Malleable and Recyclable Vitrimer–Graphene Aerogel Composite with High Electrical Conductivity

In this work, we report a flexible conductive composite based on a graphene aerogel (GA) and polyimine vitrimer. Unlike the conventional thermosetting matrix, polyimine vitrimer enables the resulting composite to have not only good mechanical properties and chemical stability but also the capabilities of bending, stretching, rehealing, and closed-loop recycling. Notably, the three-dimensional interconnected networks of the GA filler with intrinsic porosity that can accommodate the polyimine matrix endow the composite a high electrical conductivity of 161 S/m with only 5 wt % of GA loading, which is 8–30 times higher than that of the composites containing 5 wt % commercial graphene powder (19 S/m) or multiwalled carbon nanotubes (5 S/m), thus making the polyimine–GA composite promising for flexible electronic application. Furthermore, the recyclability of such composite enables the recovery and reuse of electronic waste, thus greatly reducing the environmental impact.