Fabrication of Highly Thermally Resistant and Self‐Healing Polysiloxane Elastomers by Constructing Covalent and Reversible Networks

Abstract

AbstractThe fabrication of self‐healing elastomers with high thermal stability for use in extreme thermal conditions such as aerospace remains a major challenge. A strategy for preparing self‐healing elastomers with stable covalent bonds and dynamic metal–ligand coordination interactions as crosslinking sites in polydimethylsiloxane (PDMS) is proposed. The added Fe (III) not only serves as the dynamic crosslinking point at room temperature which is crucial for self‐healing performance, but also plays a role as free radical scavenging agent at high temperatures. The results show that the PDMS elastomers possessed an initial thermal degradation temperature over 380 °C and a room temperature self‐healing efficiency as high as 65.7%. Moreover, the char residue at 800 °C of PDMS elastomer reaches 7.19% in nitrogen atmosphere, and up to 14.02% in air atmosphere by doping a small amount (i.e., 0.3 wt%) of Fe (III), which is remarkable for the self‐healing elastomers that contain weak and dynamic bonds with relatively poor thermal stability. This study provides an insight into designing self‐healing PDMS‐based materials that can be targeted for use as high‐temperature thermal protection coatings.