Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing

Ting Cui; Jing-Ming Cai; Cun-Yi Li; Zhou-Yue Lei; Pei-Yi Wu

doi:10.1007/s10118-026-3780-9

Your Location：

Home >

Browse articles >

Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing

RESEARCH ARTICLE | Updated：2026-08-19

- Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing
- Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing
- Chinese Journal of Polymer Science 2026年44卷页码：1-11
- Affiliations：
  
  a.State Key Laboratory of Advanced Fiber Materials, College of Chemistry and Chemical Engineering, Center for Advanced Low-Dimension Materials, Donghua University, Shanghai 201620, China
  b.State Key Laboratory of Digital Medical Engineering, School of Biological Science and Medical Engineering, Southeast University, Nanjing 210096, China
  c.School of Civil Engineering, Southeast University, Nanjing 210000, China
  d.School of Mechanical and Mechatronic Engineering, University of Technology Sydney, 817 Broadway, Ultimo, NSW, 2007, Australia
  e.Department of Civil Engineering, Aalto University, Espoo 02150, Finland
- Author bio：
  
  leizhouyue@seu.edu.cn (Z.Y.L.)
  wupeiyi@dhu.edu.cn (P.Y.W.)
- Funds：
  
  This work was ﬁnancially supported by the National Natural Science Foundation of China (Nos. 22305033 and 52573019 received by Z.Y.L., No. 52433003 received by P.Y.W.), and the Fundamental Research Funds for the Central Universities (No. 2232024A-05 received by Z.Y.L.).;The authors declare no interest conflict.Electronic supplementary information (ESI) is available free of charge in the online version of this article at http://doi.org/10.1007/s10118-026-3780-9.The related data of this study is data that should not be shared, and can be obtained from the author for reasonable reasons. The author’s contact information: wupeiyi@dhu.edu.cn.
- DOI：10.1007/s10118-026-3780-9
  中图分类号：
- 收稿：2026-05-11，
  
  录用：2026-06-10，
  
  网络首发：2026-08-19，
  
  纸质出版：2026-07
- Accepted：
Scan QR Code
Cui, T.; Cai, J. M.; Li, C. Y.; Lei, Z. Y.; Wu, P. Y. Synergistic spring-entanglement network design of high-modulus and low-hysteresis ionic elastomers for high-fidelity sensing. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3780-9

Ting Cui, Jing-Ming Cai, Cun-Yi Li, et al. Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11.
Cui, T.; Cai, J. M.; Li, C. Y.; Lei, Z. Y.; Wu, P. Y. Synergistic spring-entanglement network design of high-modulus and low-hysteresis ionic elastomers for high-fidelity sensing. Chinese J. Polym. Sci. https://doi.org/10.1007/s10118-026-3780-9 DOI：

Ting Cui, Jing-Ming Cai, Cun-Yi Li, et al. Synergistic Spring-entanglement Network Design of High-modulus and Low-hysteresis Ionic Elastomers for High-fidelity Sensing[J/OL]. Chinese Journal of Polymer Science, 2026, 441-11. DOI： 10.1007/s10118-026-3780-9.

摘要

Abstract

The development of high-performance ionotronics is currently hindered by the fundamental trade-off between mechanical robus

tness (high modulus and toughness) and functional reliability (low hysteresis and high elasticity). Conventional toughening mechanisms that rely on sacrificial bonds inevitably introduce significant energy dissipation and irreversible creep

leading to fatal signal drifts in long-term applications. Herein

we report a synergistic spring-entanglement network that achieves simultaneous optimization of the modulus

recovery

and extensibility

via

topological modulation. By utilizing a click-chemistry-derived covalent framework as a stiff athermal spring

the elastomer achieved a skin-like modulus (approximately 1 MPa) and near-zero hysteresis (

0.51%). The strategic integration of ultra-high-molecular-weight polymer entanglements introduces topological constraints that function as non-dissipative stress delocalisers

facilitating a fracture strain of 142% without compromising the instantaneous restorative force. This architecture maintains low hysteresis and high elasticity over 10000 cycles

ensuring impeccable signal fidelity and negligible baseline drift in multimodal sensing. This synergistic topological design provides a robust foundation for reliably stable human-machine interfaces and precision ionotronics.

