Citation: Qiyue Luo, Chen Liu, Siwu Li, Chaochao Wei, Zhongkai Wu, Lin Li, Ziling Jiang, Liping Li, Guangshe Li, Shijie Cheng, Chuang Yu. Charge carrier distribution enabling superior electrochemical performance for all-solid-state lithium batteries over wide temperature range[J]. Chinese Chemical Letters, ;2026, 37(7): 111113. doi: 10.1016/j.cclet.2025.111113 shu

Charge carrier distribution enabling superior electrochemical performance for all-solid-state lithium batteries over wide temperature range

Qiyue Luo ^{a, b} ,
Chen Liu ^a ,
Siwu Li ^{c, *,} ,
Chaochao Wei ^{a, b} ,
Zhongkai Wu ^{a, b} ,
Lin Li ^{a, b} ,
Ziling Jiang ^{a, b} ,
Liping Li ^{d, *,} ,
Guangshe Li ^d ,
Shijie Cheng ^a ,
Chuang Yu ^{a, *,}

a.
State Key Laboratory of Advanced Electromagnetic Technology, School of Electrical and Electronic Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
b.
School of Chemistry and Chemical Engineering, Huazhong University of Science and Technology, Wuhan 430074, China
c.
Key Laboratory of Artificial Olfaction of Shaanxi Higher Education Institutes, the Academy of Advanced Interdisciplinary Research, Xidian University, Xi’an 710126, China
d.
State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun 130012, China

lisiwu@xidian.edu.cn

lipingli@jlu.edu.cn

cyu2020@hust.edu.cn

Received Date: 11 July 2024
Revised Date: 13 March 2025
Accepted Date: 18 March 2025
Available Online: 18 March 2025

Figures(4)

