ArticleAdvanced science (Weinheim, Baden-Wurttemberg, Germany)2026
Dynamic Supramolecular Polyurethane Elastomers Enabling Bioinspired Strain-Adaptive Stiffening to Resolve the Softness-Strength Paradox.
Article in Advanced science (Weinheim, Baden-Wurttemberg, Germany), 2026. The graph could read no effect estimate from its abstract, so it casts no vote on the map. Not yet cited in PubMed.
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Abstract
The rapid progress of soft robotics and flexible electronics has sparked tremendous demand for elastomers that unite high mechanical strength with intrinsic softness, thereby mimicking the mechanical performance of natural skin. Herein, we report a class of dynamically crosslinked supramolecular polyurethanes that combine skin-comparable low modulus with high strength and room-temperature self-healing, achieved through a segmental molecular engineering strategy. The design leverages entropy-driven soft elasticity together with enthalpy-governed strain-stiffening and energy dissipation, dictated by polymer segment topology. Using a prototypical supramolecular elastomer, we demonstrate that incorporating an isophorone diisocyanate (IPDI) chain extender, whose steric configuration matches that of ureidopyimidinone (UPy), reinforces hydrogen bonding interaction and suppresses premature crystallization. The optimized elastomer exhibits an ultralow initial modulus (<3 MPa) yet undergoes pronounced strain-stiffening, yielding exceptional tensile strength (>50 MPa) and high fracture toughness (∼2×10
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