Toward Robust, Tough, Self-Healable Supramolecular Elastomers for Potential Application in Flexible Substrates

A robust, tough, and self-healable elastomer is a promising candidate for substrate in flexible electronic devices, but there is often a trade-off between mechanical properties (robustness and toughness) and self-healing. Here, a poly(dimethylsiloxane) (PDMS) supramolecular elastomer is developed based on metal-coordinated bonds with relatively high activation energy. The strong metal–coordination complexes and their corresponding ionic clusters acting as the cross-linking points strengthen the resultant supramolecular networks, which achieves superior mechanical robustness (2.81 MPa), and their consecutive dynamic rupture and reconstruction efficiently dissipate strain energy during the stretching process, which leads to an impressive fracture toughness (32 MJ/m 3 ). Additionally, the reversible intermolecular interactions (weak hydrogen bonds and strong sacrificial coordination complexes/clusters) can break and re-form upon heating; thus, the elastomer self-heals at a moderate temperature with the highest healing efficiency of 95%. As such, the potential of the as-prepared supramolecular elastomer for a substrate material of flexible electronic devices is discovered.