Cellulose Nanocrystals: Accelerator and Reinforcing Filler for Epoxy Vitrimerization.

The novel vitrimerization concept of converting permanently cross-linked networks of thermoset polymers into dynamic exchangeable networks often relies on transesterification reactions. Transesterification exchange reactions, for example, in epoxy vitrimers, are usually contingent on equivalent ratios of hydroxyl to ester groups and large amounts of catalysts to achieve proper dynamic exchange capability. In general, postconsumer epoxy cured with anhydrides contains very few hydroxyl groups in the network, and it is challenging to convert it into efficient dynamic networks by vitrimerization. Here, we demonstrate that introducing cellulose nanocrystals as feedstock of external hydroxyl groups in the mechanochemical vitrimerization process could improve the exchange reaction rate as well as the thermomechanical properties of the vitrimerized epoxy. This work offers an effective way to recycle and reprocess postconsumer epoxy/anhydride waste with inherent low ratios of hydroxyl to ester groups into higher value-added vitrimer nanocomposites.