关键词

Keywords

references

Keplinger, C.; Sun, J.-Y.; Foo, C. C.; Rothemund, P.; Whitesides, G. M.; Suo, Z. Stretchable, transparent, ionic Conductors. Science 2013 , 341 , 984−987..

Zhou, N.; Zhang, L.; Cui, T.; Wu, P.; Lei, Z. Design and applications of conductive polymers in wearable electrophysiological sensing. Sci. China Technol. Sci. 2025 , 68 , 2200204..

Lee, Y.; Lim, S.; Song, W. J.; Lee, S.; Yoon, S. J.; Park, J.-M.; Lee, M.-G.; Park, Y.-L.; Sun, J.-Y. Triboresistive touch sensing: grid-free touch-point recognition based on monolayered ionic power generators. Adv. Mater. 2022 , 34 , 2108586..

Zhou, X.; Yin, J.-F.; Chen, C.; Chi, Y.; Chen, J.; Liu-Fu, W.; Yang, J.; Long, S.; Tang, L.; Yao, X.; Yin, P. Hierarchical supramolecular aggregation of molecular nanopart icles for granular materials with ultra high-speed impact-resistance. Adv. Sci. 2024 , 11 , 2405285..

Liu, X.; Wu, J.; Qiao, K.; Liu, G.; Wang, Z.; Lu, T.; Suo, Z.; Hu, J. Topoarchitected polymer networks expand the space of material properties. Nat. Commun. 2022 , 13 , 1622..

Lake, G. J.; Thomas, A. G. The strength of highly elastic materials. Proc. A 1967 , 300 , 108−119..

Liu, J.; Yang, C.; Yin, T.; Wang, Z.; Qu, S.; Suo, Z. Polyacrylamide hydrogels. II. elastic dissipater. J. Mech. Phys. Solids 2019 , 133 , 103737..

Nonoyama, T.; Gong, J. P. Tough double network hydrogel andits biomedical applications. Annu. Rev. Chem. Biomol. Eng. 2021 , 12 , 393−410..

Zheng, Y.; Gong, J. P. Viscous solvent effect on fracture of predamaged double-network gels examined by pre-notch and post-notch crack tests. J. Mech. Phys. Solids 2025 , 194 , 105926..

Li, X.; You, X.; Wang, X.; Kang, J.; Zhang, H. J. Advanced lignin-based hydrogels with superior stiffness, toughness, and sensing capabilities. Adv. Funct. Mater. 2025 , 35 , 2415744..

Seiffert, S. Origin of nanostructural inhomogeneity in polymer-network gels. Polym. Chem. 2017 , 8 , 4472−4487..

Bao, B.; Shi, C.; Zeng, Q.; Chen, T.; Xiao, C.; Jiang, L.; Liu, T.; Lyu, J.; Wang, W.; Zhu, L.; Lin, Q. Photocoupling of propagating radicals during polymerization realizes universal network strengthening. Nat. Synth. 2025 , 4 , 1522−1533..

Shibayama, M. Spatial inhomogeneity and dynamic fluctuations of polymer gels. Macromol. Chem. Phys. 1998 , 199 , 1−30..

Ren, Y.; Guo, J.; Liu, Z.; Sun, Z.; Wu, Y.; Liu, L.; Yan, F. Ionic liquid–based click-ionogels. Sci. Adv. 2019 , 5 , eaax0648..

Liu, L.; Li, J.; Wang, S.; Xiang, Y.; Lu, T.; Gao, Y. Tough and anti-swelling naturally derived adhesives by long-chain toughening and electr ostatic attraction. Polymer 2025 , 336 , 128870..

Huang, Z.; Xu, L.; Liu, P.; Peng, J. Transparent, mechanically robust, conductive, self-healable, and recyclable ionogels for flexible strain sensors and electroluminescent devices. RSC Adv. 2024 , 14 , 28234−28243..

Jorge, A. M. S.; Silva, G. M. C.; Coutinho, J. A. P.; Pereira, J. F. B. Unravelling the molecular interactions behind the formation of PEG/PPG aqueous two-phase systems. Phys. Chem. Chem. Phys. 2024 , 26 , 7308−7317..

Jiang, Y.; Tang, N.; Wang, X.; Pei, D.; Zhang, H.; Li, M.-H.; Hu, J. Mechanically robust eutectogels enabled by precisely engineered crystalline domains. Nat. Commun. 2025 , 16 , 7417..

