Citation: Yuqing Dai, Zihan Hou, Gui Luo, Duo Deng, Wenjie Peng, Zhixing Wang, Huajun Guo, Xinhai Li, Guochun Yan, Hui Duan, Wenchao Zhang, Jiexi Wang. Exploring of the upper limit of nickel content in cathode materials for PEO-based solid-state batteries[J]. Chinese Chemical Letters, ;2026, 37(7): 111157. doi: 10.1016/j.cclet.2025.111157 shu

Exploring of the upper limit of nickel content in cathode materials for PEO-based solid-state batteries

Yuqing Dai ^a ,
Zihan Hou ^a ,
Gui Luo ^b ,
Duo Deng ^b ,
Wenjie Peng ^{a, b} ,
Zhixing Wang ^{a, c} ,
Huajun Guo ^{a, c} ,
Xinhai Li ^{a, c} ,
Guochun Yan ^{a, c} ,
Hui Duan ^{a, c} ,
Wenchao Zhang ^a ,
Jiexi Wang ^{a, c, *,}

a.
National Energy Metal Resources and New Materials Key Laboratory, Engineering Research Center of the Ministry of Education for Advanced Battery Materials, Hunan Provincial Key Laboratory of Nonferrous Value-Added Metallurgy, School of Metallurgy and Environment, Central South University, Changsha 410083, China
b.
BASF Shanshan Battery Materials Co., Ltd., Changsha 410205, China
c.
National Engineering Research Centre of Advanced Energy Storage Materials, Changsha 410205, China

wangjiexikeen@csu.edu.cn

Received Date: 15 February 2025
Revised Date: 19 March 2025
Accepted Date: 27 March 2025
Available Online: 27 March 2025

Figures(5)

