Rigid–Flexible Supramolecular Polyurethane Elastomers for Efficient Photothermal Deicing

Abstract Ice accretion on outdoor infrastructure can severely compromise operational safety and service reliability, creating a strong demand for energy-efficient deicing materials. Conventional photothermal polymers, however, often suffer from an inherent trade-off between mechanical robustness and functional performance, and many also show limited self-healing ability and poor recyclability. Here, we report a rigid–flexible polyurethane elastomer (TPEA) enabled by a supramolecular cooperative design. Distinct from conventional approaches that rely on homogeneous segmental associations, our strategy deliberately exploits the intrinsically lower binding energy between flexible and rigid segments, which thermodynamically drives the formation of mismatched intersegment contacts rather than self-association of identical segments. Dynamic hydrogen-bonding motifs derived from adipic dihydrazide (AD) were combined with a rigid cross-linked framework introduced by 2,4,6-triaminopyrimidine (TAP), thereby integrating structural stability, energy dissipation, and reversible intermolecular interactions within one network. The optimized elastomer exhibits a tensile strength of 3.05 MPa, an elongation at break of 8195%, and a healing efficiency of up to 98%, while remaining recyclable through dissolution in DMF followed by solution recasting. To further impart photothermal functionality, carbon nanotubes (CNT) and reduced graphene oxide (rGO) were incorporated to construct a synergistic 1D/2D thermally conductive network. Under 1 sun simulated irradiation, the resulting TPEA-CNT/rGO composite achieved a deicing ratio of 95.9% for a 4 mm ice layer within 20 min, showing promise for efficient active deicing applications. These results establish a practical molecular design strategy for multifunctional polyurethane elastomers that combine mechanical resilience, healability, recyclability, and photothermal deicing performance.