Advancing Thermoset Technology: 4R Materials with Unchanged Mechanical Properties and Enhanced Sustainability Through Repellency, Recyclability, Reprocessability, and Repairability

In this work, we present the development of a novel thermoset epoxy network that combines highly dynamic characteristics (reprocessability, reparability, and recyclability, 3R) with enhanced surface repellency. The conventional dynamic hardener of a 3R epoxy network was partially substituted with two different polydimethylsiloxane (PDMS) compounds at varying weight percentages and molecular weights, allowing us to systematically evaluate their influence on the material's properties. Mechanical, thermal, and dynamic characteristics were retained, confirming that the substitution does not compromise the functional integrity of the network. Importantly, the surface properties were significantly improved, demonstrating enhanced repellency without affecting the core 3R functionality. A comparative analysis of the two PDMS variants revealed the influence of chemical structure and molecular weight on surface performance, providing insights into the design of multifunctional, sustainable epoxy networks.