Argyrodite-based all-solid-state batteries exhibit significant potential as energy storage devices across a wide temperature zone. The Li-ion and electronic conductivities in the cathode mixture is crucial factor in determining the corresponding electrochemical performances. Here, an effective charge carrier distribution is tailored by introducing Li₃InCl₆ electrolyte with wider voltage stability surrounding the bare LiNi_0.7Co_0.2Mn_0.1O₂ to promote ionic conductivity and mixing carbon additives to enhance electronic conductivity. The Li₃InCl₆@LiNi_0.7Co_0.2Mn_0.1O₂/Li_5.5PS_4.5Cl_1.5/Li-In battery exhibits superior electrochemical performance at various C-rates over a wide operating temperature range due to the enhanced charge carrier conducting rates. It delivers high charge/discharge capacities, superior rate capability and exceptional cycling performance. Specifically, the battery delivers initial discharge capacities of 202 mAh/g at 0.2 C and retains a discharge capacity of 162 mAh/g at 2 C with a capacity retention of 91.8% over 500 cycles when cycled at room temperature. Moreover, due to the Li₃InCl₆ coating layer and the carbon additive in the cathode, it exhibits higher discharge capacities and superior cycling performances when operated at -20 and 60 ℃. This work presents a guideline for fabricating high-performance all-climate solid-state lithium batteries via tailoring the charger carriers conducting pathway in the electrode structure.
- Li_5.5PS_4.5Cl_1.5 electrolyte,
- Charge carriers,
- Li₃InCl₆ coating,
- Electronic conductivity,
- Electrochemical performances
1. [1]
  C. Yu, F. Zhao, J. Luo, L. Zhang, X. Sun, Nano Energy 83 (2021) 105858. doi: 10.1016/j.nanoen.2021.105858
2. [2]
  C. Yu, S. Ganapathy, E. Eck, et al., Nat. Commun. 8 (2017) 1086. doi: 10.1038/s41467-017-01187-y
3. [3]
  C. Yu, S. Ganapathy, N.J. de Klerk, et al., J. Am. Chem. Soc. 138 (2016) 11192–11201. doi: 10.1021/jacs.6b05066
4. [4]
  S. Chen, C. Yu, C. Wei, et al., Energy Mater. Adv. 4 (2023) 0019. doi: 10.34133/energymatadv.0019
5. [5]
  J. Wu, L. Shen, Z. Zhang, et al., Electrochem. Energy Rev. 4 (2021) 101–135. doi: 10.1007/s41918-020-00081-4
6. [6]
  Z. Jiang, C. Liu, J. Yang, et al., Chin. Chem. Lett. 36 (2025) 109741. doi: 10.1016/j.cclet.2024.109741
7. [7]
  C. Wei, R. Wang, Z. Wu, et al., Chem. Eng. J. 476 (2023) 146531. doi: 10.1016/j.cej.2023.146531
8. [8]
  Z. Wu, S. Chen, C. Yu, et al., Chem. Eng. J. 442 (2022) 136346. doi: 10.1016/j.cej.2022.136346
9. [9]
  Q. Luo, L. Ming, D. Zhang, et al., Energy Mater. Adv. 4 (2023) 0065. doi: 10.34133/energymatadv.0065
10. [10]
  Q. Luo, C. Yu, C. Wei, et al., Ceram. Int. 49 (2023) 11485–11493. doi: 10.1016/j.ceramint.2022.11.347
11. [11]
  Z. Jiang, S. Chen, C. Wei, et al., Chin. Chem. Lett. 35 (2024) 108561. doi: 10.1016/j.cclet.2023.108561
12. [12]
  C. Wei, C. Yu, R. Wang, et al., J. Power Sources 559 (2023) 232659. doi: 10.1016/j.jpowsour.2023.232659
13. [13]
  C. Wei, X. Liu, C. Yu, et al., Chin. Chem. Lett. 34 (2023) 107859. doi: 10.1016/j.cclet.2022.107859
14. [14]
  Z. Wu, C. Yu, C. Wei, et al., Chem. Eng. J. 466 (2023) 143304. doi: 10.1016/j.cej.2023.143304
15. [15]
  L. Li, R. Xu, L. Zhang, et al., Adv. Funct. Mater. 32 (2022) 2203095. doi: 10.1002/adfm.202203095
16. [16]
  L. Li, J. Yao, R. Xu, et al., Energy Storage Mater. 63 (2023) 103016. doi: 10.1016/j.ensm.2023.103016
17. [17]
  C. Wei, D. Yu, X. Xu, et al., Chem. Asian J. 18 (2023) e202300376. doi: 10.1002/asia.202300376
18. [18]
