Cellulose nanocrystals mediated assembly of graphene in rubber composites for chemical sensing applications

• Cellulose nanocrystals mediated assembly of graphene in natural rubber latex.
• NR/graphene composites with 3D conductive network and enhanced properties.
• The composites showed excellent resistance response to organic solvents.

In this study, we report a green assembled approach to prepare natural rubber (NR) composites with 3D interconnected graphene-based conductive networks. Taking advantage of the water-dispersity and amphiphilicity of cellulose nanocrystals (CNC), well suspended graphene@CNC aqueous colloids could be prepared by the CNC-mediated reduction of graphene oxide. When homogenized with NR latex under ultrasonication and subsequently co-coagulation, the graphene@CNC nanohybrids selectively located in the interstitial space between the NR latex microspheres and constructed an ordered 3D conductive structure. This unique 3D conductive network endowed the NR composites with remarkably enhanced electric conductivity (the percolation threshold is twofold lower than that of the conventional NR/graphene composites), mechanical properties and more importantly resistivity response to organic liquids. Our strategy offered a novel, simple and eco-friendly route for the fabrication of liquid sensors capable of sensing and discriminating various solvent leakage in chemical industry as well as environmental monitoring.