High toughness, healable, self-cleaning polydimethylsiloxane elastomers with “rigid-while-flexible” mutual network structure

Polydimethylsiloxane (PDMS) elastomers with high mechanical and healing properties are developed as smart materials for electrical power systems and electronic devices to address electrical or mechanical damage. However, the challenge is to reconcile the conflicting molecular mechanisms of mechanical and healing properties in the development of PDMS elastomers. This study adopts the "rigid-while-flexible" mutual network structure by copolymerizing the rigid polyimide (PI) with flexible segments with dynamic reversible crosslinking designed on the PDMS backbones. This elastomer (designated PSiPI) exhibits high toughness, tensile strength and elongation at break, as well as excellent healing efficiency and recyclability. Moreover, the PSiPI elastomer also exhibits good insulation and corona damage healing properties. Taking advantage of the recyclability and healing properties of PSiPI elastomers, healable superhydrophobic coatings with contact angles greater than 150° have been prepared by compositing PSiPI elastomers with SiO₂. Likewise, combining the elastomer with conductive materials can create a healing flexible conductor. This "rigid-while-flexible" design approach provides important inspiration for the development of high-performance, sustainable and environmentally friendly PDMS elastomers for electrical and electronic applications.