Despite the enormous potential applications
for intrinsic self-healing
materials, these materials have reached a road-block where concurrent
excellent mechanical properties and autonomous self-healing behavior
are impossible. Herein reported is a base-layer-driven self-healing
(BLDS) approach that facilitates self-healing irrespective of the
glass transition (T
g) or melting temperature
(T
m) of the top layer. The BLDS approach
enables autonomous self-healing materials that concurrently offer
ultramechanical durability and ambient healing. The BLDS relies on
an ambient healable base layer and a structural/functional top layer.
In this study, the bottom layer is prepared using reversible-dynamic
covalent linkages in polyurethane/urea. Meanwhile, the top layer is
selected from a thermoplastic (e.g., polylactic acid), thermoset (e.g.,
polyurethane), and functional thermosets (e.g., omniphobic urethane).
The resultant dual-layer coatings/films offer a modulus of >800
MPa
and still maintained excellent ambient self-healing. The antirust
efficacy of the BLDS coating is also demonstrated. As the top layer
can be selected from any commercial structural and functional materials,
this work opens a whole different direction for autonomous healable
materials, which will open additional avenues of real-world applications.