Citation: Haowen Li, Hongying Hou, Dai-Huo Liu, Bao Li, Dongmei Dai, Bao Wang, Mengmin Jia, Zhuangzhuang Zhang, Liang Wang, Yaru Qiao, Canhui Wu, Huihui Zhu, Pengyao Yan. A designed flexible solid-state electrolyte with rich hydrogen-bonded networks from TPU-PEGDA/LLZTO for Li metal batteries[J]. Chinese Chemical Letters, ;2026, 37(2): 111020. doi: 10.1016/j.cclet.2025.111020 shu

A designed flexible solid-state electrolyte with rich hydrogen-bonded networks from TPU-PEGDA/LLZTO for Li metal batteries

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

a.
Faculty of Material Science and Engineering, Kunming University of Science and Technology, Kunming 650093, China
b.
Collaborative Innovation Center of Henan Province for Green Manufacturing of Fine Chemicals, School of Chemistry and Chemical Engineering, Key Laboratory of Green Chemical Media and Reactions (Ministry of Education), Henan Normal University, Xinxiang 453007, China
c.
CAS Henan Industrial Technology Innovation & Incubation Center, Zhengzhou 450000, China
d.
State Key Laboratory of Biochemical Engineering, Institute of Process Engineering, Chinese Academy of Sciences, Beijing 100190, China

hongyinghou@kust.edu.cn

liudaihuo@htu.edu.cn

libao@htu.edu.cn

Received Date: 11 January 2025
Revised Date: 17 February 2025
Accepted Date: 27 February 2025
Available Online: 1 March 2025

Figures(7)

