Citation: Haoran Du, Shanjie Zhang, Qing Ban, Kunhong Hu, Wenjuan Yang, Yi Zhao, Xinfeng Zhang, Qiankun Chen, Wei Yang, Xin Liang, Long Qie. Anion-driven polarity reconstruction of electrolyte microenvironment enables long-life zinc-metal batteries at low temperatures[J]. Chinese Chemical Letters, ;2026, 37(11): 112654. doi: 10.1016/j.cclet.2026.112654 shu

Anion-driven polarity reconstruction of electrolyte microenvironment enables long-life zinc-metal batteries at low temperatures

Haoran Du ^a ,
Shanjie Zhang ^a ,
Qing Ban ^a ,
Kunhong Hu ^a ,
Wenjuan Yang ^a ,
Yi Zhao ^a ,
Xinfeng Zhang ^a ,
Qiankun Chen ^a ,
Wei Yang ^{a, b} ,
Xin Liang ^{a, *,} ,
Long Qie ^{c, *,}

a.
Key Laboratory of Materials and Technologies for Advanced Batteries, School of Energy Materials and Chemical Engineering, Hefei University, Hefei 230601, China
b.
Anhui Provincial Key Laboratory of Urban Rail Transit Safety and Emergency Management, Hefei University, Hefei 230601, China
c.
State Key Laboratory of Material Processing and Die & Mold Technology, School of Materials Science and Engineering, Huazhong University of Science and Technology, Wuhan 430074, China

x.liang@hfuu.edu.cn

qie@hust.edu.cn

Received Date: 3 December 2025
Revised Date: 13 March 2026
Accepted Date: 19 March 2026
Available Online: 20 March 2026

Figures(5)

