Reprocessable Polyhydroxyurethane Network Composites: Effect of Filler Surface Functionality on Cross-link Density Recovery and Stress Relaxation

Conventional polymer network composites cannot be recycled for high-value applications because of the presence of permanent covalent cross-links. We have developed reprocessable polyhydroxyurethane network nanocomposites using silica nanoparticles with different surface functionalities as reinforcing fillers. The property recovery after reprocessing is a function of the interaction between the filler surface and the network matrix during the network rearrangement process. When nonreactive silica nanoparticles lacking significant levels of surface functional groups are used at 4 wt % (2 vol %) loading, the resulting network composite exhibits substantial enhancement in mechanical properties relative to the neat network and based on values of rubbery plateau modulus is able to fully recover its cross-link density after a reprocessing step. When nanoparticles have surface functional groups that can participate in dynamic chemistries with the reprocessable network matrix, reprocessing leads to losses in mecha...