Oligosiloxane-Based Epoxy Vitrimers: Adaptable Thermosetting Networks with Dual Dynamic Bonds

Embedding dynamic covalent bonds into polymer compositions transforms static thermosets into active materials with the reprocessability of thermoplastics and the bulk properties of cross-linked networks. This class of next-generation materials, called covalent adaptable networks, shows significant promise in composites, soft optoelectronics, and robotics. Herein, we synthesized two oligosiloxane-based epoxy networks that provide fast dynamic bond exchange. Oligosiloxane diepoxides were cured with stoichiometric amounts of 1,2-phenylenediacetic acid to generate epoxy acid networks with two dynamic covalent bonding mechanisms. The resulting polymer networks provided access to fast stress-relaxation times (1–10 min) at temperatures of only 130 °C with excellent reprocessability