Zwitterionic Ionogels Resolving the Trade-Off Between Mechanical Strength and Autonomous Self-Healing for Iontronics
Corresponding Author: Do Hwan Kim
Nano-Micro Letters,
Vol. 19 (2027), Article Number: 11
Abstract
Simultaneously achieving mechanical robustness and autonomous self-healing in ionogels remains a fundamental challenge for durable, skin-like electronics. Conventional approaches often improve mechanical strength by introducing rigid or densely cross-linked polymer networks, but such strategies inevitably restrict polymer chain mobility and hinder dynamic bond reconfiguration required for healing. Here, a zwitterionic side-chain engineered tough ionogel (ZESTI) is developed to overcome this trade-off through molecular-level design. Hydrophilic zwitterions are covalently grafted onto a hydrophobic polyurethane backbone to preferentially interact with the ionic liquid through ion–dipole interactions and thereby regulate its distribution. This architecture simultaneously facilitates dipole–dipole interactions for mechanical reinforcement and ion–dipole coordination for efficient self-healing under ambient conditions. As a result, ZESTI exhibits an exceptional combination of tensile strength (10.40 MPa), stretchability (1606%), toughness (56.03 MJ m−3), and ambient self-healing efficiency exceeding 83%, while maintaining high ionic conductivity via enhanced ion hopping. When constructed as a self-reporting packaging interface, ZESTI provides stable protection and state perception under sharp contact and restores signal output after mechanical damage through self-healing. This work offers a generalizable design strategy that reconciles mechanical toughness with dynamic functionality in ionogels, establishing a general design paradigm for next-generation self-sustaining iontronic devices.
Highlights:
1 Zwitterionic side-chain engineered tough ionogel (ZESTI) resolves the trade-off between mechanical toughness and autonomous self-healing through zwitterionic side-chain engineering.
2 Synergistic dynamic ion–dipole and dipole–dipole interactions enable robust mechanical reinforcement, efficient ion transport, and room-temperature self-healing.
3 ZESTI-based iontronic devices exhibit reliable sensing performance and functional recovery after mechanical damage.
Keywords
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References
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E.K. Boahen, B. Pan, H. Kweon, J.S. Kim, H. Choi et al., Ultrafast, autonomous self-healable iontronic skin exhibiting piezo-ionic dynamics. Nat. Commun. 13, 7699 (2022). https://doi.org/10.1038/s41467-022-35434-8
J. Kang, J.B.H. Tok, Z. Bao, Self-healing soft electronics. Nat. Electron. 2(4), 144–150 (2019). https://doi.org/10.1038/s41928-019-0235-0
M. Wang, P. Zhang, M. Shamsi, J.L. Thelen, W. Qian et al., Tough and stretchable ionogels by in situ phase separation. Nat. Mater. 21(3), 359–365 (2022). https://doi.org/10.1038/s41563-022-01195-4
J. Jung, S. Lee, H. Kim, W. Lee, J. Chong et al., Self-healing electronic skin with high fracture strength and toughness. Nat. Commun. 15, 9763 (2024). https://doi.org/10.1038/s41467-024-53957-0
J. Chen, Y. Gao, L. Shi, W. Yu, Z. Sun et al., Phase-locked constructing dynamic supramolecular ionic conductive elastomers with superior toughness, autonomous self-healing and recyclability. Nat. Commun. 13, 4868 (2022). https://doi.org/10.1038/s41467-022-32517-4
M. Wang, J. Hu, M.D. Dickey, Tough ionogels: synthesis, toughening mechanisms, and mechanical properties—a perspective. JACS Au 2(12), 2645–2657 (2022). https://doi.org/10.1021/jacsau.2c00489
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H. Deng, Z. Cao, J. Yang, M. Yin, C. Yu et al., Nanomesh reinforced eutectogel by interfacial engineering for human motion monitoring and machine learning-enabled gesture recognition. Adv. Funct. Mater. 36(37), e74510 (2026). https://doi.org/10.1002/adfm.74510