The combination of high-nickel cathodes with poly(ethylene oxide) (PEO)-based solid-state electrolytes represents a promising strategy to achieve both high energy density and enhanced safety. However, existing studies predominantly employ LiFePO₄ cathodes due to the inherent limitations of PEO-based electrolytes in high-voltage stability. Even with the improved electrochemical stability window (ESW) of PEO-based electrolytes, current implementations still utilize low-nickel-content (≤80%) cathodes. To further enhance the energy density of PEO-based solid-state batteries (SSBs), this work employs high-nickel-content (> 80%) cathodes in conjunction with PEO-based electrolytes. The influence of nickel content in cathode materials (CAMs) on the electrochemical performance of PEO-based SSBs is systematically investigated through a progressive nickel content optimization approach. This study elucidates the intrinsic relationship between the nickel content and the characteristic capacity activation mechanism observed during the initial cycling phases in solid-state battery systems, revealing a nickel-content-dependent electrochemical activation pattern unique to solid-state configurations. Additionally, through a series of detection schemes, the failure mechanism of high-nickel PEO-based SSBs is systematically studied from the cathode/electrolyte interface, electrolyte, and CAM. Particularly, the degree of PEO decomposition is quantitatively analyzed using differential electrochemical mass spectrometry (DEMS) and gel permeation chromatography (GPC). This work reveals the key issues faced when further increasing the nickel content of CAMs, providing insights for targeted modification designs of high-nickel PEO-based solid-state batteries in the future.
- Poly(ethylene oxide),
- Ultrahigh-nickel cathode,
- Solid-state battery,
- Cathode-electrolyte interphase,
- Room temperature
1. [1]
  T. Ma, Q. Zhang, Y. Tang, et al., Renew. Sustain. Energy Rev. 204 (2024) 114806. doi: 10.1016/j.rser.2024.114806
2. [2]
  D. Qiao, Y. Ma, Y. Bao, et al., J. Clean. Prod. 444 (2024) 141139. doi: 10.1016/j.jclepro.2024.141139
3. [3]
  K. Shahzad, I.I. Cheema, J. Power Sources 591 (2024) 233888. doi: 10.1016/j.jpowsour.2023.233888
4. [4]
  W. Zhao, K. Zhang, F. Wu, et al., Chem. Eng. J. 453 (2023) 139348. doi: 10.1016/j.cej.2022.139348
5. [5]
  Z. Liu, Y. Ma, N.A. Khan, et al., Angew. Chem. Int. Ed. 64 (2024) e202419663.
6. [6]
  X. Hu, F. Gao, Y. Xiao, et al., Chem. Eng. J. 481 (2024) 148450. doi: 10.1016/j.cej.2023.148450
7. [7]
  M. Wu, S. Han, S. Liu, J. Zhao, W. Xie, Energy Storage Mater. 66 (2024) 103174. doi: 10.1016/j.ensm.2024.103174
8. [8]
  Y. Luo, Z. Rao, X. Yang, et al., Energy Environ. Sci. 17 (2024) 7543–7565. doi: 10.1039/d4ee02358g
9. [9]
  M. Ge, X. Zhou, Y. Qin, et al., Chin. Chem. Lett. 33 (2022) 3894–3898. doi: 10.1016/j.cclet.2021.11.073
10. [10]
  X. Huang, T. Li, W. Fan, R. Xiao, X.B. Cheng, Adv. Energy Mater. 14 (2024) 2303850. doi: 10.1002/aenm.202303850
11. [11]
  S. Liu, L. Zhou, T. Zhong, X. Wu, K. Neyts, Adv. Energy Mater. 14 (2024) 2403602. doi: 10.1002/aenm.202403602
12. [12]
  M. Xu, D. Li, Y. Feng, et al., Adv. Mater. 36 (2024) 2405079. doi: 10.1002/adma.202405079
13. [13]
  Q. Zhang, R. Yang, C. Li, et al., J. Energy Chem. 89 (2024) 18–26. doi: 10.1016/j.jechem.2023.10.025
14. [14]
  S. Xiao, L. Ren, W. Liu, L. Zhang, Q. Wang, Energy Storage Mater. 63 (2023) 102970. doi: 10.1016/j.ensm.2023.102970
15. [15]
  M.A. Cabañero Martínez, N. Boaretto, A.J. Naylor, et al., Adv. Energy Mater. 12 (2022) 2201264. doi: 10.1002/aenm.202201264
16. [16]
  S. Wan, W. Ma, Y. Wang, Y. Xiao, S. Chen, Adv. Mater. 36 (2024) 2311912. doi: 10.1002/adma.202311912
17. [17]
  F. Pei, Y. Huang, L. Wu, et al., Adv. Mater. 36 (2024) 2409269. doi: 10.1002/adma.202409269
18. [18]
  M. Zuo, Z. Bi, X. Guo, Chem. Eng. J. 463 (2023) 142463. doi: 10.1016/j.cej.2023.142463
