Citation: Juan Zeng. Anti-polyelectrolyte effect as a novel strategy to regulate the freezing point of zwitterionic hydrogels[J]. Chinese Chemical Letters, ;2026, 37(10): 112980. doi: 10.1016/j.cclet.2026.112980 shu

Anti-polyelectrolyte effect as a novel strategy to regulate the freezing point of zwitterionic hydrogels

Juan Zeng

College of Chemistry and Environmental Engineering, Wuhan Polytechnic University, Wuhan 430023, China

jzeng@whpu.edu.cn

Received Date: 24 March 2026
Revised Date: 20 May 2026
Accepted Date: 21 May 2026
Available Online: 21 May 2026

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Zwitterionic hydrogels as a new generation of functional materials are widely used in many frontier fields. However, zwitterionic hydrogels usually contain a large amount of active water and are inevitably frozen at low temperatures, thus sacrificing their mechanical properties and conductivity, which greatly limits their application. Herein, a novel strategy, namely the unique anti-polyelectrolyte effect (APE) of zwitterions is proposed to reduce the freezing point of zwitterionic hydrogels. The regulation mechanism of this strategy is that the electrostatic associated zwitterionic groups are exposed, thus increasing hydration by allowing these groups to establish strong hydrogen bonding with water molecules during the volume expansion process of zwitterionic polymer in salt. The overall water activity is decreased in the hydrogels, thus reducing the freezing point of the hydrogels. Sulfonic-based 2-(methacryloyloxy)ethyl dimethyl(3-sulfopropyl)-ammonium hydroxide (SBMA) and carboxylic-based 2-carboxy-N,N-dimethyl-N-(2′-methacryloyloxyethyl)ethanaminium inner salt (CBMA) zwitterionic monomers are selected as a proof of concept. SBMA based hydrogels with strong APE have a higher bound water content and a lower free water content than CBMA based hydrogels with almost no APE. Benefitting from the strong APE, the freezing point of SBMA based hydrogel (−20.9 ℃) is significantly lower than that of CBMA based hydrogel (−12.4 ℃). This work offers a practical and meaningful guidance for the design of anti-freezing zwitterionic hydrogels and further promotes the application of zwitterionic hydrogels in low temperature environments.
- Anti-polyelectrolyte effect,
- Zwitterionic hydrogel,
- Water activity,
- Freezing point,
- SBMA,
- CBMA
1. [1]
  L. Gao, A. Varley, H. Gao, et al., Langmuir 41 (2025) 3007–3026. doi: 10.1021/acs.langmuir.4c04788
2. [2]
  Z. Wang, X. Liu, M. Zhu, et al., J. Mater. Chem. A 13 (2025) 13693–13705. doi: 10.1039/d5ta01111f
3. [3]
  S. Moayedi, W. Xia, L. Lundergan, et al., Langmuir 40 (2024) 23125–23145. doi: 10.1021/acs.langmuir.4c02664
4. [4]
  Y. Sun, Y. Zhu, J. Si, et al., Chin. Chem. Lett. 36 (2025) 110012. doi: 10.1016/j.cclet.2024.110012
5. [5]
  S. Chen, R. Zhao, L. Dong, et al., Chin. Chem. Lett. 36 (2025) 111647. doi: 10.1016/j.cclet.2025.111647
6. [6]
  D. Gokhale, A.F. Hamelberg, P.S. Doyle, Nat. Water 2 (2024) 62–71. doi: 10.1038/s44221-023-00180-8
7. [7]
  K. Wu, X. Guo, J. Feng, et al., Gels 11 (2025) 587. doi: 10.3390/gels11080587
8. [8]
  B. Song, E. Zhang, Y. Shi, et al., ACS Appl. Mater. Interfaces 16 (2024) 27908–27916. doi: 10.1021/acsami.4c02574
9. [9]
  Y. Fu, X. Wang, S. Li, et al., Chin. Chem. Lett. 37 (2026) 111991. doi: 10.1016/j.cclet.2025.111991
10. [10]
  X. Zhou, B. Nie, R. Hu, et al., Chin. Chem. Lett. (2026), doi: 10.1016/j.cclet.2026.112547. doi: 10.1016/j.cclet.2026.112547
11. [11]
