Development of a Strong, Recyclable Poly(dimethylsiloxane) Elastomer with Autonomic Self‐Healing Capabilities and Fluorescence Response Properties at Room Temperature

Abstract With the recent emphasis on environmental protection measures, there are increasingly strong demands for environment‐friendly multifunctional materials, so research regarding high‐performance, recyclable, functional materials with self‐healing abilities is of great interest. However, the comprehensive mechanical properties of most available self‐healing materials are insufficient; to date, most developed materials are either tough but brittle or flexible but weak. This report describes the application of a crosslinking strategy based on multiple dynamic bonds for the development of an autonomically self‐healing, multifunctional, boroxine‐containing poly(dimethylsiloxane) elastomer (PDMS‐BN). This approach takes advantage of well‐designed intermolecular and intramolecular nitrogen‐coordinated boroxines by using a synergetic dynamic mechanism. The elastomers exhibit enhanced comprehensive mechanical properties (with maximum strength up to 1.72 MPa, elongation at break up to 307%, Young's modulus up to 11.18 ± 0.52 MPa, and toughness up to 4.92 MJ m −3 ) and highly autonomic self‐healing capabilities, with ≈96% efficiency at room temperature for 48 h. Moreover, the PDMS‐BN elastomer can be recycled multiple times via crushing/molding or disassembling/casting processes, without losing their original mechanical robustness. The as‐prepared elastomers also demonstrate good adhesive properties and a unique fluorescence‐quenching response in the presence of Fe 3+ ions.