The Adsorption of Aromatic Macromolecules on Graphene with Entropy-tailored Behavior and Its Utilization in Exfoliating Graphite

Abstract Aromatic macromolecules tend to form a compact conformation after physically adsorbed on graphene and it brings about great entropy loss for physisorption, due to the strong interaction between aromatic macromolecules and graphene. However, previous researches have validated the availability of aromatic macromolecules to stabilize graphene based on physisorption. In order to clarify the underlying mechanism of this physisorption process on graphene, a series of aromatic polyamide copolymers are used as models in this research. Apart from their adsorbed conformations on graphene, the conformations of these copolymers as the free states in diluted solutions are taken into consideration. Although these copolymers present the fully extended conformation on graphene, their conformations in diluted solutions vary largely with the copolymer composition. It is verified that the copolymer with smaller conformational change could have the better stabilization effectiveness for graphene, rather than the one having stronger interaction with graphene. Therefore, the entropy-tailored behavior for the adsorption of aromatic macromolecules on graphene is put forward. Based on this mechanism, the chemical structure of aromatic polyamide is optimized and furthermore it is utilized to directly exfoliate natural graphite flakes. Eventually, high-quality graphene nanosheets with a large dimension and low defects are obtained. Moreover, its exfoliating effectiveness is superior to those of the commonly used exfoliating agents nowadays.