Universal Self-Healing Poly(dimethylsiloxane) Polymer Crosslinked Predominantly by Physical Entanglements

Harsh conditions are inevitable for long-term use of self-healing polymers. However, the majority of reported self-healing materials cannot remain stable under harsh conditions due to the presence of vulnerable dynamic crosslinking sites. Herein, a universal self-healing poly(dimethylsiloxane) (PDMS) polymer is reported. In our design, the PDMS polymer chains are crosslinked predominantly through physical entanglements. Owing to the invulnerable nature of the entanglement junctions and high mobility of polymer chains, the as-synthesized polymer exhibits autonomous self-healing capabilities not only under ambient conditions but also in a variety of harsh environments, including aqueous solutions, organic solvents, and extreme conditions (strong acid/alkali, redox agents, freezing temperature). Moreover, this polymer can be easily integrated with a eutectic gallium–indium (EGaIn) alloy to achieve layer-by-layer self-healing electronic skin sensors, which realize the combination of excellent electrical conductivity, long-term sensing stability, and universal self-healing capability.