一石三鸟：路易斯酸热诱导改性Li<sub>5</sub>FeO<sub>4</sub>

引用本文: 李孟修, 毛佳辉, 倪江锋, 李亮. 一石三鸟：路易斯酸热诱导改性Li₅FeO₄[J]. 物理化学学报, 2026, 42(4): 100189. doi: 10.1016/j.actphy.2025.100189 shu

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

一石三鸟：路易斯酸热诱导改性Li₅FeO₄

苏州大学物理科学与技术学院, 江苏省前沿材料物理与器件重点实验室, 苏州市智能光电感知重点实验室, 江苏省先进负碳技术重点实验室, 能源转换材料与物理中心(CECMP), 江苏苏州 215006

通讯作者: Email: jeffni@suda.edu.cn (倪江锋); lli@suda.edu.cn (李亮)

摘要: 铁酸锂(Li₅FeO₄)是一种极具前景的锂离子电池正极预锂化添加剂，但其易与空气中的二氧化碳和水分发生副反应而导致失效。针对这一问题，本研究提出了一种基于PF₅热诱导改性的高效路易斯酸再生策略。该策略可有效去除Li₅FeO₄表面惰性杂质，并原位构建Li₃PO₄与LiF的复合包覆层。再生后的Li₅FeO₄表现出优异的分散性、空气稳定性和电解液界面相容性，能有效抑制浆料凝胶化和界面副反应。当添加1.5% (wt)再生Li₅FeO₄时，LiFePO₄正极在200次循环后仍保持135.0 mAh g⁻¹的容量和95.3%的保持率；而对照组(未添加Li₅FeO₄)仅保留113.7 mAh g⁻¹容量(保持率92.2%)。该研究为Li₅FeO₄的实际应用提供了新思路，将在长循环锂离子电池领域获得广泛应用。

关键词:

English

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

School of Physical Science and Technology, Jiangsu Key Laboratory of Frontier Material Physics and Devices, Suzhou Key Laboratory of Intelligent Photoelectric Perception, Jiangsu Key Laboratory of Advanced Negative Carbon Technologies, Center for Energy Conversion Materials & Physics (CECMP), Soochow University, Suzhou 215006, Jiangsu Province, China

Corresponding author: Email: jeffni@suda.edu.cn (Jiangfeng Ni); lli@suda.edu.cn (Liang Li)

Received Date: 10 July 2025
Accepted Date: 16 September 2025
Revised Date: 06 September 2025
Available Online: 15 April 2026

Abstract: 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.

Key words:

