Citation: Bao Li, Pengyao Yan, Mengmin Jia, Liang Wang, Yaru Qiao, Haowen Li, Canhui Wu, Zhuangzhuang Zhang, Dongmei Dai, Dai-Huo Liu. Engineering lithiophilic LiC_x layer to robust interfacial chemistry between LAGP and Li anode for Li-metal batteries[J]. Chinese Chemical Letters, ;2025, 36(7): 110145. doi: 10.1016/j.cclet.2024.110145 shu

Engineering lithiophilic LiC_x layer to robust interfacial chemistry between LAGP and Li anode for Li-metal batteries

Bao Li ^{a, b} ,
Pengyao Yan ^{a, b} ,
Mengmin Jia ^a ,
Liang Wang ^a ,
Yaru Qiao ^{a, b} ,
Haowen Li ^a ,
Canhui Wu ^a ,
Zhuangzhuang Zhang ^{a, *,} ,
Dongmei Dai ^{a, *,} ,
Dai-Huo Liu ^{a, *,}

a.
Key Laboratory of Green Chemical Media and Reactions (Ministry of Education), Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, School of Chemistry and Chemical Engineering, Henan Normal University, Xinxiang 453007, China
b.
CAS Henan Industrial Technology Innovation & Incubation Center, Zhengzhou 450000, China

zhangzhuangzhuang@htu.edu.cn

daidongmei@htu.edu.cn

liudaihuo@htu.edu.cn

Received Date: 17 April 2024
Revised Date: 16 May 2024
Accepted Date: 20 June 2024
Available Online: 22 June 2024

Figures(6)

