Citation: Mengxiu Li, Jiahui Mao, Jiangfeng Ni, Liang Li. Three birds with one stone: modification of Li5FeO4 with thermal induction of Lewis acid[J]. Acta Physico-Chimica Sinica, ;2026, 42(4): 100189. doi: 10.1016/j.actphy.2025.100189 shu

Three birds with one stone: modification of Li5FeO4 with thermal induction of Lewis acid

  • Corresponding author: Jiangfeng Ni, jeffni@suda.edu.cn Liang Li, lli@suda.edu.cn
  • Received Date: 10 July 2025
    Revised Date: 6 September 2025
    Accepted Date: 16 September 2025

  • Lithium ferrate Li5FeO4 is a promising cathode prelithiation additive for lithium-ion batteries, boasting a high theoretical capacity of 867 mAh g−1, which compensates for lithium loss due to solid electrolyte interphase (SEI) formation during the initial cycle. However, its practical application faces significant challenges due to inherent chemical instability. The material is extremely sensitive to air, readily undergoing deleterious side reactions with atmospheric carbon dioxide and moisture to form electrochemically inert Li2CO3 surface layers. This degradation in the atmosphere presents several major issues. It not only substantially reduces active lithium content but also induces severe slurry gelation during electrode manufacturing. In addition, it promotes continuous gas generation and electrolyte decomposition during battery operation, and leads to a significant increase in electrochemical impedance. Previous stabilization attempts via carbon coating or metal doping have shown limited success, often introducing new problems such as capacity reduction or inadequate protection, highlighting the urgent need for a more comprehensive and effective modification method. To address these challenges, this study proposes an efficient Lewis acid-induced regeneration strategy through thermal modification with PF5. This approach effectively removes surface inert impurities and facilitates the in-situ construction of a composite layer of Li3PO4 and LiF on the Li5FeO4 particles. The regenerated Li5FeO4 exhibits excellent dispersion, air stability, and electrolyte interfacial compatibility, effectively suppressing slurry gelation and interfacial side reactions. In comparison with the bare counterpart, the regenerated Li5FeO4 shows a significantly reduced viscosity upon slurry processing and gas generation during high-temperature storage. When 1.5% (wt) regenerated Li5FeO4 is introduced to the LiFePO4 cathode in the full cells, the cathode maintains a high capacity of 135.0 mAh g−1 and a retention rate of 95.3% after 200 cycles. In contrast, the control LiFePO4 cathode without Li5FeO4 only retains 113.7 mAh g−1 with a capacity retention of 92.2%. This approach integrates impurity removal, interfacial stabilization, and performance enhancement of Li5FeO4 into one strategy, which will find extensive applications in long-cycle lithium-ion batteries.
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