▎ 摘　　要

Understanding the adsorption and reaction between hydrogen and graphene is of fundamental importance for developing graphene-based concepts for hydrogen storage and for the chemical functionalization of graphene by hydrogenation. Recently, theoretical studies of single-sided hydrogenated graphene, so called graphone, predicted it to be a promising semiconductor for applications in graphene-based electronics. Here, we report on the synthesis of graphone bound to a Ni(111) surface. We investigate the formation process by X-ray photoelectron spectroscopy (XPS), temperature-programmed desorption (TPD), and density-functional theory calculations, showing that the hydrogenation of graphene with atomic hydrogen indeed leads to graphone, that is, a hydrogen coverage of 1 ML (4.2 wt%). The dehydrogenation of graphone reveals complex desorption processes that are attributed to coverage-dependent changes in the activation energies for the associative desorption of hydrogen as molecular H-2.