Strong and Tough Composite Hydrogels with Crack-deflecting Ability Enabled by a Viscoelastoplastic Mixing Strategy

Xiang Li; Bei Jiang; Bin Wang; Ya-Rong Yang; Gui-Ming Zhao; Li-Li Wang

doi:10.1007/s10118-025-3547-8

Your Location：

Home >

Browse articles >

Strong and Tough Composite Hydrogels with Crack-deflecting Ability Enabled by a Viscoelastoplastic Mixing Strategy

RESEARCH ARTICLE | Updated：2026-02-13

- Strong and Tough Composite Hydrogels with Crack-deflecting Ability Enabled by a Viscoelastoplastic Mixing Strategy
- Chinese Journal of Polymer Science Vol. 44, Issue 3, Pages: 768-780(2026)
- Affiliations：
  
  State Key Laboratory of Bio-Fibers and Eco-Textiles, College of Materials Science and Engineering, Qingdao University, Qingdao 266071, China
- Author bio：
  
  llwang@qdu.edu.cn
- Funds：
- DOI：10.1007/s10118-025-3547-8
  CLC：
- Received：13 November 2025，
  
  Revised：2025-12-28，
  
  Accepted：05 January 2026，
  
  Online First：06 February 2026，
  
  Published：15 March 2026
- Accepted：
Scan QR Code
Li, X.; Jiang, B.; Wang, B.; Yang, Y. R.; Zhao, G. M.; Wang, L. L. Strong and tough composite hydrogels with crack-deflecting ability enabled by a viscoelastoplastic mixing strategy. Chinese J. Polym. Sci. 2026, 44, 768–780

Xiang Li, Bei Jiang, Bin Wang, et al. Strong and Tough Composite Hydrogels with Crack-deflecting Ability Enabled by a Viscoelastoplastic Mixing Strategy[J]. Chinese Journal of Polymer Science, 2026, 44(3): 768-780.
Li, X.; Jiang, B.; Wang, B.; Yang, Y. R.; Zhao, G. M.; Wang, L. L. Strong and tough composite hydrogels with crack-deflecting ability enabled by a viscoelastoplastic mixing strategy. Chinese J. Polym. Sci. 2026, 44, 768–780 DOI： 10.1007/s10118-025-3547-8.

Xiang Li, Bei Jiang, Bin Wang, et al. Strong and Tough Composite Hydrogels with Crack-deflecting Ability Enabled by a Viscoelastoplastic Mixing Strategy[J]. Chinese Journal of Polymer Science, 2026, 44(3): 768-780. DOI： 10.1007/s10118-025-3547-8.

摘要

A novel strategy of “blending reinforcement in the viscoelastoplastic state and structural fixation in the viscoelastic state” was developed to fabricate poly(vinyl alcohol) (PVA)/silica composite hydrogels. This approach results in enhanced interfacial strength and a high-density polymer network

thereby endowing the hydrogels with outstanding mechanical properties and long-term stability.

Abstract

The weak interfacial bonding and significant modulus mismatch between the reinforcement phase and the hydrogel matrix greatly limit the reinforcing efficiency in conventional composite hydrogels. To address these issues

we propose a novel design strategy based on dynamic mechanical control

summarized as “blending reinforcement in the viscoelastoplastic state and fixing the structure in the viscoelastic state.” This approach utilizes a unique poly(vinyl alcohol) (PVA) hydrogel matrix featuring an amorphous/strong hydrogen-bonding hierarchical architecture

which undergoes a thermal-

induced transition from a viscoelastoplastic to a viscoelastic state

enabling effective filler dispersion and subsequent structural stabilization. The method effectively suppresses filler aggregation through mechanical mixing in the viscoelastoplastic matrix

while the high polymer chain density and abundant physical interactions reduce modulus mismatch between dual phases. This synergy

together with enhanced interfacial strength achieved through strong physical bonding and structural reorganization during the cooling-induced mechanical transition

creates a robust interface that promotes crack deflection and tortuous crack propagation. As a result

we successfully fabricate PVA/silica composite hydrogels with outstanding mechanical properties and long-term stability. Moreover

by leveraging the salt-responsive nature of the system

the mechanical properties of the composite hydrogels can be reversibly and broadly modulated

via

a salt solution exchange strategy. This work establishes a fundamental principle and a practical pathway for the design and fabrication of advanced hydrogel composites.

