Non‐Destructive Recycling of Ultra‐Strong Polyolefin Adhesives from Polymer Mixtures

ABSTRACT Non‐destructive recycling of polymer materials is promising to mitigate serious environmental, ecological, and healthy concerns of waste polymers, which are also energy‐efficient and cost‐effective without disrupting the covalent bonds. The solvent‐targeted recovery strategy is straightforward for reclaiming polymer mixtures with significantly different chemical solubility, but it represents a tremendous challenge to recycle partially miscible polymers usually involved in the polymer adhesive systems. Here, we show that non‐destructive recycling of ultra‐strong nucleobase‐containing polyolefin adhesives can be achieved from diverse polymer mixtures. By merging bioinspired nucleobase interactions into flexible polyolefins, thymine‐containing polyolefins display strong mechanical and remarkable adhesive properties. Furthermore, strong and stable underwater adhesion was observed for the thymine‐containing polyolefin adhesive, owing to the high activation energy for the proton exchange with water. Ultimately, the ingenious combination of pendant thymine with the hydrophobic flexible alkyl backbone affords a polar hydrophobic H‐bonding adhesive, which is capable of achieving non‐destructive recycling from complicated polymer mixtures with substantially distinct or even similar solubility. This work develops a family of robust and non‐destructive recyclable adhesives through the introduction of bioinspired nucleobase interactions into polyolefins.