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
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