A hybrid reversible crosslinked polysiloxane elastomer with high toughness and recyclability

Abstract The preparation of polysiloxane elastomers with outstanding mechanical properties, self‐healing capabilities, and high recyclability remains a formidable challenge despite their promising application prospects in flexible electronic devices. Herein, the polysiloxane elastomer is fortified with a hybrid reversible crosslinked network, incorporating Diels‐Alder (D‐A) and disulfide bonds for chemical crosslinking, as well as multiple hydrogen bonds for physical crosslinking, to effectively address this challenge. The presence of D‐A covalent bonds not only enhances the stability of the polymer network but also facilitates the reconstruction of dynamic disulfide and hydrogen bonds as sacrificial bonds for dissipating energy. This design further enhances the toughness of the obtained elastomer while simultaneously providing self‐healing capabilities and recyclability. Specially, relying on the hybrid reversible crosslinked network, the resulting polysiloxane elastomer PDMS 3 ‐IPDI 4 ‐SS‐F‐M demonstrates exceptional mechanical performance, boasting a toughness of 13.6 MJ/m 3 . Moreover, it exhibits commendable self‐healing ability with a self‐healing efficiency of 92% at 65°C for 24 h, as well as high thermal stability and recyclability without necessitating chemical treatment for polymer chain decomposition. The elastomer exhibits promising prospects for application in sustainable flexible support materials.