关键词

Keywords

references

Zhao, C. X.; Guo, M.; Mao, J.; Li, Y. T.; Wu, Y. P.; Guo, H.; Xiang, D.; Li, H. Self-healing, stretchable, temperature-sensitive and strain-sensitive hydrogel-based flexible sensors. Chinese J. Polym. Sci. 2023 , 41 , 334−344..

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..

Feng, Y. B.; Liu, H.; Zhu, W. H.; Guan, L.; Yang, X. T.; Zvyagin, A.; Zhao, Y.; Shen, C.; Yang, B.; Lin, Q. Muscle-inspired MXene conductive hydrogels with anisotropy and low-temperature tolerance for wearable flexible sensors and arrays. Adv. Funct. Mater. 2021 , 31 , 2105264..

Li, X. T.; Zhang, S. Q.; Li, X. A.; Lu, L.; Cui, B.; Yuan, C.; Guo, L.; Yu, B.; Chai, Q. Q. Starch/polyvinyl alcohol with ionic liquid/graphene oxide enabled highly tough, conductive and freezing-resistance hydrogels for multimodal wearable sensors. Carbohydr. Polym. 2023 , 320 , 121262..

Li, Y.; Zhu, C. H.; Fan, D. D.; Fu, R. Z.; Ma, P.; Duan, Z. G.; Li, X.; Lei, H.; Chi, L. A bi-layer PVA/CMC/PEG hydrogel with gradually changing pore sizes for wound dressing. Macromol. Biosci. 2019 , 19 , 1800424..

Wang, C.; Liu, Y.; Qu, X. C.; Shi, B. J.; Zheng, Q.; Lin, X. B.; Chao, S. Y.; Wang, C. Y.; Zhou, J.; Sun, Y.; Mao, G. S.; Li, Z. Ultra-stretchable and fast self-healing ionic hydrogel in cryogenic environments for artificial nerve fiber. Adv. Mater. 2023 , 35 , 2300757..

Pan, S.; Xia, M.; Li, H.; Jiang, X.; He, P.; Sun, Z.; Zhang, Y. Transparent, high-strength, stretchable, sensitive and anti-freezing poly(vinyl alcohol) ionic hydrogel strain sensors for human motion monitoring. J. Mater. Chem. C. 2020 , 8 , 2827−2837..

Li, R.; Shi, Y.; Alsaedi, M.; Wu, M.; Shi, L.; Wang, P. Hybrid hydrogel with high water vapor harvesting capacity for deployable solar-driven atmospheric water generator. Environ. Sci. Technol. 2018 , 52 , 11367−11377..

Guo, Z.;Wang, Z.;Pan, W.;Zhang, J.;Qi, Y.;Qin, Y.;Zhang, Y. Fiber-reinforced polyvinyl alcohol hydrogel via in situ fiber formation. E-Polymer 2023 , 23 , 20230056..

Wang, M.; Bai, J.; Shao, K.; Tang, W.; Zhao, X.; Lin, D.; Huang, S.; Chen, C.; Ding, Z.; Ye, J. Poly(vinyl alcohol) h ydrogels: the old and new functional materials. Int. J. Polym. Sci. 2021 , 2021 , 2225426..

Liu, Y. G.; Zhang, J.; Wang, D. Y. Preparation schemes and applications of multifunctional PVA composite hydrogels. Chem. Eng. J. 2025 , 508 , 160946..

