This study combines ¹ H NMR and chemometrics to determine optimal processing conditions for aromatic disulfide-based vitrimers, revealing a correlation between model reactions and vitrimer networks.

Disulfide-based epoxy vitrimers enable full relaxation without excess amine. Introducing up to 32% non-dynamic epoxy enhances material properties while maintaining dynamic features like repairability, recyclability, and reprocessability.

Chemical recycling of disulfide-based vitrimer carbon fiber composites offers a viable route for circular management of structural composite materials through recovery of both reinforcement fibers and matrix constituents. In this study, two vitrimer systems with different resin compositions but a common disulfide-containing hardener were evaluated to identify conditions enabling efficient network cleavage and fiber recovery. The influence of solvent and reducing agent systems was systematically assessed, leading to optimized conditions for effective matrix depolymerization while preserving carbon fiber integrity. Scale-up experiments demonstrated that the recycling process is transferable from small-scale coupons to larger laminates and continuous fiber composite architectures without loss of fiber structural performance. Recovered resin was successfully reprocessed into vitrimer-based films, demonstrating retained functionality and reprocessability. Overall, this work establishes a scalable chemical recycling strategy for carbon fiber reinforced vitrimer composites, supporting their integration into circular composite manufacturing frameworks.

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.