1. [1]
  F. Degen, M. Winter, D. Bendig, J. Tübke, Nat. Energy 8 (2023) 1284, https://doi.org/10.1038/s41560-023-01355-z. doi: 10.1038/s41560-023-01355-z
2. [2]
  C. P. Grey, D. S. Hall, Nat. Commun. 11 (2020) 6279, https://doi.org/10.1038/s41467-020-19991-4. doi: 10.1038/s41467-020-19991-4
3. [3]
  V. Viswanathan, A. H. Epstein, Y. -M. Chiang, E. Takeuchi, M. Bradley, J. Langford, M. Winter, Nature 601 (2022) 519, https://doi.org/10.1038/s41586-021-04139-1. doi: 10.1038/s41586-021-04139-1
4. [4]
  S. Link, A. Stephan, D. Speth, P. Plötz, Nat. Energy 9 (2024) 1032, https://doi.org/10.1038/s41560-024-01531-9. doi: 10.1038/s41560-024-01531-9
5. [5]
  L. Song, H. Liang, S. Li, B. Qiu, Z. Liu, Acta Phys. Chim. Sin. 41 (2025) 100085, https://doi.org/10.1016/j.actphy.2025.100085. doi: 10.1016/j.actphy.2025.100085
6. [6]
  J. Wu, Y. Wu, L. Wang, H. Ye, J. Lu, Y. Li, Adv. Mater. 36 (2023) 2308193, https://doi.org/10.1002/adma.202308193. doi: 10.1002/adma.202308193
7. [7]
  J. Zhu, W. Hu, J. Ni, L. Li, Nat. Sci. Open 3 (2024) 20230078, https://doi.org/10.1360/nso/20230078. doi: 10.1360/nso/20230078
8. [8]
  S. Zhu, Q. Wang, J. Ni, EnergyChem 5 (2023) 100097, https://doi.org/10.1016/j.enchem.2022.100097. doi: 10.1016/j.enchem.2022.100097
9. [9]
  K. Zhang, Z. Wang, Z. Xu, X. Zhou, G. Li, Z. Mei, Y. Yu, Y. Wang, C. Wang, G. Zhu, et al., Energy Stor. Mater. 75 (2025) 104081, https://doi.org/10.1016/j.ensm.2025.104081. doi: 10.1016/j.ensm.2025.104081
10. [10]
  Y. Zhu, Y. Chen, J. Chen, J. Yin, Z. Sun, G. Zeng, X. Wu, L. Chen, X. Yu, H. Luo, et al., Adv. Mater. 36 (2023) 2312159, https://doi.org/10.1002/adma.202312159. doi: 10.1002/adma.202312159
11. [11]
  B. Roy, U. Pal, D. Simondson, C. Nguyen, B. V. Kerr, R. K. Hocking, D. Al-Masri, P. C. Howlett, M. Forsyth, M. Kar, et al., Adv. Funct. Mater. 35 (2025) 2417317, https://doi.org/10.1002/adfm.202417317. doi: 10.1002/adfm.202417317
12. [12]
  L. Lu, G. Jiang, C. Gu, J. Ni, Funct. Mater. Lett. 14 (2021) 2130006, https://doi.org/10.1142/s1793604721300061. doi: 10.1142/s1793604721300061
13. [13]
  V. Nguyen-Tien, C. Zhang, E. Strobl, R. J. R. Elliott, Nat. Energy 10 (2025) 354, https://doi.org/10.1038/s41560-024-01698-1. doi: 10.1038/s41560-024-01698-1
14. [14]
  S. Weng, G. Yang, S. Zhang, X. Liu, X. Zhang, Z. Liu, M. Cao, M. N. Ateş, Y. Li, L. Chen, Z. Wang, X. Wang, Nano-Micro Lett. 15 (2023) 215, https://doi.org/10.1007/s40820-023-01183-6. doi: 10.1007/s40820-023-01183-6
15. [15]
  Y. Yang, Z. Li, M. Zhang, J. Wang, Y. Wang, J. Qiu, H. Zhao, Adv. Mater. 37 (2025) 2417981, https://doi.org/10.1002/adma.202417981. doi: 10.1002/adma.202417981
16. [16]
  Y. Peng, M. Ding, K. Zhang, H. Zhang, Y. Hu, Y. Lin, W. Hu, Y. Liao, S. Tang, J. Liang, et al., ACS Energy Lett. 9 (2024) 6022, https://doi.org/10.1021/acsenergylett.4c02898. doi: 10.1021/acsenergylett.4c02898
17. [17]
  E. W. C. Spotte-Smith, R. L. Kam, D. Barter, X. Xie, T. Hou, S. Dwaraknath, S. M. Blau, K. A. Persson, ACS Energy Lett. 7 (2022) 1446, https://doi.org/10.1021/acsenergylett.2c00517. doi: 10.1021/acsenergylett.2c00517
18. [18]
