Abstract
Developing versatile, tough, and sustainable adhesives that function effectively in both wet and dry environments is a significant challenge. Here, we report a bioinspired design for versatile, tough, reversible adhesives upcycled from consumer poly(ethylene terephthalate) (PET) waste. Our approach employs solvent-free, room-temperature dynamic crosslinking of deconstructed PET macromonomers with an acetoacetate crosslinker, generating a dynamic, vinylogous urethane-bonded, amphiphilic adhesive. Tunable crosslinker concentration and amphiphilicity yield versatile adhesives suitable for underwater, structural, and pressure-sensitive applications on diverse substrates, demonstrating superior lap-shear strength and work of debonding in both wet and dry conditions, and outperforming common commercial adhesives. The dynamic bonds enable thermal repair, on-demand multicycle debonding/rebonding, facile removal, and chemical recycling. Our strategy of transforming plastic waste into versatile, tough, and reversible adhesive offers a sustainable solution for both plastic waste management and next-generation adhesive design, while also providing a commercially viable pathway for valorizing plastic waste.
