A Cross-linked Polyethylene with Recyclability and Mechanical Robustness Enabled by Establishment of Multiple Hydrogen Bonds Network via Reactive Melt Blending

Physical cross-linking by hydrogen-bonds (H-bonds), providing a good combination of application properties of thermosets and processability of thermoplastics, is a potential strategy to resolve the recycling problem of traditional chemically cross-linked polyethylene. However, ureidopyrimidone (UPy), the most widely used H-bonding motif, is unfavorable for large-scale industrial application due to its poor thermal stability. In this work, H-bonds cross-linked polyethylene was successfully prepared by reactive melt blending maleic anhydride grafted polyethylene (PE-g-MAH) with 3-amino-1,2,4-triazole (ATA) to form amide triazole ring-carboxylic acid units. Triazole ring can easily generate multiple H-bonds with carboxylic acid and amide. More importantly, these units are more thermal stable than UPy due to the absence of unstable urea group of UPy. The introduction of H-bonds cross-linking leads to an obvious improvement in mechanical properties and creep resistance and a good maintain in thermal properties and recyclability. Furthermore, the reinforcement effect monotonically improves with increasing the density of H-bonds. The obtained good properties are mainly attributed to largely enhanced interchain interactions induced by H-bonds cross-linking and intrinsic reversibility of H-bonds. This work develops a novel way for the simple fabrication of H-bonds cross-linked PE with high performance through reactive melt blending.