[Zhao, G. M.; Li, X.; Zhang, X. S.; Chen, L. C.; Yuan, L. H.; Dong, X.; Wang, L. L.; Surfactant-driven bidirectional tuning of viscoplastic physical hydrogels and the underlying mechanism. Macromolecules 2025 , 58 , 12117−12127..

Seo, Y.; Lee, J.; Park, S.; Kim, M.; Kim, S.; Oh, T. PVA hydrogels supplemented with PLA mesh for tissue regeneration scaffold. Gels. 2024 , 10 , 364..

Xu, R. D.; She, M. H.; Liu, J. X.; Zhao, S. K.; Zhao, J. S.; Zhang, X. J.; Qu, L. J.; Tian, M. W. Skin-friendly and wearable iontronic touch panel for virtual-real handwriting interaction. ACS Nano. 2023 , 17 , 8293−8302..

Feng, X.; Tian, Y.; Gu, G.; Wang, C.; Shang, S.; Huang, X.; Jiang, J.; Song, Z.; Zhang, H. High-st rength PVA/cellulosic hydrogels with acid/base and thermo dual-responsive fluorescence. Chem. Eng. J. 2024 , 500 , 156763..

Li, Z.; Jiang, J.; Luo, J.; Meng, J.; Cheng, L.; Qin, H. A robust and conductive hydrotalcite/nanocellulose/PVA hydrogel constructed based on the Hofmeister effect. Int. J. Biol. Macromol. 2025 , 298 , 139994..

Piacentini, E.; Poerio, T.; Bazzarelli, F.; Giorno, L. Continuous production of PVA-based hydrogel nanoparticles by membrane nanoprecipitation. J. Membr. Sci. 2021 , 637 , 119649..

Hu, M.; Gu, X. Y.; Hu, Y.; Deng, Y. H.; Wang, C. Y. PVA/carbon dot nanocomposite hydrogels for simple introduction of Ag nanoparticles with enhanced antibacterial activity. Macromol. Mater. Eng. 2016 , 301 , 1352−1362..

Lorusso, E.; Ali, W.; Hildebrandt, M.; Mayer-Gall, T.; Gutmann, J. Hydrogel functionalized polyester fabrics by UV-induced photopolymerization. Polymers. 2019 , 11 , 1329..

Qin, Z. P.; Zhao, G.; Zhang, Y. Y.; Gu, Z. H.; Tang, Y. H.; Aladejana, J. T.; Ren, J . N.; Jiang, Y. H.; Guo, Z. H.; Peng, X. F.; Zhang, X. H.; Xu, B. B.; Chen, T. J. A simple and effective physical ball-milling strategy to prepare super-tough and stretchable PVA@MXene@PPy hydrogel for flexible capacitive electronics. Small. 2023 , 19 , 2303038..

Wu, M.; Peng, Q. Y.; Han, L. B.; Zeng, H. B. Self-healing hydrogels and underlying reversible intermolecular interactions. Chinese J. Polym. Sci. 2021 , 39 , 1246−1261..

Zhou, Y.; Wan, C. J.; Yang, Y. S.; Yang, H.; Wang, S. C.; Dai, Z. D.; Ji, K. J.; Jiang, H.; Chen, X. D.; Long, Y. Highly stretchable, elastic, and ionic conductive hydrogel for artificial soft electronics. Adv. Funct. Mater. 2019 , 29 , 1806220..

Jiang, B.; Nie, Z. P.; Zhao, G. M.; Wang, B.; Xu, H. X.; Zhang, X. S.; Wang, L. L. Matching combination of amorphous ionic hydrogel with elastic fabric enables integrated properties for wearable sensing. Polymer. 2024 , 315 , 127790..

Xu, R. D.; Qu, L. J.; Tian, M. W. Touch-sensing fabric encapsulated with hydrogel for human-computer interaction. Soft Matter. 2021 , 17 , 9014−9018..

