Catalytic Amine Functionalization and Polymerization of Cyclic Alkenes Creates Adhesive and Self-Healing Materials

The chemical functionalization of polyolefins to access responsive materials is a long-standing challenge in materials science. Current protocols do not typically tolerate polar functional groups, and postpolymerization modification often leads to material defects. Here the catalytic synthesis of amine-functionalized polyolefins has been achieved using a two-step catalytic combination of hydroaminoalkylation and ring-opening metathesis polymerization (ROMP). Furthermore, reduction was used to obtain an aminated polyethylene analogue. This preparation transforms simple starting materials into polar-functionalized polymers with complete atom economy. Utilizing dynamic associative interactions, including hydrogen bonding, these materials demonstrate tunable rheological properties, autonomous self-healing, and unexpected adhesion to polytetrafluoroethylene (PTFE).