Thermoplastic polyurethane (TPU) consists of a hard segment and a soft segment, where the former affords mechanical strength and thermal stability, while the latter provides a possibility of good ionic conductivity by promoting dissociation of ions from the lithium salt. Thus, TPU attracts a wide interest recently as a promising polymer electrolyte for solid-state lithium batteries. However, the relatively low ionic conductivity of TPU still restricts its actual applications due to the aggregation of polymer chains, which greatly reduces the dissociation of lithium salts. Herein, a strategy to address this challenge was adopted by in situ polymerization poly(ethylene glycol diacrylate) (PEGDA) in fully dispersed TPU. Hence a stretchable solid-state electrolyte (denoted as TELL and the contrast sample was denoted as TLL) with high ionic conductivity of 7.18 × 10⁻⁴ S/cm was obtained at room temperature. The Li⁺ transference number is 0.85 in Li|TELL|Li cell and can stably undergo charge-discharge cycles for 1400 h at a current density of 0.1 mA/cm², while the contrast sample is short-circuited after 634 h of cycling. The LiFePO₄|TELL|Li cell achieves a capacity retention of 78.93% after 200 cycles at 2 C. The LiFePO₄|TLL|Li cell only gains the capacity retention of 51.9% after 50 cycles at the same current density. So, the method adopted here may provide a new approach to realize a flexible solid-state electrolyte with high ion-conductivity.
- Poly(ethylene glycol diacrylate),
- Thermoplastic,
- Hydrogen-bonded network,
- High ion-conductivity,
- Solid-state lithium batteries
1. [1]
  W.D. Li, E.M. Erickson, A. Manthiram, Nat. Energy 5 (2020) 26–34. doi: 10.1038/s41560-019-0513-0
2. [2]
  W. Jia, J. Zhang, L. Zheng, et al., eScience 4 (2024) 100266. doi: 10.1016/j.esci.2024.100266
3. [3]
  J.X. Wang, J. Ma, Z.F. Zhuang, et al., Chem. Rev. 124 (2024) 2839–2887. doi: 10.1021/acs.chemrev.3c00884
4. [4]
  Z.Z. Dong, J.H. Zhang, L. Zhu, et al., Chin. Chem. Lett. 36 (2025) 109773. doi: 10.1016/j.cclet.2024.109773
5. [5]
  D.H. Liu, Z. Bai, M. Li, et al., Chem. Soc. Rev. 15 (2020) 5407–5445. doi: 10.1039/c9cs00636b
6. [6]
  J. Yang, X. Zhang, M. Hou, et al., Carbon Neutral. 4 (2025) e188.
7. [7]
  H. Hou, Y. Wang, X. Liu, et al., J. Energy Storage 89 (2024) 111737. doi: 10.1016/j.est.2024.111737
8. [8]
  H. Hou, B. Huang, X. Yu, et al., J. Energy Storage 68 (2023) 107680. doi: 10.1016/j.est.2023.107680
9. [9]
  A. Kwade, W. Haselrieder, R. Leithoff, et al., Nat. Energy 3 (2018) 290–300. doi: 10.1038/s41560-018-0130-3
10. [10]
  Z. Luo, Y. Cao, G. Xu, et al., Carbon Neutral. 3 (2024) 647–672. doi: 10.1002/cnl2.147
11. [11]
  A. Manthiram, X.W. Yu, S.F. Wang, Nat. Rev. Mater. 2 (2017) 16103. doi: 10.1038/natrevmats.2016.103
12. [12]
  D. Sui, J. Liu, Chin. Chem. Lett. 36 (2025) 110417. doi: 10.1016/j.cclet.2024.110417
13. [13]
  X.W. Yu, A. Manthiram, Energy Environ. Sci. 11 (2018) 527–543. doi: 10.1039/c7ee02555f
14. [14]
  C. Sun, J. Liu, Y. Gong, et al., Nano Energy 33 (2017) 363–386. doi: 10.1016/j.nanoen.2017.01.028
15. [15]
  M. Forsyth, L. Porcarelli, X. Wang, et al., Acc. Chem. Res. 52 (2019) 686–694. doi: 10.1021/acs.accounts.8b00566
16. [16]
  V. Thangadurai, S. Narayanan, D. Pinzaru, Chem. Soc. Rev. 43 (2014) 4714–4727. doi: 10.1039/c4cs00020j
17. [17]
  R.S. Chen, Q.H. Li, X.Q. Yu, et al., Chem. Rev. 120 (2020) 6820–6877. doi: 10.1021/acs.chemrev.9b00268
18. [18]