  J. Wu, S. Liu, F. Han, X. Yao, C. Wang, Adv. Mater. 33 (2021) 2000751. doi: 10.1002/adma.202000751
19. [19]
  W. Weng, D. Zhou, G. Liu, et al., Mater. Futures 1 (2022) 021001. doi: 10.1088/2752-5724/ac66f5
20. [20]
  S. Lou, F. Zhang, C. Fu, et al., Adv. Mater. 33 (2021) e2000721. doi: 10.1002/adma.202000721
21. [21]
  S. Lou, Z. Yu, Q. Liu, et al., Chem 6 (2020) 2199–2218. doi: 10.1016/j.chempr.2020.06.030
22. [22]
  R. Song, J. Yao, R. Xu, et al., Adv. Energy Mater. 13 (2023) 2203631. doi: 10.1002/aenm.202203631
23. [23]
  Z. Zhang, J. Yao, C. Yu, et al., J. Mater. Chem. A 10 (2022) 22155–22165. doi: 10.1039/d2ta03168j
24. [24]
  L. Peng, H. Ren, J. Zhang, et al., Energy Storage Mater. 43 (2021) 53–61. doi: 10.1016/j.ensm.2021.08.028
25. [25]
  Y. Seino, T. Ota, K. Takada, J. Power Sources 196 (2011) 6488–6492. doi: 10.1016/j.jpowsour.2011.03.090
26. [26]
  C. Liao, C. Yu, S. Chen, et al., Renewables 1 (2023) 266–276. doi: 10.31635/renewables.023.202200021
27. [27]
  L. Ming, D. Liu, Q. Luo, et al., Chin. Chem. Lett. 35 (2024) 109387. doi: 10.1016/j.cclet.2023.109387
28. [28]
  L. Hu, J. Wang, K. Wang, et al., Nat. Commun. 14 (2023) 3807. doi: 10.1038/s41467-023-39522-1
29. [29]
  T. Asano, A. Sakai, S. Ouchi, et al., Adv. Mater. 30 (2018) 1803075. doi: 10.1002/adma.201803075
30. [30]
  X. Li, J. Liang, N. Chen, et al., Angew. Chem. Int. Ed. 58 (2019) 16427–16432. doi: 10.1002/anie.201909805
31. [31]
  X. Li, J. Liang, J. Luo, et al., Energy Environ. Sci. 12 (2019) 2665–2671. doi: 10.1039/c9ee02311a
32. [32]
  W. Li, J.A. Quirk, M. Li, et al., Adv. Mater. 36 (2024) 2302647. doi: 10.1002/adma.202302647
33. [33]
  S. Deng, M. Jiang, N. Chen, et al., Adv. Funct. Mater. 32 (2022) 2205594. doi: 10.1002/adfm.202205594
34. [34]
  Q. Luo, C. Liu, C. Wei, et al., J. Power Sources 608 (2024) 234616. doi: 10.1016/j.jpowsour.2024.234616
35. [35]
  L. Zhou, T.T. Zuo, C.Y. Kwok, et al., Nat. Energy 7 (2022) 83–93. doi: 10.1038/s41560-021-00952-0
36. [36]
  L. Zhou, C.Y. Kwok, A. Shyamsunder, et al., Energy Environ. Sci. 13 (2020) 2056–2063. doi: 10.1039/d0ee01017k
37. [37]
  K. Wang, Q. Ren, Z. Gu, et al., Nat. Commun. 12 (2021) 4410. doi: 10.1038/s41467-021-24697-2
38. [38]
  L. Zhou, T. Zuo, C. Li, et al., ACS Energy Lett. 8 (2023) 3102–3111. doi: 10.1021/acsenergylett.3c00763
39. [39]
  C. Rosenbach, F. Walther, J. Ruhl, et al., Adv. Energy Mater. 13 (2022) 2203673.
40. [40]
  T. Koç, M. Hallot, E. Quemin, et al., ACS Energy Lett. 7 (2022) 2979–2987. doi: 10.1021/acsenergylett.2c01668
41. [41]
  M. Bianchini, M. Roca-Ayats, P. Hartmann, T. Brezesinski, J. Janek, Angew Chem. Int. Ed. 58 (2019) 10434–10458. doi: 10.1002/anie.201812472
42. [42]
  F. Wu, Q. Li, L. Chen, et al., ACS Appl Mater Interfaces 11 (2019) 36751– 36762. doi: 10.1021/acsami.9b12595
43. [43]
  T. Koç, F. Marchini, G. Rousse, R. Dugas, J.M. Tarascon, ACS Appl. Energy Mater. 4 (2021) 13575–13585. doi: 10.1021/acsaem.1c02187
44. [44]
  R. Koerver, I. Aygün, T. Leichtweiß, et al., Chem. Mat. 29 (2017) 5574–5582. doi: 10.1021/acs.chemmater.7b00931
45. [45]
  Z. Zhang, W. Jia, Y. Feng, et al., Energy Environ. Sci. 16 (2023) 4453–4463. doi: 10.1039/d3ee01551c
46. [46]
  T.A. Hendriks, M.A. Lange, E.M. Kiens, C. Baeumer, W.G. Zeier, Batteries Supercaps 6 (2023) e202200544. doi: 10.1002/batt.202200544
47. [47]
  W. Jiang, X. Zhu, R. Huang, et al., Adv. Energy Mater. 12 (2022) 2103473. doi: 10.1002/aenm.202103473
48. [48]
  L. Peng, C. Yu, Z. Zhang, et al., Chem. Eng. J. 430 (2022) 132896. doi: 10.1016/j.cej.2021.132896
