Chemisorption of hydrogen on graphene: insights from atomistic simulations

The properties of graphene can be chemically altered by changing its local binding configurations. In the present work, we investigate fundamentals of chemisorption of atomic hydrogen on graphene and its influence on mechanical properties of as-hydrogenated graphene by means of molecular dynamics simulations. Our simulation results indicate that there are diversiform hydrogen-graphene configurations formed in the chemisorption process. Especially, energetically favorable hydrogen pairs result in less even no atomic distortion of graphene than sp3 hybridization. The hydrogenation-induced deterioration of mechanical properties of graphene shows a strong dependence on its chirality. The evolution of bond structures in uniaxial tension along armchair direction is more sensitive to local failure of graphene than zigzag direction, leading to a more pronounced decrease in both fracture stress and fracture strain. It is indicated that the chemisorption of hydrogen on graphene can be strongly affected by operating temperature primarily due to the temperature dependent graphene morphology. These findings advance our understanding of chemical vapor deposition of graphene synthesis and hydrogenation of graphene.