  S.F. Wang, H.H. Xu, W.D. Li, et al., J. Am. Chem. Soc. 140 (2018) 250–257. doi: 10.1021/jacs.7b09531
19. [19]
  L.Z. Long, S.J. Wang, M. Xiao, et al., J. Mater. Chem. A 4 (2016) 10038–10069. doi: 10.1039/C6TA02621D
20. [20]
  K.S. Ngai, S. Ramesh, K. Ramesh, et al., Ionics 22 (2016) 1259–1279 (Kiel). doi: 10.1007/s11581-016-1756-4
21. [21]
  A.J. Li, X.B. Liao, H.R. Zhang, et al., Adv. Mater. 32 (2020) 1905517. doi: 10.1002/adma.201905517
22. [22]
  D. Dai, P. Yan, X. Zhou, et al., Green Carbon 2 (2024) 310–315. doi: 10.1016/j.greenca.2024.06.002
23. [23]
  W. Yu, N. Deng, Y. Feng, et al., eScience 5 (2025) 100278. doi: 10.1016/j.esci.2024.100278
24. [24]
  D. Dai, X. Zhou, P. Yan, et al., ACS Appl. Mater. Interfaces 16 (2023) 2428–2437.
25. [25]
  Y. Wang, C.J. Zanelotti, X. Wang, et al., Nat. Mater. 20 (2021) 1255–1263. doi: 10.1038/s41563-021-00995-4
26. [26]
  K. Ramanjaneyulu, N. Bar, M.S. Arif Sher Shah, et al., J. Power Sources 217 (2012) 29–36. doi: 10.1016/j.jpowsour.2012.05.075
27. [27]
  C. Tao, M.H. Gao, B.H. Yin, et al., Electrochim. Acta 257 (2017) 31–39. doi: 10.1016/j.electacta.2017.10.037
28. [28]
  J. Zou, J. Zhang, L. Wang, et al., Sci. China Mater. 67 (2024) 1445–1454. doi: 10.1007/s40843-024-2913-8
29. [29]
  X. An, Y. Kang, G. Li, Chem. Phys. 520 (2019) 100–107. doi: 10.1016/j.chemphys.2018.12.009
30. [30]
  L. Tabari, D. Farmanzadeh, Appl. Surf. Sci. 500 (2020) 144029. doi: 10.1016/j.apsusc.2019.144029
31. [31]
  H. Peng, T.R. Long, J. Peng, et al., Adv. Energy Mater. 14 (2024) 2400428. doi: 10.1002/aenm.202400428
32. [32]
  F. Gao, Q. Wang, X. Yang, Colloid Polym. Sci. 298 (2020) 303–312. doi: 10.1007/s00396-020-04606-7
33. [33]
  A.I. Boronin, S.V. Koscheev, G.M. Zhidomirov, J. Electron. Spectros. Relat. Phenom. (1998) 43–51.
1. [1]
  Xiaofei Wang , Shuonan Wang , Zhangkuo Han , Jiahan Zheng , Yu Chen , Libing Liao , Hao Liu . Shear-engineered flower-like spherulites enable record ionic conductivity of PEO-based electrolytes for solid-state lithium batteries. Chinese Chemical Letters, 2026, 37(2): 111434-. doi: 10.1016/j.cclet.2025.111434
2. [2]
  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
3. [3]
  Xin Li , Ling Zhang , Yunyan Fan , Shaojing Lin , Yong Lin , Yongsheng Ying , Meijiao Hu , Haiying Gao , Xianri Xu , Zhongbiao Xia , Xinchuan Lin , Junjie Lu , Xiang Han . Carbon interconnected microsized Si film toward high energy room temperature solid-state lithium-ion batteries. Chinese Chemical Letters, 2025, 36(2): 109776-. doi: 10.1016/j.cclet.2024.109776
4. [4]
  Qiao Wang , Ziling Jiang , Chuang Yu , Liping Li , Guangshe Li . Research progress of inorganic sodium ion conductors for solid-state batteries. Chinese Chemical Letters, 2025, 36(6): 110006-. doi: 10.1016/j.cclet.2024.110006
5. [5]
  Sheng Zhao , Junjie Lu , Bifu Sheng , Siying Zhang , Hao Li , Jizhang Chen , Xiang Han . High-performance room temperature solid-state lithium battery enabled by PP-PVDF multilayer composite electrolyte. Chinese Chemical Letters, 2025, 36(6): 110008-. doi: 10.1016/j.cclet.2024.110008
6. [6]
  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
7. [7]
  Ya Song , Mingxia Zhou , Zhu Chen , Huali Nie , Jiao-Jing Shao , Guangmin Zhou . Integrated interconnected porous and lamellar structures realized fast ion/electron conductivity in high-performance lithium-sulfur batteries. Chinese Chemical Letters, 2024, 35(6): 109200-. doi: 10.1016/j.cclet.2023.109200
8. [8]