  J. Zheng, J. Liang, J. Xu, et al., Chem. Eng. J. 508 (2025) 161021. doi: 10.1016/j.cej.2025.161021
12. [12]
  X. Zou, L. Mei, Q. Liu, et al., ACS Appl. Polym. Mater. 7 (2025) 8065–8080. doi: 10.1021/acsapm.5c01145
13. [13]
  G. Wang, H. Ni, Y. Li, et al., Adv. Funct. Mater. 35 (2025) 2505048. doi: 10.1002/adfm.202505048
14. [14]
  J. Wang, Y. Huang, B. Liu, et al., Energy Storage Mater. 41 (2021) 599–605. doi: 10.1016/j.ensm.2021.06.034
15. [15]
  Q.J. Fu, S.W. Hao, X.R. Zhang, et al., Energy Environ. Sci. 16 (2023) 1291–1311. doi: 10.1039/d2ee03793a
16. [16]
  D. Han, Y. Cai, X. Wang, et al., Adv. Funct. Mater. 35 (2025) 2501362. doi: 10.1002/adfm.202501362
17. [17]
  Z.J. Chen, T.Y. Shen, M.H. Zhang, et al., Adv. Funct. Mater. 34 (2024) 2314864. doi: 10.1002/adfm.202314864
18. [18]
  X.P. Morelle, W.R. Illeperuma, K. Tian, et al., Adv. Mater. 30 (2018) 1801541. doi: 10.1002/adma.201801541
19. [19]
  R. Gao, J. Wang, Y. Song, et al., Adv. Funct. Mater. 36 (2025) e14585.
20. [20]
  L.X. Hou, H. Ju, X.P. Hao, et al., Adv. Mater. 35 (2023) 2300244. doi: 10.1002/adma.202300244
21. [21]
  S. Xiao, Y. Zhang, M. Shen, et al., Langmuir 34 (2018) 97–105. doi: 10.1021/acs.langmuir.7b03667
22. [22]
  M.G. Petroff, E.A. Garcia, M. Herrera-Alonso, et al., Langmuir 35 (2019) 4976–4985. doi: 10.1021/acs.langmuir.9b00218
23. [23]
  S. Hou, Y. Liu, J. Yan, et al., Macromol. Chem. Phys. 226 (2025) e00106. doi: 10.1002/macp.202500106
24. [24]
  K.T. Huang, K. Ishihara, C.J. Huang, Biomacromolecules 20 (2019) 3524–3534. doi: 10.1021/acs.biomac.9b00796
25. [25]
  J. Zeng, H. Chen, L. Dong, et al., Adv. Funct. Mater. 34 (2024) 2314651. doi: 10.1002/adfm.202314651
26. [26]
  W. Choi, S. Park, J.S. Kwon, et al., ACS Nano 15 (2021) 6811–6828. doi: 10.1021/acsnano.0c10431
27. [27]
  J. Zeng, H. Chen, L. Dong, et al., J. Colloid Interface Sci. 652 (2023) 856–865. doi: 10.1016/j.jcis.2023.08.037
28. [28]
  Y.N. Chou, M.Z. Ou, ACS Appl. Polym. Mater. 5 (2023) 5411–5428. doi: 10.1021/acsapm.3c00762
29. [29]
  R. Lalani, L. Liu, Polymer 52 (2011) 5344–5354. doi: 10.1016/j.polymer.2011.09.015
30. [30]
  K. Sivashanmugan, P.C. Liu, K.W. Tsai, et al., Nanoscale 9 (2017) 2865–2874. doi: 10.1039/C6NR08077D
31. [31]
  C. Li, W. Zhu, Y. Ma, et al., Anal. Bioanal. Chem. 416 (2024) 4849–4860. doi: 10.1007/s00216-024-05429-z
32. [32]
  S. Mai, X. Yao, C. Li, et al., Biomacromolecules 24 (2023) 2392–2405. doi: 10.1021/acs.biomac.3c00247
33. [33]
  X. Zhou, Y. Guo, F. Zhao, et al., Adv. Mater. 32 (2020) 2007012. doi: 10.1002/adma.202007012
34. [34]
  D. Li, Z. Zhu, D.W. Sun, Analyst 145 (2020) 897–907. doi: 10.1039/c9an01743g
35. [35]
  W. Hu, Y. Luo, E. Zhu, et al., Adv. Sustain. Syst. 8 (2024) 2400387. doi: 10.1002/adsu.202400387
36. [36]
  Q. Shao, S. Jiang, Adv. Mater. 27 (2015) 15–26. doi: 10.1002/adma.201404059
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2. [2]
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5. [5]
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6. [6]
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7. [7]
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8. [8]
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9. [9]
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10. [10]
  Yihan Fu , Xinyi Wang , Sen Li , Weifeng Lin , Mingjie Liu . Molecularly-engineered zwitterionic micelles for adaptive lubrication. Chinese Chemical Letters, 2026, 37(6): 111991-. doi: 10.1016/j.cclet.2025.111991
11. [11]
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12. [12]
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