  C. An, T. Liu, Acta Phys. Chim. Sin. 41 (2025) 100101, https://doi.org/10.1016/j.actphy.2025.100101. doi: 10.1016/j.actphy.2025.100101
19. [19]
  C. Yang, H. Ma, R. Yuan, K. Wang, K. Liu, Y. Long, F. Xu, L. Li, H. Zhang, Y. Zhang, et al., Nat. Energy 8 (2023) 703, https://doi.org/10.1038/s41560-023-01272-1. doi: 10.1038/s41560-023-01272-1
20. [20]
  W. Zhong, Z. Zeng, S. Cheng, J. Xie, Adv. Funct. Mater. 34 (2023) 2307860, https://doi.org/10.1002/adfm.202307860. doi: 10.1002/adfm.202307860
21. [21]
  Y. Sun, H. -W. Lee, Z. W. Seh, N. Liu, J. Sun, Y. Li, Y. Cui, Nat. Energy 1 (2016) 15008, https://doi.org/10.1038/nenergy.2015.8. doi: 10.1038/nenergy.2015.8
22. [22]
  H. Zhang, J. Cheng, H. Liu, D. Li, Z. Zeng, Y. Li, F. Ji, Y. Guo, Y. Wei, S. Zhang, et al., Adv. Energy Mater. 13 (2023) 2300466, https://doi.org/10.1002/aenm.202300466. doi: 10.1002/aenm.202300466
23. [23]
  Y. Chen, Y. Zhu, Z. Sun, X. Kuai, J. Chen, B. Zhang, J. Yin, H. Luo, Y. Tang, G. Zeng, et al., Adv. Mater. 36 (2024) 2407720, https://doi.org/10.1002/adma.202407720. doi: 10.1002/adma.202407720
24. [24]
  M. Diaz‐Lopez, P. A. Chater, P. Bordet, M. Freire, C. Jordy, O. I. Lebedev, V. Pralong, Adv. Energy Mater. 10 (2020) 1902788, https://doi.org/10.1002/aenm.201902788. doi: 10.1002/aenm.201902788
25. [25]
  Y. Sun, H. W. Lee, Z. W. Seh, G. Zheng, J. Sun, Y. Li, Y. Cui, Adv. Energy Mater. 6 (2016) 1600154, https://doi.org/10.1002/aenm.201600154. doi: 10.1002/aenm.201600154
26. [26]
  Z. Rao, J. Wu, B. He, W. Chen, H. Wang, Q. Fu, Y. Huang, ACS Appl. Mater. Interfaces 13 (2021) 38194, https://doi.org/10.1021/acsami.1c06703. doi: 10.1021/acsami.1c06703
27. [27]
  Y. Chen, Y. Zhu, W. Zuo, X. Kuai, J. Yao, B. Zhang, Z. Sun, J. Yin, X. Wu, H. Zhang, et al., Angew. Chem. Int. Ed. 63 (2023) e202316112, https://doi.org/10.1002/anie.202316112. doi: 10.1002/anie.202316112
28. [28]
  W. Zhong, S. Li, M. Liu, Q. Wu, Z. Zeng, S. Cheng, J. Xie, Nano Energy 115 (2023) 108757, https://doi.org/10.1016/j.nanoen.2023.108757. doi: 10.1016/j.nanoen.2023.108757
29. [29]
  H. Kobayashi, Y. Nakamura, M. Nakayama, S. Kodaki, R. Matsuo, I. Honma, Adv. Energy Mater. 13 (2023) 2203441, https://doi.org/10.1002/aenm.202203441. doi: 10.1002/aenm.202203441
30. [30]
  Y. Zhu, R. Xu, Y. Zheng, Y. Chen, J. Yin, J. Xue, B. Zhang, L. Li, G. Zeng, H. Luo, et al., Angew. Chem. Int. Ed. 64 (2025) e202502126, https://doi.org/10.1002/anie.202502126. doi: 10.1002/anie.202502126
31. [31]
  J. Jung, Y. S. Byeon, D. Kim, S. H. Jeong, C. H. Song, E. -J. Lee, S. -M. Oh, M. -S. Park, J. Mater. Chem. A 13 (2025) 1313, https://doi.org/10.1039/d4ta07513g. doi: 10.1039/d4ta07513g
32. [32]
  N. Yao, F. Liu, A. Shao, R. Xue, Q. Jia, Y. Liu, H. Wang, X. Wang, Y. Zhang, M. Zhang, et al., Adv. Mater. 36 (2024) 2408268, https://doi.org/10.1002/adma.202408268. doi: 10.1002/adma.202408268
33. [33]
  L. Feng, J. Guo, C. Sun, X. Xiao, L. Feng, Y. Hao, G. Sun, Z. Tian, T. Li, Y. Li, et al., Small 20 (2024) 2403084, https://doi.org/10.1002/smll.202403084. doi: 10.1002/smll.202403084
34. [34]
  Y. Xia, A. Chen, K. Wang, Q. Mao, H. Huang, J. Zhang, X. He, Y. Gan, Z. Xiao, W. Zhang, Chem. Eng. J. 450 (2022) 138382, https://doi.org/10.1016/j.cej.2022.138382. doi: 10.1016/j.cej.2022.138382
