Construction of a Transparent, Robust, Shape-Memory and Self-Healing MDI-Based Polyurethane Elastomer

Integrating strong mechanical properties and excellent optical properties for self-healing materials is challenging in both academia and industry. Robust self-healing polyurethane elastomers are expected to have superior mechanical properties, transparency, remarkable healing capability, and shape-memory performance via the adjustment of chemical and microphase separation structure. Herein, a robust transparent self-healable 4,4'-diphenylmethane diisocyanate (MDI)-based polyurethane elastomer containing disulfide bonds and branched structure (MPUE-SS) was synthesized. The chemical and topological structures, compatibility of soft-hard phases, and hard domain size of polyurethane could be adjusted via branched structure and mixed chain extender containing disulfide bonds and 1,4-butanediol (BDO), leading to enhanced self-healing, transparency, and mechanical properties. MPUE-SS exhibited a maximal tensile strength of 40 MPa. The microphase separation structure and reduced crystallinity led to a high transparency of about 91%, close to that of alicyclic polyurethane elastomers. After cutting in half and splicing, the MPUE-SS film recovered more than 95% of the original mechanical properties in 24 h. The shape recovery ratio at 40 °C and shape fixity ratio at -20 °C of MPUE-SS were 96.0% and 99.6%, respectively, higher than those of MPUE without disulfide bonds. Therefore, the chemical, topological structures, and microphase separation of polyurethane could be adjusted to achieve desired self-healing, transparency, shape-memory, and mechanical properties.