NASICON type solid electrolyte Li_1+xAl_xGe₂₋_x(PO₄)₃ (LAGP) is one of the most potential candidates in view of their high ionic conductivity, high oxidation resistance and excellent air stability. However, inevitable interface issues often cause severe performance degradation, seriously affecting its commercial application. Herein, a lithiophilic carbon buffer layer is constructed on the LAGP surface adjacent to the Li electrode side by a facile pyrolysis reaction, then the LiC_x interlayer is generated in situ between the carbon buffer layer and lithium metal, which can guide uniform ion transport while improving interface contact. Thus, the LiC_x-LAGP showed excellent ionic conductivity, high flexibility and lithiophilic interphase. Specially, the LiLiC_x-LAGPLi battery has achieved a 1000 h stable cycles at 0.1 mA/cm², remarkably, the LiLiC_x-LAGPLFP battery retains 85% of their initial capacity after 200 cycles under 1 C, even for the NCM811 cathode, the battery still has a good cycle performance.
- Lithiophilic LiC_x layer,
- Interfacial chemistry,
- Li_1+xAl_xGe_2−x(PO₄)₃,
- Side reaction,
- Solid-state Li-metal batteries
1. [1]
  L. Xu, S. Tang, Y. Cheng, et al., Joule 2 (2018) 1991–2015.
2. [2]
  X. Cao, Y. Xu, L. Zou, et al., Energy Environ. Sci. 16 (2023) 1548–1559. doi: 10.1039/d2ee03557j
3. [3]
  D.H. Liu, Z. Bai, M. Li, et al., Chem. Soc. Rev. 49 (2020) 5407–5445. doi: 10.1039/c9cs00636b
4. [4]
  X. Zhao, X. Wang, Z. Gu, et al., Adv. Funct. Mater. 34 (2024) 2402447. doi: 10.1002/adfm.202402447
5. [5]
  J. Yu, Q. Liu, X. Hu, et al., Energy Stor. Mater. 46 (2022) 68–75. doi: 10.36463/idw.2022.0068
6. [6]
  R. Jia, H. Dai, X. Tu, et al., Adv. Energy Mater. 13 (2023) 2302747.
7. [7]
  Y. Liu, J. Meng, M. Lei, et al., Adv. Funct. Mater. 33 (2023) 2208013.
8. [8]
  J. Janek, W.G. Zeier, Nat. Energy 8 (2023) 230–240. doi: 10.1038/s41560-023-01208-9
9. [9]
  X. Ma, J. Yu, Y. Hu, J. Texter, F. Yan, Ind. Chem. Mater. 1 (2023) 39–59. doi: 10.1039/d2im00051b
10. [10]
  P. Zhai, T. Wang, H. Jiang, et al., Adv. Mater. 33 (2021) 2006247.
11. [11]
  Y. Zhu, M. Ge, F. Ma, et al., Adv. Funct. Mater. 34 (2023) 2301964.
12. [12]
  H. Dai, X. Gu, J. Dong, et al., Nat. Commun. 11 (2020) 643.
13. [13]
  W. Diao, D. Xie, Y. Wang, et al., Inorg. Chem. Front. 11 (2024) 947–956. doi: 10.1039/d3qi02243a
14. [14]
  Y. Liu, M. Su, Z. Gu, et al., Chem. Rec. 22 (2022) e202200081.
15. [15]
  C. Yang, H. Xie, W. Ping, et al., Adv. Mater. 31 (2019) 1804815.
16. [16]
  Z. Zhang, Y. Qiao, Q. Deng, et al., Inorg. Chem. Front. 10 (2023) 1286–1293. doi: 10.1039/d2qi02393h
17. [17]
  L. Xue, H. Gao, Y. Li, J.B. Goodenough, J. Am. Chem. Soc. 140 (2018) 3292–3298. doi: 10.1021/jacs.7b12267
18. [18]
  H. Hou, J. Qiu, B. Li, et al., Chin. Chem. Lett. 34 (2023) 108810.
19. [19]
  W. Xia, Y. Zhao, F. Zhao, et al., Chem. Rev. 122 (2022) 3763–3819. doi: 10.1021/acs.chemrev.1c00594
20. [20]
  H. Wang, N. Qin, Y. Li, et al., Carbon 205 (2023) 435–443.
21. [21]
  S. Zeng, G.M. Arumugam, W. Li, et al., J. Energy Chem. 51 (2020) 222–229.
22. [22]
  X. Chen, W. He, L.X. Ding, S. Wang, H. Wang, Energy Environ. Sci. 12 (2019) 938–944. doi: 10.1039/c8ee02617c
23. [23]
  M. Ihsan-Ul-Haq, H. Huang, J. Wu, et al., Carbon 171 (2021) 119–129.
24. [24]
  Q. Liu, Q. Yu, S. Li, et al., Energy Stor. Mater. 25 (2020) 613–620.
25. [25]
  Z. Zhang, S. Chen, X. Yao, et al., Energy Stor. Mater. 24 (2020) 714–718.
26. [26]
  R. Dewees, H. Wang, ChemSusChem 12 (2019) 3713–3725. doi: 10.1002/cssc.201900725
27. [27]
  A. Paolella, W. Zhu, G.L. Xu, et al., Adv. Energy Mater. 10 (2020) 2001497.
28. [28]
  Z.T. Xiao, J.S. Meng, F.J. Xia, et al., Energy Environ. Sci. 13 (2020) 3129–3137. doi: 10.1039/d0ee01607a
29. [29]
  Y.D. Huang, H.X. Wei, P.Y. Li, et al., J. Energy Chem. 75 (2022) 301–309.
30. [30]
  G. Hou, X. Ma, Q. Sun, et al., ACS Appl. Mater. 10 (2018) 18610–18618. doi: 10.1021/acsami.8b01003
31. [31]
  R. Zhao, L. Gao, M. Song, et al., ACS Energy Lett. 6 (2021) 3141–3150. doi: 10.1021/acsenergylett.1c01551
32. [32]
  P. Jiang, J. Cao, B. Wei, et al., Energy Stor. Mater. 48 (2022) 145–154.
33. [33]
  D. Dai, X. Zhou, P. Yan, et al., ACS Appl. Mater. Inter. 16 (2023) 2428–2437.
34. [34]
  C. Cui, C. Zeng, G. Huang, et al., Adv. Energy Mater. 12 (2022) 2202250.
35. [35]
  L. Zhai, K. Yang, F. Jiang, et al., J. Energy Chem. 79 (2023) 357–364.
36. [36]
  J. Liu, J. Cao, W. Liang, L. Yang, D. Wu, ACS Appl. Polym. 4 (2022) 4003–4012. doi: 10.1021/acsapm.2c00467
37. [37]
  S. Lee, S. Jung, S. Yang, et al., Appl. Surf. Sci. 586 (2022) 152790.
38. [38]
  Z. Gao, H. Sun, L. Fu, et al., Adv. Mater. 30 (2018) 1705702.
39. [39]
  W. Yan, Z. Mu, Z. Wang, et al., Nat. Energy 8 (2023) 800–813. doi: 10.1038/s41560-023-01279-8
40. [40]
  N. Ci, L. Zhang, J. Li, et al., Carbon 187 (2022) 13–21.
41. [41]
  P. Shi, T. Li, R. Zhang, et al., Adv. Mater. 31 (2019) 1807131.
42. [42]
  F. Hu, Y. Li, Y. Wei, et al., ACS Appl. Mater. Interfaces 12 (2020) 12793–12800. doi: 10.1021/acsami.9b21717
43. [43]
  L. He, Q. Sun, C. Chen, et al., ACS Appl. Mater. Interfaces 11 (2019) 20895–20904. doi: 10.1021/acsami.9b05516
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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

Engineering lithiophilic LiCx layer to robust interfacial chemistry between LAGP and Li anode for Li-metal batteries

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通讯作者: 陈斌, bchen63@163.com

Engineering lithiophilic LiC_x layer to robust interfacial chemistry between LAGP and Li anode for Li-metal batteries