Citation: Haotian Zhang, Shengfa Feng, Mufan Cao, Xiong Xiong Liu, Pengcheng Yuan, Yaping Wang, Min Gao, Long Pan, Zhengming Sun. Al₂O₃ coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries[J]. Chinese Chemical Letters, ;2025, 36(8): 111096. doi: 10.1016/j.cclet.2025.111096 shu

Al₂O₃ coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries

School of Materials Science and Engineering, Southeast University, Nanjing 211189, China

panlong@seu.edu.cn

zmsun@seu.edu.cn

Received Date: 3 January 2025
Revised Date: 11 March 2025
Accepted Date: 16 March 2025
Available Online: 18 March 2025

Figures(6)

The ineluctable introduction of lithium salt to polymer solid-state electrolytes incurs a compromise between strength, ionic conductivity, and thickness. Here, we propose Al₂O₃-coated polyimide (AO/PI) porous film as a high-strength substrate to support fast-ion-conducting polymer-in-salt (PIS) solid-state electrolytes, aiming to suppress lithium dendrite growth and improve full-cell performance. The Al₂O₃ coating layer not only refines the wettability of polyimide porous film to PIS, but also performs as a high modulus protective layer to suppress the growth of lithium dendrites. The resulting PI/AO@PIS exhibits a small thickness of only 35 µm with an outstanding tensile strength of 11.3 MPa and Young's modulus of 537.6 MPa. In addition, the PI/AO@PIS delivers a high ionic conductivity of 0.1 mS/cm at 25 ℃. As a result, the PI/AO@PIS enables symmetric Li cells to achieve exceptional cyclability for over 1000 h at 0.1 mA/cm² without noticeable lithium dendrite formation. Moreover, the PI/AO@PIS-based LiFePO₄Li full cells demonstrate outstanding rate performance (125.7 mAh/g at 5 C) and impressive cycling stability (96.1% capacity retention at 1 C after 200 cycles). This work highlights the efficacy of enhancing the mechanical properties of polymer matrices and extending cell performance through the incorporation of a dense inorganic interface layer.
- Polymer-in-salt solid-state electrolytes,
- Inorganic interface layer,
- Al₂O₃ interfacial layer,
- Li dendrites,
- Cycling performance
1. [1]
  Z. Cheng, T. Liu, B. Zhao, et al., Energy Storage Mater. 34 (2021) 388–416.
2. [2]
  L. Xu, J. Li, H. Shuai, et al., J. Energy Chem. 67 (2022) 524–548.
3. [3]
  B.H. Zhang, Y. Wu, Y.L. Hou, et al., Small 20 (2023) 2305322.
4. [4]
  Y.L. Liao, J.K. Hu, Z.H. Fu, et al., J. Energy Chem. 80 (2023) 458–465.
5. [5]
  S.J. Yang, X. Shen, X.B. Cheng, et al., J. Energy Chem. 69 (2022) 70–75.
6. [6]
  S.J. Yang, J.K. Hu, F.N. Jiang, et al., InfoMat 6 (2023) e12512.
7. [7]
  P. Liu, Z. Qiu, F. Cao, et al., J. Mater. Sci. Technol. 177 (2024) 68–78.
8. [8]
  Y. Zheng, Y. Yao, J. Ou, et al., Chem. Soc. Rev. 49 (2020) 8790–8839. doi: 10.1039/d0cs00305k
9. [9]
  P.P. Paul, E.J. McShane, A.M. Colclasure, et al., Adv. Energy Mater. 11 (2021) 2100372.
10. [10]
  S.J. Yang, H. Yuan, N. Yao, et al., Adv. Mater. 36 (2024) 2405086.
