Protection from Below: Stabilizing Hydrogenated Graphene Using Graphene Underlayers

We show that dehydrogenation of hydrogenated graphene proceeds much more slowly for bilayer systems than for single layer systems. We observe that an underlayer of either pristine or hydrogenated graphene will protect an overlayer of hydrogenated graphene against a number of chemical oxidants, thermal dehydrogenation, and degradation in an ambient environment over extended periods of time. Chemical protection depends on the ease of oxidant intercalation, with good intercalants such as Br₂ demonstrating much higher reactivity than poor intercalants such as 1,2-dichloro-4,5-dicyanonbenzoquinone (DDQ). Additionally, the rate of dehydrogenation of hydrogenated graphene at 300 °C in H₂/Ar was reduced by a factor of roughly 10 in the presence of a protective underlayer of graphene or hydrogenated graphene. Finally, the slow dehydrogenation of hydrogenated graphene in air at room temperature, which is normally apparent after a week, could be completely eliminated in samples with protective underlayers over the course of 39 days. Such protection will be critical for ensuring the long-term stability of devices made from functionalized graphene.