Graphene in Ionic Liquids: Collective van der Waals Interaction and Hindrance of Self-Assembly Pathway

Over the past decade, there has been much controversy regarding the microscopic mechanism by which the π-electron-rich carbon nanomaterials such as graphene and carbon nanotubes can be dispersed in ionic liquids. Through a combination of a quantum mechanical calculation on the level of density functional theory, an extensive molecular dynamics study on the time scale of microseconds, and a kinetic analysis at the experimental time scale, we have demonstrated that collective van der Waals forces between ionic liquids and graphene are able to describe both the short-ranged cation−π interaction and the long-ranged dispersion interaction and this microscopic interaction drives two graphene plates trapped in their metastable state while two graphene plates easily self-assemble into graphite in water.