Zhang, L.; Liu, S.; Wang, Z.; Lei, Z.; Wu, P. An enthalpy-entropy compensated ionogel with a broadband viscoelastic plateau for non-invasive and high-fidelity neurointerfaces. Adv. Mater. 2026 , 38 , e21208..

Zhou, N.; Cui, T.; Lei, Z.; Wu, P. Bioinspired learning and memory in ionogels through fast response and slow rel axation dynamics of ions. Nat. Commun. 2025 , 16 , 4573..

Zhu, W.; Wu, B.; Lei, Z.; Wu, P. Piezoionic elastomers by phase and interface engineering for high-performance energy-harvesting ionotronics. Adv. Mater. 2024 , 36 , 2313127..

Liu, Y.; Zhang, J.; Wu, P. Near-frictionless long-distance water transport in trees enabled by hierarchically helical molecular pumps. CCS Chem. 2025 , 7 , 484−492..

Wang, H.; Wang, H.; Chen, D.; Tian, X.; Yang, J.; Liu, W. Solvent polarity-induced ultrahigh strength supramolecular polyzwitterionic organogels with impact-stiffening, damping, and anti-freezing properties. Small 2025 , 21 , 2501737..

[Yuan, Z.; Cao, Z.; Wang, H.; Wu, H.; Zheng, J.; Zhang, R.; Wu, J. Tough hydrogels enabled by transient entanglements. Nat. Commun . 2026 , 17 , 4145..

Zhao, L. J.; Tang, N.; Wang, X. T.; Li, M. H.; Hu, J. Conductive polyaniline hydrogel featuring high toughness and low hysteresis. Chinese J. Polym. Sci. 2025 , 43 , 581−587..

Wang, J.; Tang, F.; Yao, C.; Li, L. Low hysteresis hydrogel induced by spatial confinement. Adv. Funct. Mater. 2023 , 33 , 2214935..

Xue, Q.; He, X.; Lei, J.; Hong, W.; Yang, C. Synergizing network topology and solvent compatibility for gels with hyperelasticity and omniadhesion. Sci. Adv. 2026 , 12 , eaec7718..

Du, R.; Bao, T.; Zhu, T.; Zhang, J.; Huang, X.; Jin, Q.; Xin, M.; Pan, L.; Zhang, Q.; Jia, X. A low-hysteresis and highly stretchable ionogel enabled by well dispersed slidable cross-linker for rapid human-machine interaction. Adv. Funct. Mater. 2023 , 33 , 2212888..

Li, W.; Wang, X.; Liu, Z.; Zou, X.; Shen, Z.; Liu, D.; Li, L.; Guo, Y.; Yan, F. Nanoconfined polymerization limits crack propagation in hysteresis-free gels. Nat. Mater. 2024 , 23 , 131−138..

Tan, S.; Wang, C.; Yang, B.; Luo, J.; Wu, Y. Unbreakable hydrogels with self-recoverable 10200% stretchability. Adv. Mater. 2022 , 34 , 2206904..

Hou, X.; Huang, B.; Zhou, L.; Liu, S.; Kong, J.; He, C. An amphiphilic entangled network design toward ultratough hydrogels. Adv. Mater. 2023 , 35 , 2301532..

Nian, G.; Kim, J.; Bao, X.; Suo, Z. Making highly elastic and tough hydrogels from doughs. Adv. Mater. 2022 , 34 , 2206577..

Kim, J.; Zhang, G.; Shi, M.; Suo, Z. Fracture, fatigue, and friction of polymers in which entanglements greatly outnumber cross-links. Science 2021 , 374 , 212−216..

Wang, Z.; Yang, F.; Liu, X.; Han, X.; Li, X.; Huyan, C.; Liu, D.; Chen, F. Hydrogen bonds-pinned entanglement blunting the interfacial crack of hydrogel–elastomer hybrids. Adv. Mater. 2024 , 36 , 2313177..

Wang, W.; Guo, P.; Liu, X.; Chen, M.; Li, J.; Hu, Z.; Li, G.; Chang, Q.; Shi, K.; Wang, X.; Lei, K. Fully polymeric conductive hydrogels with low hysteresis and high toughness as multi-responsive and self-powered wearable sensors. Adv. Funct. Mater. 2024 , 34 , 2316346..

