1-D polymer ternary composites: Understanding materials interaction, percolation behaviors and mechanism toward ultra-high stretchable and super-sensitive strain sensors

A series of 1-D polymer ternary composites based on poly(styrene-butadiene-styrene) (SBS)/carbon nanotubes (CNTs)/few-layer graphene (FLG) conductive fibers (SCGFs) were prepared via wet-spinning. Employed as ultra-high stretchable and super-sensitive strain sensors, the ternary composite fiber materials’ interaction, percolation behaviors and mechanism were systematically explored. The resultant SCGFs-based strain sensors simultaneously exhibited high sensitivity, superior stretchability (with a gauge factor of 5,467 under 600% deformation) and excellent durability under different test conditions due to excellent flexibility of SBS, the synergistic effect of hybrid conductive nanofibers and the strong π-π interaction. Besides, the conductive networks in SBS matrix were greatly affected by the mass ratio of CNTs and FLG, and thus the piezoresistive performances of the strain sensors could be controlled by changing the content of hybrid conductive fillers. Especially, the SCGFs with 0.30 wt.% CNTs (equal to their percolation threshold 0.30 wt.%) and 2.7 wt.% FLG demonstrated the highest sensitivity owing to the bridge effect of FLG between adjacent CNTs. Whereas, the SCGFs with 1.0 wt.% CNTs (higher than their percolation threshold) and 2.0 wt.% FLG showed the maximum strain detection range (600%) due to the welding connection caused by FLG between the contiguous CNTs. To evaluate the fabricated sensors, the tensile and the cyclic mechanical recovery properties of SCGFs were tested and analyzed. Additionally, a theoretical piezoresistive mechanism of the ternary composite fiber was investigated by the evolution of conductive networks according to tunneling theory.