19. [19]
  Y. Guo, X. Qu, Z. Li, R. Tian, X. Liu, Chin. Chem. Lett. 35 (2024) 108482. doi: 10.1016/j.cclet.2023.108482
20. [20]
  H.R. Oliveira Filho, H. Zanin, R.S. Monteiro, M.H.P. Barbosa, R.F. Teófilo, J. Energy Storage 82 (2024) 110536. doi: 10.1016/j.est.2024.110536
21. [21]
  S.Y. Kim, Y.J. Yang, E.G. Lee, et al., Chem. Eng. J. 482 (2024) 148869. doi: 10.1016/j.cej.2024.148869
22. [22]
  S. Kim, M. Kim, M. Ku, et al., ACS Nano 18 (2024) 25096–25106. doi: 10.1021/acsnano.4c06720
23. [23]
  M. Lu, Z. Wang, G. Luo, et al., Chin. Chem. Lett. 35 (2024) 108638. doi: 10.1016/j.cclet.2023.108638
24. [24]
  Y. Yusim, E. Trevisanello, R. Ruess, et al., Angew. Chem. Int. Ed. 62 (2023) e202218316. doi: 10.1002/anie.202218316
25. [25]
  X. Tang, X. Xu, M. Bai, et al., Adv. Funct. Mater. 33 (2023) 2210465. doi: 10.1002/adfm.202210465
26. [26]
  H. An, M. Li, Q. Liu, et al., Nat. Commun. 15 (2024) 9150. doi: 10.1038/s41467-024-53094-8
27. [27]
  H. Xiang, N. Deng, L. Gao, et al., Chin. Chem. Lett. 35 (2024) 109182. doi: 10.1016/j.cclet.2023.109182
28. [28]
  Y. Dai, J. Tan, Z. Hou, et al., ACS Nano 18 (2024) 22518–22532. doi: 10.1021/acsnano.4c07997
29. [29]
  Z. Zhang, Y. Ren, J. Liang, et al., Energy Storage Mater. 71 (2024) 103667. doi: 10.1016/j.ensm.2024.103667
30. [30]
  J. Huang, C. Li, D. Jiang, et al., Adv. Funct. Mater. 35 (2025) 2411171. doi: 10.1002/adfm.202411171
31. [31]
  B. Chu, Y.J. Guo, J.L. Shi, et al., J. Power Sources 544 (2022) 231873. doi: 10.1016/j.jpowsour.2022.231873
32. [32]
  K. Zhou, Z. Gao, X. Deng, et al., J. Mater. Chem. A 9 (2021) 11219–11227. doi: 10.1039/d1ta01408k
33. [33]
  Y. Fu, K. Yang, S. Xue, et al., Adv. Funct. Mater. 33 (2023) 2210845. doi: 10.1002/adfm.202210845
34. [34]
  J. Li, H. Hu, W. Fang, et al., Adv. Funct. Mater. 33 (2023) 2303718. doi: 10.1002/adfm.202303718
35. [35]
  W. Wu, Z. Wei, J. Wang, et al., Chem. Eng. J. 424 (2021) 130335. doi: 10.1016/j.cej.2021.130335
36. [36]
  R. Zhang, C. Wang, M. Ge, H.L. Xin, Nano Lett. 22 (2022) 3818–3824. doi: 10.1021/acs.nanolett.2c01103
37. [37]
  Z. Wang, H. Zhu, H. Yu, et al., Chin. Chem. Lett. 34 (2023) 107718. doi: 10.1016/j.cclet.2022.07.061
38. [38]
  Y. Zheng, Y. Yao, J. Ou, et al., Chem. Soc. Rev. 49 (2020) 8790–8839. doi: 10.1039/d0cs00305k
39. [39]
  Z. Feng, X. Qiu, X. Chen, H. Wang, X. Guo, ACS Appl. Mater. Interfaces 16 (2024) 42995–43005. doi: 10.1021/acsami.4c09122
40. [40]
  Y.Y. Sun, Q. Zhang, L. Yan, T.B. Wang, P.Y. Hou, Chem. Eng. J. 437 (2022) 135179. doi: 10.1016/j.cej.2022.135179
41. [41]
  B. Guo, Y. Fu, J. Wang, et al., Chem. Commun. 58 (2022) 8182–8193. doi: 10.1039/d2cc02306g
42. [42]
  P. Liu, L. Yang, B. Xiao, et al., Adv. Funct. Mater. 32 (2022) 2208586. doi: 10.1002/adfm.202208586
43. [43]
  H. Wang, E. Rus, T. Sakuraba, et al., Anal. Chem. 86 (2014) 6197–6201. doi: 10.1021/ac403317d
44. [44]
  K. Nie, X. Wang, J. Qiu, et al., ACS Energy Lett. 5 (2020) 826–832. doi: 10.1021/acsenergylett.9b02739
45. [45]
  J. Li, Y. Ji, H. Song, et al., Nano-Micro Lett. 14 (2022) 191. doi: 10.1007/s40820-022-00936-z
46. [46]
  Q. Zhang, K. Liu, C. Li, et al., Nano Energy 86 (2021) 106096. doi: 10.1016/j.nanoen.2021.106096
47. [47]
  Q. Han, S. Wang, W. Kong, et al., Chem. Eng. J. 454 (2023) 140104. doi: 10.1016/j.cej.2022.140104
48. [48]
  X. Tang, C. Zhu, Y. Yang, et al., Chin. Chem. Lett. 35 (2024) 110014. doi: 10.1016/j.cclet.2024.110014
49. [49]
  X. Yang, M. Jiang, X. Gao, et al., Energy Environ. Sci. 13 (2020) 1318–1325. doi: 10.1039/d0ee00342e
50. [50]
  J. Chen, S. Han, Chem. Eng. J. 470 (2023) 144150. doi: 10.1016/j.cej.2023.144150
51. [51]
  M.A.H. Farmer, O.M. Musa, S.P. Armes, Angew. Chem. Int. Ed. 62 (2023) e202309526. doi: 10.1002/anie.202309526
52. [52]
  C. Xu, P.J. Reeves, Q. Jacquet, C.P. Grey, Adv. Energy Mater. 11 (2021) 2003404. doi: 10.1002/aenm.202003404
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