Xu, K.; Shen, K.; Yu, J.; Yang, Y.; Wei, Y.; Lin, P.; Zhang, Q.; Xiao, C.; Zhang, Y.; Cheng, Y. Ultradurable noncovalent cross-linked hydrogels with low hysteresis and robust elasticity for flexible electronics. Chem. Mater. 2022 , 34 , 3311−3322..

Bao, X.; Chen, Z.; Nian, G.; Tan, M. W. M.; Ahn, C. H.; Kutsovsky, Y.; Suo, Z. Unusually long polymers crosslinked by domains of physical bonds. Nat. Commun. 2025 , 16 , 4749..

Zhu, R.; Zhu, D.; Zheng, Z.; Wang, X. Tough double network hydrogels with rapid self-reinforcement and low hysteresis based on highly entangled networks. Nat. Commun. 2024 , 15 , 1344..

Li, T.; Li, X.; Yang, J.; Sun, H.; Sun, J. Healable ionic conductors with extremely low-hysteresis and high mechanical strength enabled by hydrophobic domain-locked reversible interactions. Adv. Mater. 2023 , 35 , 2307990..

Sun, Y.; Cheng, Y.; Shi, L.; Sun, J.; Chen, S.; Wang, R. Dual ion regulated eutectogels with high elasticity and adhesive strength for accurate strain sensors. Adv. Funct. Mater. 2024 , 34 , 2401808..

Zhang, S.; Ren, D.; Zhao, Q.; Peng, M.; Wang, X.; Zhang, Z.; Liu, W.; Huang, F. Observation of topological hydrogen-bonding domains in physical hydrogel for excellent self-healing and elasticity. Nat. Commun. 2025 , 16 , 2371..

Zhao, X.; Xu, J.; Zhang, J.; Guo, M.; Wu, Z.; Li, Y.; Xu, C.; Yin, H.; Wang, X. Fluorescent double network ionogels with fast self-healability and high resilience for reliable human motion detection. Mater. Horiz. 2023 , 10 , 646−656..

Li, X. L.; Shang, W. D.; Xu, T. Q. Super-tough and resilient recyclable polyester elastomers enabled by dynamic cross-linking. Macromolecules 2026 , 59 , 2292−2301..

Chen, M.; Qin, W.; Wang, Y.; Zhai, H.; Gu, C.; Zhao, X.; Bi, Y.; Xu, Y.; Ming, Z.; Li, S.; Hu, S.; Zhang, X.; Ma, X.; Yin, S. Dynamic Na+ bridges: a 3D printing strategy for hydrogels with high strength, low hysteresis, strong adhesion, and self-healing. Adv. Funct. Mater. 2026 , 36 , e24993..

Zhan, H.; Lei, Z.; Wu, P. Colossal piezoionic effect from hierarchical asymmetries in soft ionotronics. Adv. Mater . 2026 , 38 , e73067..

He, Y.; Cheng, Y.; Yang, C.; Guo, C. F. Creep-free polyelectrolyte elastomer for drift-free iontronic sensing. Nat. Mater. 2024 , 23 , 1107−1114..

Du, H. Y.; Zhang, J.; Xu, Q.; Cao, Y. C.; Jia, H.; Li, Y. Anti-swelling zwitterionic gels with high stretchability, conductivity for wireless underwater strain sensing. Chinese J. Polym. Sci. 2026 , 44 , 792−802..

Wu, J.; Fan, X.; Liu, X.; Ji, X.; Shi, X.; Wu, W.; Yue, Z.; Liang, J. Highly sensitive temperature–pressure bimodal aerogel with stimulus discriminability for human physiological monitoring. Nano Lett. 2022 , 22 , 4459−4467..

浏览量

Downloads

CSCD

文章被引用时，请邮件提醒。

Submit

工具集

关联资源

Soft Polymer Iontronics for Neuromorphic Intelligence

MXene Nanosheet-enhanced Ionotronic Hydrogels for Wireless Powering and Noncontact Sensing

Dynamic Structural Colors in Helical Superstructures: from Supramolecules to Polymers

Micro-sized Silicon Carbonitride Prepared by Radical Polymerization as a High-performance Anode Material for Lithium-ion Batteries

Water/Alcohol-soluble Organic Luminophores: A Review