Self-assembly of C4H-type hydrogenated graphene

Abstract

We demonstrate by molecular dynamic (MD) simulations that patterned partially hydrogenated graphene (C₄H) can self-assemble at room temperature. The main driving force of the self-assembly of C₄H is due to the one-sided distribution of hydrogen and the corresponding asymmetric orientation of sp³ bonding, there exists strong electrostatic repulsion between the relatively close H atoms. The simulations show that C₄H can self-assemble into various carbon nanoscroll (CNS) structures, this is mainly controlled by its geometry (size and aspect ratio). And the carbon nanotube (CNT) is a good candidate to activate and guide C₄H to form CNS, whose core size can be controlled. Meanwhile, a novel CNT/C₄H core/shell composite nanostructure is also formed. The theoretical results shed important light on a feasible approach to fabricate high-quality CNS and other novel nanostructures including core/shell structures, which hold great potential applications in optics, optoelectronic devices, hydrogen storage, sensors, and energy storage in supercapacitors or batteries.