The high freezing point (T_f) of aqueous electrolytes, stemming from strong H-bonds of water, severely restricts the application of rechargeable zinc-metal batteries (RZMBs) in cold regions. Organic co-solvents can disrupt the H-bond network of water, reducing the T_f of aqueous electrolytes. However, limited by the polarity matching principle, most low-T_f organic molecules are excluded from the range of co-solvents due to their inability to dissociate zinc salts and immiscibility with water. Herein, we propose an anion-driven strategy for reconstructing the polarity of the electrolyte microenvironment. Relying on the “bridging” effect of the amphiphilic trifluoromethanesulfonate (OTf⁻), the weakly polar 2-methyltetrahydrofuran (2-MeTHF) is successfully induced into the strongly polar electrolytes, endowing the optimized electrolyte with a dramatically reduced T_f of −112.1 °C. Moreover, this strategy enables long-term stability in ZnZn cells and full cells operated at −30 °C, broadening the selection of antifreeze co-solvents and offering insights into cold-region energy storage devices.
- Co-solvents,
- Dendrite-free,
- Amphiphilic anion,
- Micelles,
- Solvation
1. [1]
  J. Xu, J. Zhang, T.P. Pollard, et al., Nature 614 (2023) 694–700. doi: 10.1038/s41586-022-05627-8
2. [2]
  Z. Xing, P. Ye, X. Shi, et al., Angew. Chem. Int. Ed. 64 (2025) e202516974. doi: 10.1002/anie.202516974
3. [3]
  J. Cong, Y. Wang, X. Lin, et al., J. Am. Chem. Soc. 147 (2025) 8607–8617. doi: 10.1021/jacs.4c16880
4. [4]
  M. Qiu, P. Sun, K. Han, et al., Nat. Commun. 14 (2023) 601. doi: 10.1038/s41467-023-36198-5
5. [5]
  H. Du, X. Qi, L. Qie, Y. Huang, Adv. Funct. Mater. 33 (2023) 2302546. doi: 10.1002/adfm.202302546
6. [6]
  Y. Dong, H. Hu, P. Liang, et al., Nat. Rev. Chem. 9 (2025) 102–117. doi: 10.1038/s41570-024-00670-7
7. [7]
  W. Liu, Q. Zhao, H. Qi, et al., Chin. Chem. Lett. 37 (2026) 110893. doi: 10.1016/j.cclet.2025.110893
8. [8]
  X. Yu, M. Chen, J. Wang, et al., Nat. Commun. 16 (2025) 3820. doi: 10.1038/s41467-025-59069-7
9. [9]
  S. Li, Y. Zhong, J. Huang, et al., Energy Environ. Sci. 18 (2025) 2599–2609. doi: 10.1039/d4ee04372c
10. [10]
  J. Ji, H. Du, Z. Zhu, et al., Angew. Chem. Int. Ed. 64 (2025) e202414562. doi: 10.1002/anie.202414562
11. [11]
  Y. Lv, Y. Xiao, L. Ma, C. Zhi, S. Chen, Adv. Mater. 34 (2022) 2106409. doi: 10.1002/adma.202106409
12. [12]
  X. Zhao, Q. Dou, B. Yang, et al., Chin. Chem. Lett. 37 (2026) 110952. doi: 10.1016/j.cclet.2025.110952
13. [13]
  X. Liu, X. Dong, H. Adenusi, Y. Wu, S. Passerini, Nat. Rev. Chem. 9 (2025) 415–426. doi: 10.1038/s41570-025-00714-6
14. [14]
  W.M. Haynes, CRC Handbook of Chemistry and Physics, 97th ed., CRC Press, Boca Raton, 2016.
15. [15]
  Y. Kang, F. Zhang, H. Li, et al., Energy Environ. Mater. 7 (2024) e12707. doi: 10.1002/eem2.12707
16. [16]
  M.A. Wiebe, J.E.T. Watson, C. Killeen, et al., Polym. Chem. 16 (2025) 1305–1312. doi: 10.1039/d4py01362j
17. [17]
  H. Ge, X. Feng, D. Liu, Y. Zhang, Nano Res. Energy 2 (2023) e9120039. doi: 10.26599/nre.2023.9120039
18. [18]
  H. Chen, P. Ruan, H. Zhang, et al., Angew. Chem. Int. Ed. 64 (2025) e202423999. doi: 10.1002/anie.202423999
19. [19]
  J. Durig, K. Kizer, J. Karriker, J. Raman Spectrosc. 1 (1973) 17–45. doi: 10.1002/jrs.1250010103
20. [20]
  L. Miao, R. Wang, S. Di, et al., ACS Nano 16 (2022) 9667–9678. doi: 10.1021/acsnano.2c02996
21. [21]
  H. Du, Y. Dong, Q. Li, et al., Adv. Mater. 35 (2023) 2210055. doi: 10.1002/adma.202210055
22. [22]
  R. Zhang, W.K. Pang, J. Vongsvivut, et al., Energy Environ. Sci. 17 (2024) 4569–4581. doi: 10.1039/d4ee00942h
23. [23]
  B. Kakoty, R. Vengarathody, S. Mukherji, et al., J. Mater. Chem. A 10 (2022) 12597–12607. doi: 10.1039/d2ta01501c
24. [24]
  C. Zhou, L. Shan, Z. Xing, et al., Adv. Mater. 38 (2026) e16045. doi: 10.1002/adma.202516045
25. [25]
  Y. Shen, P. Fu, J. Liu, et al., Nano Res. Energy 3 (2024) e9120115. doi: 10.26599/nre.2024.9120115
26. [26]
  H. Du, R. Zhao, Y. Yang, et al., Angew. Chem. Int. Ed. 61 (2022) e202114789. doi: 10.1002/anie.202114789
27. [27]
  C. Liu, Q. Li, Y. Lin, et al., Nano Res. Energy 2 (2023) e9120064. doi: 10.26599/nre.2023.9120064
28. [28]
  H. Du, R. Zhao, J. Ji, et al., Energy Storage Mater. 54 (2023) 461–468. doi: 10.1016/j.ensm.2022.10.060
29. [29]
  M. Li, X. Liu, J. Wu, et al., Adv. Energy Mater. 15 (2025) 2404037. doi: 10.1002/aenm.202404037
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