The development of covalent adaptable networks has addressed
the
issue that conventional epoxy thermosets are difficult to degrade
and reprocess, but the greater challenge lies in how to overcome the
trade-off between excellent degradability and mechanical properties
such as stiffness and extensibility. Herein, a new concept of a dual-dynamic
cross-linked network composed of dynamic covalent and non-covalent
bonds (imine bonds and hydrogen bonds) was proposed for closed-loop
recovery of epoxy thermosets/composites. Among them, the additional
non-covalent crosslinks were constructed through the designed imine-containing
hardener as the medium. The cooperative effects of hydrogen-bond interactions
and molecular interlocking of rigid–flexible molecular chains
enhanced greatly the stiffness and ductility, and the recoverable
energy dissipation enabled the prepared epoxy thermoset to have excellent
fracture toughness. Its tensile strength and impact strength reached
∼80.3 MPa and ∼24.2 kJ/m2, respectively.
Importantly, driven by the pH-sensitive feature of the dual-dynamic
network, the resultant thermoset was completely degraded within 3
h. Along the closed-loop sustainable route, the recoverable oligomer
from the thermoset/matrix resin showed good potential in toughening
brittle materials with a 55–94% increase in impact strength.
Further, the recovered CF cloths that kept their usage value were
re-prepared into new high-performance composites, realizing the conversion
of waste to high-value applications.