Self-Healing Thermoplastic Polyurethane Linked via Host-Guest Interactions

High toughness with self-healing ability has become the ultimate goal in materials research. Herein, thermoplastic polyurethane (TPU) was linked via host-guest (HG) interactions to increase its mechanical properties and self-healing ability. TPU linked via HG interactions was prepared by the step-growth bulk polymerization of hexamethylene diisocyanate (HDI), tetraethylene glycol (TEG), and HG interactions between permethylated amino βCD (PMeAmβCD) and adamantane amine (AdAm). TPU linked with 10 mol% of HG interactions (HG(10)) showed the highest rupture stress and fracture energy (G(F)) of 11 MPa and 25 MJ·m(−3), which are almost 40-fold and 1500-fold, respectively, higher than those of non-functionalized TEG-based TPU (PU). Additionally, damaged HG(10) shows 87% recovery after heated for 7 min at 80 °C, and completely cut HG(10) shows 80% recovery after 60 min of reattachment at same temperature. The HG interactions in TPU are an important factor in stress dispersion, increasing both its mechanical and self-healing properties. The TPU linked via HG interactions has great promise for use in industrial materials in the near future.