49. [49]
  C. Liao, C. Yu, X. Miao, et al., Materialia 26 (2022) 101603. doi: 10.1016/j.mtla.2022.101603
50. [50]
  L. Peng, S. Chen, C. Yu, et al., J. Power Sources 520 (2022) 230890. doi: 10.1016/j.jpowsour.2021.230890
51. [51]
  T. Ma, Z. Wang, D. Wu, et al., Energy Environ. Sci. 16 (2023) 2142–2152. doi: 10.1039/d3ee00420a
52. [52]
  W. Mao, G. Ai, Y. Dai, et al., J. Power Sources 310 (2016) 54–60. doi: 10.1016/j.jpowsour.2016.02.002
53. [53]
  C. Wang, J. Liang, S. Hwang, et al., Nano Energy 72 (2020) 104686. doi: 10.1016/j.nanoen.2020.104686
54. [54]
  J.S. Horner, G. Whang, D.S. Ashby, et al., ACS Appl. Energy Mater. 4 (2021) 11460–11469. doi: 10.1021/acsaem.1c02218
1. [1]
  Ziling Jiang , Shaoqing Chen , Chaochao Wei , Ziqi Zhang , Zhongkai Wu , Qiyue Luo , Liang Ming , Long Zhang , Chuang Yu . Enabling superior electrochemical performance of NCA cathode in Li_5.5PS_4.5Cl_1.5-based solid-state batteries with a dual-electrolyte layer. Chinese Chemical Letters, 2024, 35(4): 108561-. doi: 10.1016/j.cclet.2023.108561
2. [2]
  Chaochao Wei , Ru Wang , Zhongkai Wu , Qiyue Luo , Ziling Jiang , Liang Ming , Jie Yang , Liping Wang , Chuang Yu . Revealing the size effect of FeS₂ on solid-state battery performances at different operating temperatures. Chinese Chemical Letters, 2024, 35(6): 108717-. doi: 10.1016/j.cclet.2023.108717
3. [3]
  Linfeng Peng , Cong Liao , Jiayue Peng , Shuai Chen , Tianyu Lei , Shijie Cheng , Jia Xie . Effect of oxygen doping sources on enhancing air stability and lithium metal compatibility of Li_5.5PS_4.5Cl_1.5 electrolyte. Chinese Chemical Letters, 2026, 37(6): 111015-. doi: 10.1016/j.cclet.2025.111015
4. [4]
  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. Chinese Chemical Letters, 2026, 37(6): 111040-. doi: 10.1016/j.cclet.2025.111040
5. [5]
  Ziling Jiang , Chen Liu , Jie Yang , Xia Li , Chaochao Wei , Qiyue Luo , Zhongkai Wu , Lin Li , Liping Li , Shijie Cheng , Chuang Yu . Designing F-doped Li₃InCl₆ electrolyte with enhanced stability for all-solid-state lithium batteries in a wide voltage window. Chinese Chemical Letters, 2025, 36(6): 109741-. doi: 10.1016/j.cclet.2024.109741
6. [6]
  Jie Chen , Hannan Chen , Bingbing Tian . Enhancing moisture and electrochemical stability of the Li_5.7PS_4.7Cl_1.3 electrolyte by boron nitride coating for all-solid-state lithium metal batteries. Chinese Chemical Letters, 2025, 36(7): 109775-. doi: 10.1016/j.cclet.2024.109775
7. [7]
  Liang Ming , Dan Liu , Qiyue Luo , Chaochao Wei , Chen Liu , Ziling Jiang , Zhongkai Wu , Lin Li , Long Zhang , Shijie Cheng , Chuang Yu . Si-doped Li₆PS₅I with enhanced conductivity enables superior performance for all-solid-state lithium batteries. Chinese Chemical Letters, 2024, 35(10): 109387-. doi: 10.1016/j.cclet.2023.109387
8. [8]
  Jinrui Qian , Yue Sun , Feixiang Long , Yiqing Liu , Guozhen Chang , Yuzhu Song , Naike Shi , Andrea Sanson , Xiuzhu Han , Chang Zhou , Jun Chen . Significantly improving the performances of thermal conductivity and thermal expansion in aluminum matrix composites through a multiphase design strategy. Chinese Chemical Letters, 2026, 37(7): 111849-. doi: 10.1016/j.cclet.2025.111849
9. [9]
  Qiang Zhang , Weiran Gong , Huinan Che , Bin Liu , Yanhui Ao . S doping induces to promoted spatial separation of charge carriers on carbon nitride for efficiently photocatalytic degradation of atrazine. Chinese Journal of Structural Chemistry, 2023, 42(12): 100205-100205. doi: 10.1016/j.cjsc.2023.100205
