Catalyst-Free Mechanochemical Recycling of Biobased Epoxy with Cellulose Nanocrystals

Mechanochemical vitrimerization, as a method to recycle cross-linked thermosets by converting the permanent network into a recyclable and reprocessable vitrimer network, inevitably requires a catalyst to accelerate the bond exchange reactions. Here, we demonstrate a catalyst-free approach to achieve the recycling of a cross-linked biobased epoxy into high-performance nanocomposites with cellulose nanocrystals (CNCs). CNCs provide abundant free hydroxyl groups to promote the transesterification exchange reactions while also acting as reinforcing fillers for the resultant nanocomposites. This technique introduces an effective way to fabricate high-performance thermoset nanocomposites based on recycled polymers in an ecofriendly way, promoting the recycle and reuse of thermosets as sustainable nanocomposites for different applications.