Tough and Rapidly Relaxing Hydrogels Via Programmable Crosslink Kinetics.
basic_science · Level V
Where this comes from
- Record sourced from PubMed, PMID 41957865.
- Also identified by DOI 10.1002/adma.202523440 and PMC identifier 13155329.
- Licence recorded as CC BY.
- The licence permits redistribution, so the abstract is shown in full and the full text is available from the publisher.
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 ( <math xmlns="http://www.w3.org/1998/Math/MathML"> <semantics><msub><mi>t</mi> <mrow><mn>1</mn> <mo>/</mo> <mn>2</mn></mrow> </msub> <annotation>${t}_{1/2}$</annotation></semantics> </math> = 0.1-100 s) two orders of magnitude faster than conventional networks while achieving exceptional fracture energy ( <math xmlns="http://www.w3.org/1998/Math/MathML"> <semantics> <mrow><msub><mi>G</mi> <mi>c</mi></msub> <mo>=</mo> <mn>14</mn> <mo>,</mo> <mn>500</mn> <mspace></mspace> <mi>J</mi> <mspace></mspace> <msup><mi>m</mi> <mrow><mo>-</mo> <mn>2</mn></mrow> </msup> </mrow> <annotation>$G_c = 14{,}500\,\mathrm{J\,m^{-2}}$</annotation></semantics> </math> ), 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.