35. [35]
  B. Zhu, W. Zhang, Q. Wang, Y. Lai, J. Zheng, N. Wen, Z. Zhang, Adv. Funct. Mater. 34 (2024) 2315010, https://doi.org/10.1002/adfm.202315010. doi: 10.1002/adfm.202315010
36. [36]
  S. Ramakrishnan, B. Park, J. Wu, W. Yang, B. D. McCloskey, J. Am. Chem. Soc. 142 (2020) 8522, https://doi.org/10.1021/jacs.0c02859. doi: 10.1021/jacs.0c02859
37. [37]
  N. Wen, J. Li, B. Zhu, J. Guo, Z. Zhang, Chem. Eng. J. 497 (2024) 154536, https://doi.org/10.1016/j.cej.2024.154536. doi: 10.1016/j.cej.2024.154536
38. [38]
  B. Zhu, N. Wen, J. Wang, Q. Wang, J. Zheng, Z. Zhang, Chem. Sci. 15 (2024) 12879, https://doi.org/10.1039/d4sc03052d. doi: 10.1039/d4sc03052d
39. [39]
  X. Wang, D. Ren, H. Liang, Y. Song, H. Huo, A. Wang, Y. Gao, J. Liu, Y. Gao, L. Wang, X. He, Energy Environ. Sci. 16 (2023) 1200, https://doi.org/10.1039/d2ee04109j. doi: 10.1039/d2ee04109j
40. [40]
  Y. Wu, R. Xu, Z. Xiao, Z. Wang, R. Zheng, Z. Song, Y. Liu, Adv. Funct. Mater. 35 (2025) 2423478, https://doi.org/10.1002/adfm.202423478. doi: 10.1002/adfm.202423478
41. [41]
  S. S. Zhang, Energy Stor. Mater. 24 (2020) 247, https://doi.org/10.1016/j.ensm.2019.08.013. doi: 10.1016/j.ensm.2019.08.013
42. [42]
  L. Niu, M. Wu, Y. Zhang, C. Gao, X. Li, H. Ding, N. He, P. Wang, J. Zhang, J. Yan, et al., Chem. Eng. J. 498 (2024) 155242, https://doi.org/10.1016/j.cej.2024.155242. doi: 10.1016/j.cej.2024.155242
43. [43]
  L. Li, Y. Hu, J. Liu, Y. Deng, G. Chen, Chem. Eng. J. 503 (2025) 158439, https://doi.org/10.1016/j.cej.2024.158439. doi: 10.1016/j.cej.2024.158439
44. [44]
  B. P. Thapaliya, A. Y. Borisevich, H. M. Meyer, X. G. Sun, C. A. Bridges, S. Dai, Adv. Mater. Interfaces 9 (2022) 2201600, https://doi.org/10.1002/admi.202201600. doi: 10.1002/admi.202201600
45. [45]
  J. Chen, C. Li, J. Zhang, C. Li, J. Chen, Y. Ren, Materials 11 (2018) 1256, https://doi.org/10.3390/ma11071256. doi: 10.3390/ma11071256
46. [46]
  Y. Chu, Y. Mu, L. Zou, Y. Hu, J. Cheng, B. Wu, M. Han, S. Xi, Q. Zhang, L. Zeng, Adv. Mater. 35 (2023) 2212308, https://doi.org/10.1002/adma.202212308. doi: 10.1002/adma.202212308
47. [47]
  M. Sun, Z. Wang, J. Ni, L. Li, Adv. Funct. Mater. 30 (2020) 1910043, https://doi.org/10.1002/adfm.201910043. doi: 10.1002/adfm.201910043
48. [48]
  J. Ni, Y. Zhao, J. Chen, L. Gao, L. Lu, Electrochem. Commun. 44 (2014) 4, https://doi.org/10.1016/j.elecom.2014.04.004. doi: 10.1016/j.elecom.2014.04.004

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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

一石三鸟：路易斯酸热诱导改性Li₅FeO₄

通讯作者: Email: jeffni@suda.edu.cn (倪江锋); lli@suda.edu.cn (李亮)

English

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

Corresponding author: Email: jeffni@suda.edu.cn (Jiangfeng Ni); lli@suda.edu.cn (Liang Li)

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一石三鸟：路易斯酸热诱导改性Li5FeO4

通讯作者: Email: jeffni@suda.edu.cn (倪江锋); lli@suda.edu.cn (李亮)

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

Corresponding author: Email: jeffni@suda.edu.cn (Jiangfeng Ni); lli@suda.edu.cn (Liang Li)

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