Guan, Q. F.; Yang, H. B.; Han, Z. M.; Ling, Z. C.; Yin, C. H.; Yang, K. P.; Zhao, Y. X.; Yu, S. H. Sustainable cellulose-nanofiber-based hydrogels. ACS Nano 2021 , 15 , 7889−7898..

Hubbard, A. M.; Cui, W.; Huang, Y. W.; Takahashi, R.; Dickey, M. D.; Genzer, J.; King, D. R.; Gong, J. P. Hydrogel/elastomer laminates bonded via fabric interphases for stimuli-responsive actuators. Matter. 2019 , 1 , 674−689..

Zhang, N.; Zhang, B.; Pang, Y.; Yang, H. S.; Zong, L.; Duan, Y. X.; Zhang, J. M. High performance of PVA nanocomposite reinforced by Janus-like asymmetrically oxidized graphene: synergetic effect of H-bonding interaction and interfacial crystallization. Chinese J. Polym. Sci. 2022 , 40 , 373−383..

Ren, J.; Yang, X.; Xiang, X. Carboxymethyl cellulose-reinforced sandwich-structured carbon nanotube composite hydrogels for strain sensing and joule heating. Carbohydr. Polym. 2025 , 369 , 124291..

Ratwani, C.; Zhao, S.; Huang, Y.; Hadfield, M.; Kamali, A.; Abdelkader, A. Surface modification of transition metal dichalcogenide nanosheets for intrinsically self-healing hydrogels with enhanced mechanical p roperties. Small. 2023 , 19 , 2207081..

Zhang, R.; Wu, Y.; Lin, P.; Jia, Z. F.; Zhang, Y. J.; Liu, F. Z.; Yu, B.; Zhou, F. Extremely tough hydrogels with cotton fibers reinforced. Adv. Eng. Mater. 2020 , 22 , 2000508..

Sun, M. Z.; Li, H. G.; Hou, Y.; Huang, N.; Xia, X. Y.; Zhu, H. J.; Xu, Q.; Lin, Y.; Xu, L. Z. Multifunctional tendon-mimetic hydrogels. Sci. Adv. 2023 , 9 , eade6973..

Arno, M. C.; Inam, M.; Weems, A. C.; Li, Z. H.; Binch, A. L. A.; Platt, C. I.; Richardson, S. M.; Hoyland, J. A.; Dove, A. P.; O'Reilly, R. K. Exploiting the role of nanoparticle shape in enhancing hydrogel adhesive and mechanical properties. Nat. Commun. 2020 , 11 , 1420..

[Zhang, X. Y.; Deng, S, Y.; Cai, C, M.; Li, J, C.; Lei, C. H.; Chen, A. F.; Gao, Y. F. Preparation and viscoelastic behavior of hydrogel composites. Acta Polymerica Sinica (in Chinese) 2025 , 56, 1215−1222..

Views

Downloads

CSCD

Alert me when the article has been cited

Submit

Tools

Publicity Resources

Simulation of the Specific Contributions of Molecular Weight, Orientation Degree, and Crystallinity to the Tensile Mechanics of Polyethylene Fibers

A Self-healing and Flame-retardant Poly(urethane-urea) Elastomer Driven by Hydrogen Bonds and Phosphorus-Nitrogen Synergy

Bio-derived Flame-retardant Curing Agents Enable One-step, Ambient Synthesis of Ultra-tough, Smoke-suppressed Epoxy

Related Author

Tian-Hao Yang

Jing-Han Wu

Ming-Ming Ding

Wen Zhai

Ke Wang

Qiang Fu

Yang Liu

Chen-Qing Wu

Related Institution

College of Polymer Science and Engineering, Sichuan University, State Key Laboratory of Polymer Materials Engineering

Shandong Nonmetallic Materials Institute

National Engineering Lab of Textile Fiber Materials & Processing Technology, Zhejiang Sci-Tech University

Tongxiang Research Institute, Zhejiang Sci-Tech University

School of Chemistry and Materials Engineering, Zhejiang A & F University

⁰