S. Chen, Q. Wang, J. Shao, X. Li, Y. Bian et al., Decoupling of bonding strength and water retention in aqueous wood adhesive inspired by plant cell. ACS Nano 19(16), 15876–15885 (2025). https://doi.org/10.1021/acsnano.5c01165
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B.-X. Cheng, W.-C. Gao, X.-M. Ren, X.-Y. Ouyang, Y. Zhao et al., A review of microphase separation of polyurethane: characterization and applications. Polym. Test. 107, 107489 (2022). https://doi.org/10.1016/j.polymertesting.2022.107489
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A. Clark, M.E. Taylor, M.J. Panzer, P. Cebe, Interactions between ionic liquid and fully zwitterionic copolymers probed using thermal analysis. Thermochim. Acta 691, 178710 (2020). https://doi.org/10.1016/j.tca.2020.178710
S. Wang, D. Zhang, X. He, J. Yuan, W. Que et al., Polyzwitterionic double-network ionogel electrolytes for supercapacitors with cryogenic-effective stability. Chem. Eng. J. 438, 135607 (2022). https://doi.org/10.1016/j.cej.2022.135607
L. Rebollar, M.J. Panzer, Zwitterionic copolymer-supported ionogel electrolytes: impacts of varying the zwitterionic group and ionic liquid identities. ChemElectroChem 6(9), 2482–2488 (2019). https://doi.org/10.1002/celc.201900378
J. Zhu, X. Yin, W. Zhang, M. Chen, D. Feng et al., Simultaneous and sensitive detection of three pesticides using a functional poly(sulfobetaine methacrylate)-coated paper-based colorimetric sensor. Biosensors 13(3), 309 (2023). https://doi.org/10.3390/bios13030309
H. Wen, S. Chen, Z. Ge, H. Zhuo, J. Ling et al., Development of humidity-responsive self-healing zwitterionic polyurethanes for renewable shape memory applications. RSC Adv. 7(50), 31525–31534 (2017). https://doi.org/10.1039/c7ra05212j
O. Plohl, K. Fric, A. Filipić, P. Kogovšek, M. Tušek Žnidarič et al., First insights into the antiviral activity of chitosan-based bioactive polymers towards the bacteriophage Phi6: physicochemical characterization, inactivation potential, and inhibitory mechanisms. Polymers 14(16), 3357 (2022). https://doi.org/10.3390/polym14163357
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D.H. Ho, Y.M. Kim, U.J. Kim, K.S. Yu, J.H. Kwon et al., Zwitterionic polymer gel-based fully self-healable ionic thermoelectric generators with pressure-activated electrodes. Adv. Energy Mater. 13(32), 2301133 (2023). https://doi.org/10.1002/aenm.202301133
G. Bellisola, C. Sorio, Infrared spectroscopy and microscopy in cancer research and diagnosis. Am. J. Cancer Res. 2(1), 1 (2011)
H. Yuan, S. University, H. Huang, S. University, G. Huang et al., Dynamically adaptive and durable poly(ionic liquid) elastomer enabled by ion–dipole interactions for underwater sensing. Macromolecules 59(7), 4519–4534 (2026). https://doi.org/10.1021/acs.macromol.6c00496
Q. Shao, Y. He, S. Jiang, Molecular dynamics simulation study of ion interactions with zwitterions. J. Phys. Chem. B 115(25), 8358–8363 (2011). https://doi.org/10.1021/jp204046f
M.Y. Tadesse, Z. Zhang, N. Marioni, E.S. Zofchak, T.J. Duncan et al., Mechanisms of ion transport in lithium salt-doped zwitterionic polymer-supported ionic liquid electrolytes. J. Chem. Phys. 160(2), 024905 (2024). https://doi.org/10.1063/5.0176149
M.E. Taylor, M.J. Panzer, Fully-zwitterionic polymer-supported ionogel electrolytes featuring a hydrophobic ionic liquid. J. Phys. Chem. B 122(35), 8469–8476 (2018). https://doi.org/10.1021/acs.jpcb.8b05985
W.B. Ying, J.S. Kim, Z. Kong, Z. Yu, E.K. Boahen et al., A reconfigurable piezo-ionotropic polymer membrane for sustainable multi-resonance acoustic sensing. Nat. Commun. 16, 8180 (2025). https://doi.org/10.1038/s41467-025-63643-4
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