Abstract

Ultimately soft electronics seek affordable and high mechanical performance universal self‐healing materials that can autonomously heal in harsh environments within short times scales. As of now, such features are not found in a single material. Herein, interpenetrated elastomer network with bimodal chain length distribution showing rapid autonomous healing in universal conditions (<7200 s) with high efficiency (up to 97.6 ± 4.8%) is reported. The bimodal elastomer displays strain‐induced photoelastic effect and reinforcement which is responsible for its remarkable mechanical robustness (≈5.5 MPa stress at break and toughness ≈30 MJ m−3). The entropy‐driven elasticity allows an unprecedented shape recovery efficiency (100%) even after fracturing and 100% resiliency up to its stretching limit (≈2000% strain). The elastomers can be mechanically conditioned leading to a state where they recover their shape extremely quickly after removal of stress (nearly order of magnitude faster than pristine elastomers). As a proof of concept, universal self‐healing mechanochromic strain sensor is developed capable of operating in various environmental conditions and of changing its photonic band gap under mechanical stress.

Highlights

  • Resilin-Inspired Bimodal Self-Healing ElastomerSimilar polymer backbone structures (Figures S1 and S2, Supporting Information) with cross-linking elements allow the formation of permanent net-/junction-points (Figure 1b,c)

  • Soft electronics seek affordable and high mechanical performance counterparts.[4,5,6,7,8] thin and compliant soft systems are deformable and reuniversal self-healing materials that can autonomously heal in harsh sistant to blunt damage, they have poor environments within short times scales

  • Soft materials inspired by biological systems hold great promise for soft robotics, prostheses, and implantable and skinmountable electronics

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Summary

Resilin-Inspired Bimodal Self-Healing Elastomer

Similar polymer backbone structures (Figures S1 and S2, Supporting Information) with cross-linking elements allow the formation of permanent net-/junction-points (Figure 1b,c). These are formed by covalent bonds and interpenetrating networks, both of which have a role in the entropy-driven elasticity by preventing the occurrence of chain slippage and flow (Figure 1di). The system is in equilibrium because the long polymer chains (of the soft phase) with freely rotating links are in their energetically favorable conformation.[34] The conformation has a high degree of freedom as it can be distributed in various randomly kinked and oriented conformations (Figure 1ei). The system is driven by the gain of conformational entropy when the force is removed to recover the energetically favorable conformation and restore the equilibrium

Material Characterization
Mechanical Characterization
Universal Self-Healing Properties
Universal Self-Healing Mechanism in Dry and Wet Conditions
Application as Mechanochromic Sensor
Conclusions
Experimental Section
Data Availability Statement

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