Mechanically Enhanced and Reprocessable Vanillin-Based Epoxy Resin via Synergistic Effect of Rigid Cross-Linked Networks and Alkyl Dangling Chains

The cross-linked network structure of epoxy resins gives them excellent mechanical properties and heat resistance. However, it also makes them difficult to reprocess and recycle. This leads to environmental pollution and resource waste. Dynamic covalent bonds can make epoxy resins reprocessable. However, this involves a hard trade-off: adding flexible segments improves processing stability at the cost of mechanical strength, whereas keeping a rigid backbone retains the initial strength but leads to incomplete network reformation after multiple reprocessing cycles. As a result, performance continues to decrease. To solve this problem, this paper proposes a new strategy. It combines rigid cross-linked networks with alkyl dangling chains. The strategy does not sacrifice the rigid backbone of the epoxy. Instead, the alkyl dangling chains form physical entanglements during reprocessing. These entanglements compensate for the loss of chemical cross-linking density. Thus, the mechanical properties are retained or even enhanced. A vanillin-based Schiff base epoxy system was used. Alkyl dangling chains of different lengths were compared, and the results show that the system with longer alkyl dangling chains had higher mechanical properties after three reprocessing cycles; its tensile toughness increased by 85.7% compared to the system without dangling chains. At the same time, its thermal stability and glass transition temperature remained almost unchanged. This strategy effectively solves the conflict between strength and processing stability in reprocessable epoxy resins, as well as providing a new idea for designing green, high-performance, and closed-loop recyclable epoxy materials.