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/m3). 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.