Topological network design toward high‐performance vegetable oil–based elastomers

As a kind of bio‐derived feedstock, vegetable oil (VO) shows great potential to replace petroleum‐based monomers to develop sustainable polymer materials because of its easy availability, low cost, bio‐renewable, and environmentally friendly nature. However, due to the high cross‐linking density and amorphous nature, directly cured VOs generally tend to be brittle and weak. To date, it is still difficult to adopt VOs and their derivatives as structural materials to prepare high‐performance elastomers. To address this important issue, a multi‐scale topology design strategy was proposed in this work. First, topology regulation and functionalization of VO‐based networks were realized by managing functional groups proportion during the bulk polymerization of epoxidized soybean oil with dimer fatty acids. Furthermore, a second polymer (SN) network was introduced into the VO‐based network as a protective layer via interfacial cross‐links. The generated VO‐based elastomers (VOEs) exhibit unprecedented comprehensive properties (VO content ≥70 wt.%, T g as low as −24.4°C, toughness up to 6.8 MJ/m 3 ). Besides, the VOEs also exhibit excellent reprocessability and self‐healing capability. Overall, this work developed a novel kind of VOEs with significant comprehensive advantages and provided important inspiration for the preparation of high‐performance elastomers through multi‐scale topology regulation.