Highly Conductive, Reconfigurable Nanocomposites of a Nanostructured Carbon Material and a Dynamic Polymer Network

Utilizing high aspect ratio nanofillers with exceptional electrical conductivity opens the opportunities for the fabrication of multifunctional conductive polymer composites (CPCs). However, achieving fine filler dispersion for advanced nanocomposite performance has remained challenging. Here, we report a fine dispersion of a carbon nanostructured material assisted by liquefication of dynamic polymer network dissociation via a temperature-reversible Diels-Alder (DA) reaction. The resulting DA polymer composites (DAPCs) demonstrate an ultra-low percolation threshold (0.04 wt. %) and high electrical conductivity of 4 S/m at only 1 wt. % filler loading. Dissociation of DA bonds under low-power electrical-assisted fast heating enables efficient healing of the composite networks. Moreover, the 3D printed DAPC network shows a unique shape memory behavior which can be reprogramed by tuning stereochemistry of DA attachments. This work introduced a new approach to address major challenges in polymer nanocomposites including good filler dispersity, enhanced electrical and mechanical properties, and 3D printability of CPCs.