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Tough and Rapidly Relaxing Hydrogels Via Programmable Crosslink Kinetics.

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Synthetic hydrogels now achieve high toughness and rapid stress relaxation by decoupling these properties using kinetic programming. This breakthrough enables advanced soft materials with programmable, time-dependent mechanics, mimicking natural tissues.

Keywords:
kinetic programmingprogrammable time‐dependent mechanicsstress relaxation dynamicssupramolecular hydrogelstoughness

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Area of Science:

  • Materials Science
  • Polymer Chemistry
  • Biomaterials Engineering

Background:

  • Synthetic hydrogels face a mechanical-temporal trade-off, limiting their ability to mimic native tissue properties.
  • Achieving both high toughness and rapid stress relaxation simultaneously is a significant challenge in hydrogel development.

Purpose of the Study:

  • To develop a supramolecular hydrogel platform that decouples toughness and relaxation dynamics.
  • To engineer hydrogels with tunable, time-dependent mechanical properties.

Main Methods:

  • Utilizing kinetic programming to precisely control crosslink dynamics via molecular dissociation kinetics.
  • Designing supramolecular hydrogels with tailored molecular dissociation rates.

Main Results:

  • Achieved stress relaxation two orders of magnitude faster than conventional networks (t1/2 = 0.1-100 s).
  • Obtained exceptional fracture energy (Gc = 14,500 J m⁻²), surpassing natural rubber.
  • Demonstrated that slowing crosslink dissociation enhances energy dissipation, revealing a kinetic toughening principle.

Conclusions:

  • Established a molecular design strategy for independent tuning of relaxation dynamics and fracture toughness in hydrogels.
  • Developed a kinetic principle for toughening viscoelastic soft materials.
  • Provided a molecular blueprint for creating soft materials with programmable, time-dependent mechanics.