Stretchable elastomer composites with segregated filler networks: effect of carbon nanofiller dimensionality

Electrically conductive elastomer composites (CECs) have great potential in wearable and stretchable electronic applications. However, it is often challenging to trade off electrical conductivity and mechanical flexibility in melt-processed CECs for wearable electronic applications. Here, we develop CECs with high electrical conductivity and mechanical elasticity by controlling the segregated networks of carbon nanofillers formed at the elastomer interface. The carbon nanofiller dimensionality has a significant influence on the electrical and mechanical properties of thermoplastic polyurethane (TPU) composites. For instance, 3D branched carbon nanotubes (carbon nanostructures, CNSs) have a very low percolation threshold (phi(C) = 0.01 wt%), which is about 8-10 times lower than that of 1D carbon nanotubes (CNTs) and 2D graphene nanosheets (GNSs). Besides, the TPU/CNS system has a higher electrical conductivity than other fillers at all filler contents (0.05-2 wt%). On the other hand, TPU/CNT systems can retain high elongation at break, whereas for the TPU/GNS systems elongation at break is severely deteriorated, especially at a high filler content. Different electrical and mechanical properties in the TPU-based CECs enable potential applications in flexible conductors/resistors and stretchable strain sensors, respectively.