Hydrogen‐Bonding Mediated Cosolvency: Boosting Facile and Rapid Depolymerization of Epoxy Thermosets

Thermosetting polymers feature highly cross‐linked networks that are fundamentally distinct from those of thermoplastics. Even with similar cross‐linking point, their three‐dimensional architecture imposes significant mass transfer barriers and necessitates harsh, energy‐intensive degradation conditions. Overcoming these limitations to achieve efficient and low‐energy recycling of epoxy thermosets remains a major challenge. To address this challenge, this article developed a cosolvent‐enhanced diethylenetriamine (DETA) catalytic system that enables rapid and efficient degradation under mild conditions. This approach achieved complete decomposition within 30 min at 60°C, significantly reducing time and energy consumption compared to conventional methods. The cosolvents accelerate degradation by disrupting the resin morphology to enhance mass transport and activating the amine catalyst through hydrogen‐bonding interactions. This article provides a practical and sustainable pathway for recycling of thermosetting polymers, highlighting the potential of solvent‐catalyst synergy in promoting circular polymer economies.