10. [10]
  Saadullah Khattak , Hong-Tao Xu , Jianliang Shen . Bio-electronic bandage: Self-powered performances to accelerate intestinal wound healing. Chinese Chemical Letters, 2024, 35(12): 110210-. doi: 10.1016/j.cclet.2024.110210
11. [11]
  Mingjiao Lu , Zhixing Wang , Gui Luo , Huajun Guo , Xinhai Li , Guochun Yan , Qihou Li , Xianglin Li , Ding Wang , Jiexi Wang . Boosting the performance of LiNi_0.90Co_0.06Mn_0.04O₂ electrode by uniform Li₃PO₄ coating via atomic layer deposition. Chinese Chemical Letters, 2024, 35(5): 108638-. doi: 10.1016/j.cclet.2023.108638
12. [12]
  Fengyu Zhang , Yali Liang , Zhangran Ye , Lei Deng , Yunna Guo , Ping Qiu , Peng Jia , Qiaobao Zhang , Liqiang Zhang . Enhanced electrochemical performance of nanoscale single crystal NMC811 modification by coating LiNbO₃. Chinese Chemical Letters, 2024, 35(5): 108655-. doi: 10.1016/j.cclet.2023.108655
13. [13]
  Hanqing Zhang , Xiaoxia Wang , Chen Chen , Xianfeng Yang , Chungli Dong , Yucheng Huang , Xiaoliang Zhao , Dongjiang Yang . Selective CO2-to-formic acid electrochemical conversion by modulating electronic environment of copper phthalocyanine with defective graphene. Chinese Journal of Structural Chemistry, 2023, 42(10): 100089-100089. doi: 10.1016/j.cjsc.2023.100089
14. [14]
  Chunxuan Chen , Wanyuan Li , Chengyu Ni , Wubin Dai . Manganese valence modulation in ZnGa2O4 via simultaneously localized charge accumulation and oxygen vacancy engineering controlled by Li+ and F- substitutions for tailored applications. Chinese Journal of Structural Chemistry, 2026, 45(5): 100868-100868. doi: 10.1016/j.cjsc.2026.100868
15. [15]
  Kunyao Peng , Xianbin Wang , Xingbin Yan . Converting LiNO₃ additive to single nitrogenous component Li₂N₂O₂ SEI layer on Li metal anode in carbonate-based electrolyte. Chinese Chemical Letters, 2024, 35(9): 109274-. doi: 10.1016/j.cclet.2023.109274
16. [16]
  Weizhong LING , Jingyi LIN , Jianglin ZHU , Yuyi LIANG , Shanshan DAI , Yu LI . Syntheses, structures, and catalytic performances of complexes with 4,4′-dihydroxy-[1,1′-biphenyl]-3,3′-dicarboxylic acid ligands. Chinese Journal of Inorganic Chemistry, 2026, 42(1): 152-160. doi: 10.11862/CJIC.20250204
17. [17]
  Ruizhi Yang , Xia Li , Weiping Guo , Zixuan Chen , Hongwei Ming , Zhong-Zhen Luo , Zhigang Zou . New thermoelectric semiconductors Pb5Sb12+xBi6-xSe32 with ultralow thermal conductivity. Chinese Journal of Structural Chemistry, 2024, 43(3): 100268-100268. doi: 10.1016/j.cjsc.2024.100268
18. [18]
  Ying Li , Yanjun Xu , Xingqi Han , Di Han , Xuesong Wu , Xinlong Wang , Zhongmin Su . A new metal–organic rotaxane framework for enhanced ion conductivity of solid-state electrolyte in lithium-metal batteries. Chinese Chemical Letters, 2024, 35(9): 109189-. doi: 10.1016/j.cclet.2023.109189
19. [19]
  Jingyu Shi , Xiaofeng Wu , Yutong Chen , Yi Zhang , Xiangyan Hou , Ruike Lv , Junwei Liu , Mengpei Jiang , Keke Huang , Shouhua Feng . Structure factors dictate the ionic conductivity and chemical stability for cubic garnet-based solid-state electrolyte. Chinese Chemical Letters, 2025, 36(5): 109938-. doi: 10.1016/j.cclet.2024.109938
20. [20]
  Yupeng TANG , Haiying YANG , Fan JIN , Nan LI . Hydrogen storage properties of C₆S₆Li₆: A density functional theory study. Chinese Journal of Inorganic Chemistry, 2025, 41(9): 1827-1839. doi: 10.11862/CJIC.20240460

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(16)
HTML views(0)

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