels facilitates direct regeneration of spent LiFePO4 cathode materials

  • 期刊论文

  • 发表日期：

    2026年1月4日

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  • Menghang Sun,
  • Sen Dang,
  • Kai Jia,
  • Bo Wen,
  • Jiyuan Xiao,
  • Xiaofeng Liu,
  • Weijia Li,
  • Song Xue,
  • Limin Liu,
  • Yang Gao,
  • Lili Li,
  • Kai Xi,
  • Wei Yan,
  • Shujiang Ding,
  • Guorui Yang

摘要

Direct regeneration is considered a sustainable solution to the issue of resource recycling and the environmental pollution caused by discarded lithium-ion batteries (LIBs). However, the direct regeneration of spent LiFePO4 cathode materials still faces a formidable challenge that the irregular strains induced by the irreversible FePO4 phase after several charge and discharge cycles hinder the regenerative replenishment of Li+. This work proposes a lattice stress modulation strategy that reduces FePO4 phase into Fe2P2O7 phase (reduction of unit cell volume from 271.7 to 122.6 Å3), which releases the residual stress, paving continuous transport channels for Li+. In addition, the phase transformation reconstructs the FeO6 octahedra, significantly decreasing the migration energy barrier of ions within the lattice. Ultimately, the steric effect is synergistically weakened, facilitating the replenishment of Li+ and the elimination of Li-Fe anti-site defects. The regenerated LiFePO4 cathodes outperform commercial cathodes (80.2% capacity retention after 1000 cycles at 2 C). This work establishes fundamental principles for the pretreatment stage of the direct regeneration process and provides a paradigm shifting solution for sustainable LIBs recycling technology.