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

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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：
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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

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