Catalytic Amine Functionalization and Polymerization of Cyclic Alkenes Creates Adhesive and Self-Healing Materials
Damon J. Gilmour, Tanja Tomković, Nirmalendu Kuanr, Mitchell R. Perry, Hans Gildenast, Savvas G. Hatzikiriakos, Laurel L. Schafer
Abstract
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).