Supramolecular Interface Engineering via Interdiffusion for Reusable and Dismantlable Polymer Adhesion.

Controllable adhesion that enables both reuse and dismantling is a key requirement for sustainable materials and device integration. Here,a polymeric adhesion system is demonstrated based on reversible interactions at the interface, in which the association and dissociation of supramolecular complexes are externally regulated by thermal and chemical stimuli. By tuning the glass transition temperature (Tg) of the polymers, chain mobility and complex reformation are simultaneously optimized, leading to enhanced interdiffusion and bond recombination at the adhesion interface. Neutron reflectivity (NR) measurements with deuterium labeling revealed that the interfacial width increased with annealing temperature, reaching up to 24.4 nm at 200 °C after 24 hours. The presence of reversible bonds suppressed polymer interdiffusion despite promoting adhesion strength. The resulting materials exhibit excellent reusability and dismantlability under mild stimuli, with strong potential for applications in recyclable electronics, automotive manufacturing, and temporary assembly technologies.