A facile one-pot route to elastomeric vitrimers with tunable mechanical performance and superior creep resistance

The transfer of vitrimer concept to diene-rubber materials can enable these thermosets with thermo-activated malleability and reprocessability. However, there are still significant gaps in the knowledge of introducing dynamic covalent bonds-based networks directly into rubber matrix without the need for elaborated modification of the molecular architecture. Herein, we demonstrate a one-pot approach to prepare covalently cross-linked diene-rubbers by engineering dynamic silyl ether linkages into the networks. Specifically, based on a thermally initiated thiol-ene reaction, silyl ether-based networks were directly achieved through incorporating silyl ether-containing multifunctional thiols (SE-T x ) into commercially available diene-rubber. The mechanical and dynamic behaviors of the resulting networks can be rationally tuned upon the regulation of the content and functionality of SE-T x cross-linkers. In addition, by virtue of the thermal stability of silyl ether linkages, the resulting networks feature with superior creep resistance at moderate temperatures, while the corresponding network rearrangement ability at elevated temperatures is barely affected, enabling the networks with malleability and recyclability.