Manipulating the self-assembly behavior of graphene nanosheets via adenine-functionalized biodegradable polymers

Abstract

Electrically conductive supramolecular polymer composites, based on a combination of natural graphite and the adenine-functionalized biodegradable oligomer 3A-PCL, are able to directly exfoliate crystalline graphite into highly disordered graphene nanosheets with well-tailored structural and physical properties. Herein, we discover 3A-PCL can self-assemble into well-ordered lamellar nanostructures on the surface of graphite due to the strong affinity between 3A-PCL and graphite, and thus lead to direct exfoliation of graphite into well-suspended graphene nanosheets in an organic solvent. Furthermore, after drying, the resulting graphite/3A-PCL composites exhibit stable thermoreversible phase transition behavior between viscous and elastic states, and the number of graphene layers exfoliated can be controlled by tuning the content of 3A-PCL within the composites. Importantly, these newly developed graphene composites possess a low electrical resistivity of 1.5 ± 0.7 mΩ·cm at a graphite loading of 23 wt%, which is more than an order of magnitude lower than that of pristine graphite. Given the simplicity of the production process, well-tailored physical properties and excellent conductive performance, this development offers a highly efficient process for the fabrication of multifunctional supramolecular graphene nanosheets that holds great potential for conductive device applications.