  Zhangran Ye , Zhixuan Yu , Jingming Yao , Lei Deng , Yunna Guo , Hantao Cui , Chongchong Ma , Chao Tai , Liqiang Zhang , Lingyun Zhu , Peng Jia . An ionically conductive and compressible sulfochloride solid-state electrolyte for stable all-solid-state lithium-based batteries. Chinese Chemical Letters, 2025, 36(8): 110272-. doi: 10.1016/j.cclet.2024.110272
9. [9]
  Qianqian Song , Yunting Zhang , Jianli Liang , Si Liu , Jian Zhu , Xingbin Yan . Boron nitride nanofibers enhanced composite PEO-based solid-state polymer electrolytes for lithium metal batteries. Chinese Chemical Letters, 2024, 35(6): 108797-. doi: 10.1016/j.cclet.2023.108797
10. [10]
  Yang Deng , Yitao Ouyang , Chao Han . Constriction-susceptible makes fast cycling of lithium metal in solid-state batteries: Silicon as an example. Chinese Journal of Structural Chemistry, 2024, 43(7): 100276-100276. doi: 10.1016/j.cjsc.2024.100276
11. [11]
  Hong-Li Long , Hong-Jie Peng . Lithium-bond chemistry enlightens 600 Wh/kg solid-state batteries. Chinese Chemical Letters, 2026, 37(2): 112045-. doi: 10.1016/j.cclet.2025.112045
12. [12]
  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
13. [13]
  Zhong-Hui Sun , Yu-Qi Zhang , Zhen-Yi Gu , Dong-Yang Qu , Hong-Yu Guan , Xing-Long Wu . CoPSe nanoparticles confined in nitrogen-doped dual carbon network towards high-performance lithium/potassium ion batteries. Chinese Chemical Letters, 2025, 36(1): 109590-. doi: 10.1016/j.cclet.2024.109590
14. [14]
  Jing Guo . Stacking solid-state electrolyte and aluminum pellets for anode-free solid-state batteries. Chinese Chemical Letters, 2025, 36(5): 110764-. doi: 10.1016/j.cclet.2024.110764
15. [15]
  Tianyi Hou , Yunhui Huang , Henghui Xu . Interfacial engineering for advanced solid-state Li-metal batteries. Chinese Journal of Structural Chemistry, 2024, 43(7): 100313-100313. doi: 10.1016/j.cjsc.2024.100313
16. [16]
  Peining Zhu , Xi Guo , Qinqin Yu , Zuyong Wang , Xiangxiao Lei , Zhiwei Zhu , Juan Du , Xiaojia Zhang , Yuan-Li Ding . Design strategies of Si-based anode for solid-state batteries. Chinese Chemical Letters, 2025, 36(9): 111383-. doi: 10.1016/j.cclet.2025.111383
17. [17]
  Longhao Hu , Lingshan Gong , Wenlong Ye , Hao Chen , Xiao-Li Lai , Yingxiang Ye . Luminescent hydrogen-bonded organic frameworks: From design to applications. Chinese Journal of Structural Chemistry, 2025, 44(11): 100703-100703. doi: 10.1016/j.cjsc.2025.100703
18. [18]
  Shuai Li , Liuting Zhang , Fuying Wu , Yiqun Jiang , Xuebin Yu . Efficient catalysis of FeNiCu-based multi-site alloys on magnesium-hydride for solid-state hydrogen storage. Chinese Chemical Letters, 2025, 36(1): 109566-. doi: 10.1016/j.cclet.2024.109566
19. [19]
  Linhui Liu , Wuwan Xiong , Mingli Fu , Junliang Wu , Zhenguo Li , Daiqi Ye , Peirong Chen . Efficient NO_x abatement by passive adsorption over a Pd-SAPO-34 catalyst prepared by solid-state ion exchange. Chinese Chemical Letters, 2024, 35(4): 108870-. doi: 10.1016/j.cclet.2023.108870
20. [20]
  Xiaoxiao Huang , Zhi-Long He , Yangpeng Chen , Lei Li , Zhenyu Yang , Chunyang Zhai , Mingshan Zhu . Novel P-doping-tuned Pd nanoflowers/S,N-GQDs photo-electrocatalyst for high-efficient ethylene glycol oxidation. Chinese Chemical Letters, 2024, 35(6): 109271-. doi: 10.1016/j.cclet.2023.109271

Get Citation

PDF

XML

Metrics

PDF Downloads(0)
Abstract views(11)
HTML views(1)

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