Computational Prediction of New Hydrocarbon Materials: The Hydrogenated Forms of Graphdiyne

Periodic density functional theory calculations were used to assess the thermodynamic stability of the hydrogenated forms of graphdiyne. The sp carbons of graphdiyne films in principle can be hydrogenated to generate extended two-dimensional hydrocarbons that consist of benzene rings linked with either sp 2 or sp 3 carbon chains. Free energy calculations for the addition of H 2 to graphdiyne suggest that the fully hydrogenated form of the material (“graphbutane”) is thermodynamically favored up to very high temperatures. This prediction opens up the possibility of tailoring the electronic properties of graphdiyne via hydrogenation.