Citation: Bingxu Chen, Lei Yi, Ruixi Xie, Rui Gao, Jia Yu, Siqi Shi. Enable high-power fluorinated graphite cathode for lithium primary batteries by metallic ionic liquid-derived surface activation engineering[J]. Chinese Chemical Letters, ;2026, 37(6): 111040. doi: 10.1016/j.cclet.2025.111040 shu

Enable high-power fluorinated graphite cathode for lithium primary batteries by metallic ionic liquid-derived surface activation engineering

Bingxu Chen ^{a, b} ,
Lei Yi ^a ,
Ruixi Xie ^a ,
Rui Gao ^a ,
Jia Yu ^{a, b, *,} ,
Siqi Shi ^{a, *,}

a.
Materials Genome Institute, School of Materials Science and Engineering, Shanghai University, Shanghai 200444, China
b.
State Key Laboratory of Precision and Intelligent Chemistry, University of Science and Technology of China, Hefei 230026, China

jiayu@ustc.edu.cn

sqshi@shu.edu.cn

Received Date: 19 January 2025
Revised Date: 27 February 2025
Accepted Date: 5 March 2025
Available Online: 5 March 2025

Figures(5)

Lithium/fluorinated graphite (Li/CF_x) primary batteries with great energy density advantages still struggle to realize large-scale applications, due to the sluggish cathode reaction kinetics accompanied by poor rate capability and power density. One key challenge arises from the inert electronic structure of CF_x predominated by covalent C–F bond, which results in poor intrinsic electronic conductivity. To address this issue, cathode surface activation engineering is proposed to modify CF_x with hybrid transitional metal oxide/carbon layer, which is derived by one-pot pyrolysis of structurally designable metallic ionic liquids (Bmim[MCl_n], M = Fe, Al, Cu, Zn, etc.). Generally, the presence of metal oxides induces generation of highly conductive semi-ionic C–F species, cooperating with abundant oxygen vacancies and carbon matrix to synergistically improve electronic/ionic conduction and accelerate CF_x conversion kinetics, while the Bmim[FeCl₄]-derived system is the optimal solution. As expected, the surface activated CF_x cathode achieves nearly 4 times the power density (22,581 W/kg at 14 C) of pristine CF_x and higher conversion depth. This metallic ionic liquid-derived surface activation design efficiently regulates the intrinsically inert electronic structure of CF_x cathode, and widens its chemical design space of metal oxides as composite components, furthermore, providing a universal solution for electrodes faced with electronic conduction challenges.
- Lithium primary battery,
- Fluorinated graphite,
- Semi-ionic bond,
- Ionic liquid,
- Electronic conductivity,
- Power density
1. [1]
  D. Wang, G.X. Wang, M.M. Zhang, et al., J. Power Sourc. 541 (2022) 231716. doi: 10.1016/j.jpowsour.2022.231716
2. [2]
  J. Ban, X. Jiao, Y. Feng, et al., ACS Appl. Energy Mater. 4 (2021) 3777–3784. doi: 10.1021/acsaem.1c00177
3. [3]
  J. Meng, Z. Xiao, L. Zhu, et al., Matter 6 (2023) 1685–1716. doi: 10.1016/j.matt.2023.03.032
4. [4]
  D. Li, Y. Yu, C. Li, Adv. Mater. 36 (2024) 2408301. doi: 10.1002/adma.202408301
5. [5]
  Z. Fang, Y. Yang, T.L. Zheng, et al., Energy Stor. Mater. 42 (2021) 477–483.
6. [6]
  Z. Luo, J. Ma, X. Wang, et al., Adv. Mater. 35 (2023) 2303444. doi: 10.1002/adma.202303444
7. [7]
  G.M. Zhong, H.X. Chen, Y. Cheng, et al., J. Mater. Chem. A 7 (2019) 19793–19799. doi: 10.1039/c9ta06800g
8. [8]
  W. Feng, P. Long, Y. Feng, et al., Adv. Sci. 3 (2016) 1500413. doi: 10.1002/advs.201500413
9. [9]
  L. Kong, Y. Li, C. Peng, et al., Nano Energy 104 (2022) 107905. doi: 10.1016/j.nanoen.2022.107905
10. [10]
  S. Jiang, P. Huang, J. Lu, et al., RSC Adv. 11 (2021) 25461–25470. doi: 10.1039/d1ra03873g
11. [11]
  X.Z. Xu, C. Liu, Z.H. Sun, et al., Chem. Soc. Rev. 47 (2018) 3059–3099. doi: 10.1039/c7cs00836h
12. [12]
  X. Chen, K. Fan, Y. Liu, et al., Adv. Mater. 34 (2022) e2101665. doi: 10.1002/adma.202101665
13. [13]
  C. Peng, S. Zhang, L. Kong, et al., Small Meth. 8 (2024) 2301090. doi: 10.1002/smtd.202301090
14. [14]
