Preparation of Robust, Room-Temperature Self-Healable and Recyclable Polysiloxanes Based on Hierarchical Hard Domains

The contradiction between high mechanical strength and mild healing conditions has long existed in self-healing materials, which limits the application of self-healing materials. The preparation of robust materials with excellent healing performance under mild conditions can effectively reduce resource waste and environmental pollution. Herein, self-healing polysiloxane elastomer materials, APDMS-MDI-IPDI-Bs, based on microphase separation strategy are reported. Through the synergistic effect of the designed urea hydrogen bond and the nitrogen-coordinated boroxine structure, the materials can maintain high mechanical properties (maximum tensile strength up to 3.35 MPa, elongation at break up to 316%), while maintaining excellent self-healing and recyclable ability (24 h healing efficiency at room temperature can reach 94.77 +/- 3.23%), and the performance can be repeated many times without decay. APDMS-MDI-IPDI-Bs also exhibit unique hydrophobicity, expanding the application scenarios of materials containing boroxine structure.