【ACS Appl. Polym. Mater.】Biobased Recyclable Dynamically Cross-Linked Thermosets with Rapid Reprocessability via Guanidine Urea Linkages and Multiple Hydrogen Bonding
writer：Ruyue Li, Zhen Yu, Hongyun Hu, Zhaobin Tang, Yanlin Liu
keywords：生物基，胍脲，氫鍵，快速加工
source：期刊
Issue time：2025年
Conventional thermoset polyureas suffer from inherent limitations in sustainability and recyclability due to their irreversible cross-linked networks and heavy dependence on fossil-derived feedstocks. Herein, we report a biobased molecular design strategy for recyclable thermosets, leveraging guanidine acetic acid and lysine diisocyanate to construct a dynamic cross-linked architecture featuring reversible guanidine urea linkages reinforced by multiple hydrogen bonding interactions. This design endows the resulting material with both outstanding mechanical performance and rapid catalyst-free reprocessability. The synthesized poly(guanidine urea) thermoset exhibits a tensile strength of up to 37 ± 8 MPa and a glass transition temperature of 86 °C, rivaling that of commercial polyureas. Remarkably, the material can be reprocessed within 30 min under 120 °C and 10 MPa without a catalyst. This work offers a versatile molecular engineering approach toward the full life-cycle design of high-performance thermosets and paves the way for the development of recyclable, biobased polymeric materials, marking a significant step toward sustainable polymer innovation.