  A. Tressaud, F. Moguet, S. Flandrois, et al., J. Phys. Chem. Solid 57 (1996) 745–751. doi: 10.1016/0022-3697(96)00343-5
15. [15]
  S. Zhang, L. Kong, Y. Li, et al., Energy Environ. Sci. 16 (2023) 1907–1942. doi: 10.1039/d2ee04179k
16. [16]
  L.Y. Li, R.Z. Wu, H.C. Ma, et al., Small 19 (2023) 2300762. doi: 10.1002/smll.202300762
17. [17]
  Z. Luo, J. Wan, W. Lei, et al., Mater. Technol. 35 (2020) 836–842. doi: 10.1080/10667857.2019.1701255
18. [18]
  Z. Fang, Y. Peng, X. Zhou, et al., ACS Appl. Energy Mater. 5 (2022) 3966–3978. doi: 10.1021/acsaem.1c03476
19. [19]
  Q. Zhang, S. D'Astorg, P. Xiao, et al., J. Power Sourc. 195 (2010) 2914–2917. doi: 10.1016/j.jpowsour.2009.10.096
20. [20]
  J. Yu, D. Wang, G. Wang, et al., Adv. Mater. 35 (2023) 2209210. doi: 10.1002/adma.202209210
21. [21]
  U. Nisar, S.A.J.A. Al-Hail, R.K. Petla, et al., ACS Appl. Energy Mater. 2 (2019) 7263–7271. doi: 10.1021/acsaem.9b01211
22. [22]
  U. Nisar, R. Amin, R. Essehli, et al., J. Power Sourc. 396 (2018) 774–781. doi: 10.1016/j.jpowsour.2018.06.065
23. [23]
  H. Liu, H. Yu, J. Mater. Sci. Technol. 35 (2019) 674–686. doi: 10.1016/j.jmst.2018.10.007
24. [24]
  W. Su, Z. Chen, X. Wang, et al., Chem. Eng. J. 504 (2025) 158827. doi: 10.1016/j.cej.2024.158827
25. [25]
  Y. Zhu, L. Zhang, H. Zhao, et al., J. Mater. Chem. A 5 (2017) 796–803. doi: 10.1039/C6TA07919A
26. [26]
  O. Höfft, S. Báhr, V. Kempter, Langmuir 24 (2008) 11562–11566. doi: 10.1021/la802045j
27. [27]
  F. Lei, M. Yang, F. Jiang, et al., Chem. Eng. J. 360 (2019) 673–679. doi: 10.1016/j.cej.2018.12.044
28. [28]
  R. Zhou, Y. Li, Y. Feng, et al., Compos. Commun. 21 (2020) 100396. doi: 10.1016/j.coco.2020.100396
29. [29]
  P. Kaspar, D. Sobola, R. Dallaev, et al., Appl. Surf. Sci. 493 (2019) 673–678. doi: 10.1016/j.apsusc.2019.07.058
30. [30]
  Z. Ding, C. Yang, J. Zou, et al., Adv. Mater. 33 (2021) 2006118. doi: 10.1002/adma.202006118
31. [31]
  C. Yue, N. Sun, Y. Qiu, et al., Chin. Chem. Lett. 35 (2024) 109698. doi: 10.1016/j.cclet.2024.109698
32. [32]
  Z. Lu, X. Yin, Y. Ji, et al., Energy Mater. 4 (2024) 400038.
33. [33]
  Y. Ito, C. Lee, Y. Miyahara, et al., Chem. Mater. 34 (2022) 8711–8718. doi: 10.1021/acs.chemmater.2c01850
34. [34]
  B. Deng, P.A. Advincula, D.X. Luong, et al., Nat. Commun. 13 (2022) 5027.
35. [35]
  J.L. Meng, Z.H. Yang, L.L. Chen, et al., Mater. Today Energy 15 (2020) 100370. doi: 10.1016/j.mtener.2019.100370
36. [36]
  C.W. Yang, P. Woottapanit, S.N. Geng, et al., Adv. Mater. 36 (2024) 2408908. doi: 10.1002/adma.202408908
37. [37]
  Y. Lu, J.L. Qin, T. Shen, et al., Adv. Energy Mater. 11 (2021) 2101780. doi: 10.1002/aenm.202101780
38. [38]
  L. Yu, G. Diao, F. Ye, et al., Catal. Lett. 141 (2011) 111–119. doi: 10.1007/s10562-010-0475-0
39. [39]
  H.S. Kim, J.B. Cook, H. Lin, et al., Nat. Mater. 16 (2017) 454–460. doi: 10.1038/nmat4810
40. [40]
  J. Yu, Y. Wang, L. Kong, et al., ACS Nano 13 (2019) 9148–9160. doi: 10.1021/acsnano.9b03474
41. [41]
  J. Liu, Y. Xiang, Y. Chen, et al., Environ. Sci. Technol. 57 (2023) 12453–12464. doi: 10.1021/acs.est.3c03441
42. [42]
  M.S. Whittingham, J. Electrochem. Soc. 122 (1975) 526–527. doi: 10.1149/1.2134252
43. [43]
  S. Rana, R.C. Thakur, H.S. Dosanjh, Solid State Ion. 400 (2023) 116340. doi: 10.1016/j.ssi.2023.116340
44. [44]
  Z. Guo, H. Yang, Q. Wei, et al., Chin. Chem. Lett. 35 (2024) 108622. doi: 10.1016/j.cclet.2023.108622
45. [45]
  R. Tian, S.H. Park, P.J. King, et al., Nat. Commun. 10 (2019) 1933.
46. [46]
  T. Xu, W. Sun, T. Kong, et al., Acta Phys. Chim. Sin. 40 (2024) 2303021.
47. [47]
  Z. Luo, X. Wang, D. Chen, et al., ACS Appl. Mater. Interf. 13 (2021) 18809–18820. doi: 10.1021/acsami.1c02064
48. [48]
  Y. Meng, M. Wang, K. Li, et al., Nano Lett. 23 (2023) 2295–2303. doi: 10.1021/acs.nanolett.2c05077
49. [49]
  C. Sun, Y. Feng, Y. Li, et al., Nanoscale 6 (2014) 2634–2641.
50. [50]
  X. Miao, J. Yang, W. Pan, et al., Electrochim. Acta 210 (2016) 704–711.
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