Elucidation of structure-to-property relationships of piezoresistive polymer-carbon nanotube nanocomposites

Polymeric nanocomposites (PNC) filled with carbon nanotubes (CNTs) possess superior multifunctionality, including electrical, thermal, and mechanical properties, making them an emerging family of advanced and multifunctional materials. In recent years, flexible polymer/CNT nanocomposites are increasingly being considered as promising alternatives to conventional smart materials. Their piezoresistive behaviours have led to many potential applications in strain sensing. Despite extensive experimental and theoretical research, the underlying mechanisms for polymer/CNT nanocomposites' piezoresistive behaviours have yet been elucidated. This paper reports comprehensive investigations on the mechanisms and the structure-to-property relationships of these piezoresistive nanocomposites. Quantitative analyses revealed that piezoresistivity of polymer/CNT nanocomposites is predominantly governed by the three mechanisms related to the strain-induced morphological evolution of the CNT network embedded in the polymer matrix. Furthermore, both CNT content and CNT alignment are key structural parameters that affect the contribution of different mechanisms on PNCs' piezoresistivity and the sensitivity of flexible PNCs as strain sensors. For PNC filled with high content of randomly dispersed CNTs, the piezoresistivity was predominantly caused by the breakage of a complex conductive network into two or more simpler conductive paths. For PNC filled with low content of highly aligned CNTs, the piezoresistivity was mainly contributed by the complete disruption of originally interconnected CNTs in electrically conductive pathways. (C) 2015 AIP Publishing LLC.