Effect of the Processing on the Resistance–Strain Response of Multiwalled Carbon Nanotube/Natural Rubber Composites for Use in Large Deformation Sensors

The dispersion, electrical conductivities, mechanical properties and resistance–strain response behaviors of multiwalled carbon nanotube (MWCNT)/natural rubber (NR) composites synthesized by the different processing conditions are systematically investigated at both macro- and micro-perspectives. Compared with the solution and flocculation methods, the two roll method produced the best MWCNTs distribution since the materials are mixed by strong shear stress between the two rolls. An excellent segregated conductive network is formed and that a low percolation threshold is obtained (~1 wt.%) by the two roll method. Different from the higher increases in conductivity for the composites obtained by the solution and flocculation methods when the MWCNT content is higher than 3 wt.%, the composite prepared by the two roll method displays obvious improvements in its mechanical properties. In addition, the two roll method promotes good stability, repeatability, and durability along with an ultrahigh sensitivity (GF(max) = 974.2) and a large strain range (ε = 109%). The ‘shoulder peak’ phenomenon has not been observed in the composite prepared by the two roll method, confirming its potential for application as a large deformation monitoring sensor. Moreover, a mathematical model is proposed to explain the resistance–strain sensing mechanism.