Implication of multi-walled carbon nanotubes on polymer/graphene composites

Highlights: • Influence of adding carbon nanotubes (CNTs) into elastomer/graphene composites. • Multi-walled CNTs work supplementally to GnPs by forming conductive networks. • The findings illuminate marked synergistic effect between MWCNTs and graphene sheets. - Abstract: Graphene sheets stack in polymer matrices while multi-walled carbon nanotubes (MWCNTs) entangle themselves, forming two daunting challenges in the design and fabrication of polymer composites. Both challenges have been simultaneously addressed in this study by hybridizing the two nanomaterials through melt compounding to develop elastomer/graphene platelet/MWCNT (3-phase) composites, where MWCNTs were fixed at 2.8 vol% (5 wt%) for all fractions. We investigated the composites' structure and properties, and compared the 3-phase composites with elastomer/graphene platelet (2-phase) composites. MWCNTs may bridge graphene platelets (GnPs) and promote their dispersion in the matrix, which would provide more interface area between the matrix and the fillers. MWCNTs worked supplementally to GnPs by forming conductive networks, where MWCNTs acted as long nanocables to transport electrons and stress while GnPs served as interconnection sites between the tubes forming local conductive paths. This produced a percolation threshold of electrical conductivity at 2.3 vol% for 3-phase composites, 88% lower than that of 2-phase composites. At 26.7 vol% of total filler content (MWCNTs + GnPs), tensile strength, Young's modulus and tear strength showed respectively 303%, 115%, 155% further improvements over those of 2-phase composites. These improvements are originated from the synergistic effect between GnPs and MWCNTs. The conducting elastomeric composites developed would potentially open the door for applications in automotive and aerospace industries