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April 12, 2026Advanced Materials3 citationsOpen Access

Tough and Rapidly Relaxing Hydrogels Via Programmable Crosslink Kinetics

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YWYuanyuan WeiSOStephen J.K. O'NeillJMJade A. McCune

Key Points

  • This work aims to address the challenge of combining high toughness and rapid stress relaxation in synthetic hydrogels.
  • Developed a supramolecular hydrogel platform with programmable crosslink dynamics.
  • Regulated molecular dissociation kinetics to independently tune relaxation and toughness.
  • Conducted mechanical testing to evaluate stress relaxation and fracture properties.
  • Achieved stress relaxation times of 0.1-100 seconds, significantly faster than traditional hydrogels.
  • Obtained fracture energy of 14,500 J/m², exceeding that of natural rubber.
  • Demonstrated enhanced energy dissipation by slowing crosslink dissociation in viscoelastic networks.

Abstract

Replicating the synergy of high toughness and rapid stress relaxation found in native tissues remains a central challenge for synthetic hydrogels on account of their intrinsic mechanical-temporal trade-off. Here we introduce a supramolecular hydrogel platform that leverages kinetic programming to precisely regulate crosslink dynamics through molecular dissociation kinetics. This molecular design allows independent tuning of relaxation dynamics and fracture toughness, decoupling properties that are typically correlated. The resulting hydrogels exhibit stress relaxation (t 1 / 2 t₁/₂ = 0. 1-100 s) two orders of magnitude faster than conventional networks while achieving exceptional fracture energy (G c = 14, 500 J m - 2 Gc = 14, 500\, J\, m^-2), well above natural rubber. Slowing crosslink dissociation significantly enhances energy dissipation under load, revealing a kinetic principle for toughening viscoelastic networks. This work establishes a molecular blueprint for designing soft materials with programmable, time-dependent mechanics.

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Cite This Study

Wei et al. (2026) studied this question.

synapsesocial.com/papers/69db37ca4fe01fead37c5d57https://doi.org/10.1002/adma.202523440
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