Fused Filament Fabrication of a Dynamically Crosslinked Network Derived from Commodity Thermoplastics

[Image: see text] A massive carbon footprint is associated with the ubiquitous use of plastics and their afterlife. Greenhouse gas (GHG) emissions from plastics are rising and increasingly consuming the global “carbon budget”. It is, hence, paramount to implement an effective strategy to reclaim postconsumer plastic as feedstock for technologically innovative materials. Credible opportunity is offered by advances in materials chemistry and catalysis. Here, we demonstrate that by dynamically crosslinking thermoplastic polyolefins, commodity plastics can be upcycled into technically superior and economically competitive materials. A broadly applicable crosslinking strategy has been applied to polymers containing solely carbon–carbon and carbon–hydrogen bonds, initially by maleic anhydride functionalization, followed by epoxy–anhydride curing. These dynamic networks show a distinct rubber modulus above the melting transition. We demonstrate that sustainability and performance do not have to be mutually exclusive. The dynamic network can be extruded into a continuous filament to be in three-dimensional (3D) printing of complex objects, which retain the mechanical integrity of vitrimers. Being covalently crosslinked, these networks show a thermally triggered shape-memory response, with 90% recovery of a programmed shape. This study opens up the possibility of reclaiming recycled thermoplastics by imparting performance, sustainability, and technological advances to the reprocessed plastic.