Constructing High-Transparency, Self-Healing and Reprocessable Poly(thiourethane) Elastomers Based on Zn2+-Multidentate Pyrimidine Coordination

To develop self-healing polyurethane materials with high transparency and superior mechanical performance, in this work, the poly(thiourethane) elastomers were prepared by incorporating the dynamic thiourethane bonds via thiol–isocyanate click reaction, followed by the addition of 1-(3-aminopropyl)imidazole (IZ), 3-hydroxypyridine (HP), and 2,4-diamino-6-hydroxypyrimidine (HPM) as ligands to produce three different polyurethane networks (named PTU-IZ, PTU-HP, and PTU-HPM). Zinc chloride (ZnCl2) was further introduced to construct metal-coordinated crosslinking networks, recorded as PTU-IZ-Zn, PTU-HP-Zn, and PTU-HPM-Zn, respectively. The effects of ligands and Zn2+ coordination on the materials’ optical transmittance, mechanical properties, self-healing capability, and reprocessability were systematically investigated. The results demonstrate that HPM and Zn2+ will facilitate the formation of more effective crosslinking, which significantly enhances the mechanical properties of PTU-HPM from 4.61 MPa up to 9.04 MPa (PTU-HPM-Zn), while maintaining high transparency (89.0% light transmittance at 650 nm). Self-healing tests reveal that the PTU-HPM-Zn scratches can fully repair within 4 h at 70 °C. Reprocessability tests demonstrate that the internal crosslinked network of the material undergoes reversible dissociation, enabling a topological transition from a crosslinked to a linear structure and thereby imparting excellent thermal reprocessability. This study provides novel insights for the design and fabrication of high-performance transparent self-healing polyurethane materials.