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Vitrimers - a class of polymer networks which are covalently crosslinked andinsoluble like thermosets, but flow when heated like thermoplastics - containdynamic links and/or crosslinks that undergo an associative exchange reaction.These dynamic crosslinks enable vitrimers to have interestingmechanical/rheological behavior, self-healing, adhesive, and shape memoryproperties. We demonstrate that vitrimers can self-assemble into complex meso-and nanostructures when crosslinks and backbone monomers strongly interact.Vitrimers featuring polyethylene (PE) as the backbone and dioxaborolanemaleimide as the crosslinkable moiety were studied in both the molten andsemi-crystalline states. We observed that PE vitrimers macroscopically phaseseparated into dioxaborolane maleimide rich and poor regions, and characterizedthe extent of phase separation by optical transmission measurements. This phaseseparation can explain the relatively low insoluble fractions and overallcrystallinities of PE vitrimers. Using synchrotron-sourced small-angle X-rayscattering (SAXS), we discovered that PE vitrimers and their linear precursorsmicro-phase separated into hierarchical nanostructures. Fitting of the SAXSpatterns to a scattering model strongly suggests that the nanostructures -which persist in both the melt and amorphous fraction of the semi-crystallinestate - may be described as dioxaborolane maleimide rich aggregates packed in amass fractal arrangement. These findings of hierarchical meso- andnanostructures point out that incompatibility effects between networkcomponents and resulting self-assembly must be considered for understandingbehavior and the rational design of vitrimer materials.

Phase separation and self-assembly in vitrimers: hierarchical morphology of molten and semi-crystalline polyethylene/dioxaborolane maleimide systems