Controlled 3D Assembly of Graphene Sheets to Build Conductive, Chemically Selective and Shape-Responsive Materials

Driven by the surface activity of graphene, electrically conductive elastomeric foams have been synthesized by the controlled reassembly of graphene sheets; from their initial stacked morphology, as found in graphite, to a percolating network of exfoliated sheets, defining hollow spheres. This network creates a template for the formation of composite foams, whose swelling behavior is sensitive to the composition of the solvent, and whose electrical resistance is sensitive to physical deformation. The self-assembly of graphene sheets is driven thermodynamically, as graphite is found to act as a 2D surfactant and is spread at high-energy interfaces. This spreading, or exfoliation, of graphite at an oil/water interface stabilizes water-in-oil emulsions, without the need for added surfactants or chemical modification of the graphene. Using a monomer such as butyl acrylate for the emulsion's oil phase, elastomeric foams are created by polymerizing the continuous oil phase. Removal of the aqueous phase then results in robust, conductive, porous, and inexpensive composites, with potential applications in energy storage, filtration, and sensing.