Polyethylene vitrimers via silyl ether exchange reaction

Abstract Functional polyethylene (PE) bearing pendant hydroxyl groups was dynamically crosslinked via reactive extrusion using commercially available N,N′-Bis[3-(trimethoxysilyl)propyl] ethylenediamine (TMSPEDA). This fast and efficient way allowed to produce PE vitrimers without synthetic effort or use of solvents, which makes the process environmentally friendly and easy to upscale. The dynamic crosslinking transformed thermoplastic PE into an elastic solid with greatly improved melt strength as revealed by DMTA and rheology. Mechanical properties could be tuned by varying the amount of TMSPEDA crosslinker. All prepared vitrimers were sparingly soluble in xylene and were not affected by moisture demonstrating crosslinked character, improved solvent resistance and excellent hydrolysis resistance which is of great importance for industrial applications. Despite the crosslink nature of the material, the dynamic silyl ether exchange enabled processability and recyclability of this system using industrially relevant techniques like injection and compression molding.