11. [11]
  H. Zhang, C. Li, M. Piszcz, et al., Chem. Soc. Rev. 46 (2017) 797–815.
12. [12]
  Y. Chen, K. Wen, T. Chen, et al., Energy Storage Mater. 31 (2020) 401–433.
13. [13]
  X. Li, C. Yi, W. Hu, et al., Chin. Chem. Lett. 36 (2025) 110215.
14. [14]
  T.T. Vu, H.J. Cheon, S.Y. Shin, et al., Energy Storage Mater. 61 (2023) 102876.
15. [15]
  S. Liu, W. Liu, D. Ba, et al., Adv. Mater. 35 (2023) e2110423.
16. [16]
  C. Fang, K. Huang, J. Zhao, et al., Nano Res. 17 (2024) 5251–5260. doi: 10.1007/s12274-024-6502-z
17. [17]
  B. Halder, M.G. Mohamed, S.W. Kuo, P. Elumalai, Mater. Today Chem. 36 (2024) 101926.
18. [18]
  M. Martinez-Ibañez, E. Sanchez-Diez, L. Qiao, et al., Adv. Funct. Mater. 30 (2020) 2000455.
19. [19]
  S. Zhao, J. Lu, B. Sheng, et al., Chin. Chem. Lett. 36 (2025) 110008.
20. [20]
  Y. Ma, C. Wang, K. Yang, et al., ACS Appl. Mater. Interface. 15 (2023) 17978–17985. doi: 10.1021/acsami.3c02084
21. [21]
  H. Liang, L. Wang, A. Wang, et al., Nano-Micro Lett. 15 (2023) 42.
22. [22]
  A. Du, H. Lu, S. Liu, et al., Adv. Energy Mater. 14 (2024) 2400808.
23. [23]
  Z. Wang, L. Shen, S. Deng, P. Cui, X. Yao, Adv. Mater. 33 (2021) e2100353.
24. [24]
  Y. Wang, P. Yuan, X.X. Liu, et al., Adv. Funct. Mater. 34 (2024) 2405060.
25. [25]
  Z. Zhao, Y. Pan, H. Chen, et al., Adv. Funct. Mater. 34 (2024) 2402182.
26. [26]
  X. Shi, Z. Jia, D. Wang, et al., Adv. Mater. 36 (2024) e2405097.
27. [27]
  Y. Han, B. Liu, Z. Xiao, et al., InfoMat 3 (2021) 155–174. doi: 10.1002/inf2.12166
28. [28]
  Y. Zhang, Y.Z. Song, J.J. Yuan, et al., J. Appl. Polym. Sci. 135 (2018) 46423.
29. [29]
  M.M. Methani, M. Revilla-Leon, A. Zandinejad, J. Esthet. Restor. Dent. 32 (2020) 182–192. doi: 10.1111/jerd.12535
30. [30]
  M. Choudhuri, D. Choudhury, J. Mukhopadhyay, M. Mukhopadhyay, Macromol. Symp. 388 (2019) 1900031.
31. [31]
  S. Ahmad, S.A. Agnihotry, Curr. Appl. Phys. 9 (2009) 108–114.
32. [32]
  J. Wang, Y. Liu, Q. Cai, et al., Adv. Mater. 34 (2021) 2107957.
33. [33]
  A.J. Blake, R.R. Kohlmeyer, J.O. Hardin, et al., Adv. Energy Mater. 7 (2017) 1602920.
34. [34]
  W. Yang, Y. Liu, X. Sun, et al., Angew. Chem. Int. Ed. 63 (2024) e202401428.
35. [35]
  Y. Yao, Z. Wei, H. Wang, et al., Adv. Energy Mater. 10 (2020) 1903698.
36. [36]
  X. Huang, S. Huang, T. Wang, et al., Adv. Funct. Mater. 33 (2023) 2300683.
37. [37]
  W. Liu, S.W. Lee, D. Lin, et al., Nat. Energy 2 (2017) 17035.
38. [38]
  P. Liu, S. Shen, Z. Qiu, et al., Adv. Mater. 36 (2024) 2312812.
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12. [12]
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沈阳化工大学材料科学与工程学院沈阳 110142

Al2O3 coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries

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通讯作者: 陈斌, bchen63@163.com

Al₂O₃ coated polyimide porous films enable thin yet strong polymer-in-salt solid-state electrolytes for dendrite-free lithium metal batteries