Disulfide Exchange Reactions: The Bridge Between Processability, Performance, and High‐Throughput Recyclability in Crosslinked Elastomers

Abstract Developing crosslinked elastomers that are easily produced and easily recyclable is complex, usually requiring a compromise between performance and recyclability. However, combining reversible exchange reactions together with phase separation phenomena appears as a promising approach. Herein, a simple and up‐scalable extrusion process is proposed, involving commercial maleated ethylene propylene rubber (EPRgMA), maleated polypropylene (PPgMA), and a suitable crosslinker. It is shown that a crosslinker enabling disulfide exchange reactions can provide local and long‐range rearrangements required for extrusion, yielding a robust crosslinked blend (BlendSS) with strength of 15 MPa and an impressive elongation of 1000%. Moreover, the presence of the disulfide crosslinker provided the required fast exchanges for three repetitive recycling cycles by extrusion with close to 80% retention of initial properties. In comparison, the use of a crosslinker without the capability to establish reversible reactions (BlendCC), yielded crosslinked blends of marginal compatibility, strength of 4 MPa and only 40% elongation. The absence of reversible reactions restricted chain rearrangements and consecutive recycling is only possible by compression molding. The recycled blends presented even lower compatibility, elasticity and thermomechanical performance, demonstrating that the proper design of interfacial interactions between PPgMA and EPRgMA can build a bridge between processability, performance, and high‐throughput recyclability.