Efficient Hydrogen Storage in Defective Graphene and its Mechanical Stability: A Combined Density Functional Theory and Molecular Dynamics Simulation Study

A combined density functional theory and molecular dynamics approach is employed to study modifications of graphene at atomistic level for better H2 storage. The study reveals H₂ desorption from hydrogenated defective graphene structure, V₂₂₂, to be exothermic. H₂ adsorption and desorption processes are found to be more reversible for V₂₂₂ as compared to pristine graphene. Our study shows that V₂₂₂ undergoes brittle fracture under tensile loading similar to the case of pristine graphene. The tensile strength of V₂₂₂ shows slight reduction with respect to their pristine counterpart, which is attributed to the transition of sp2 to sp3-like hybridization. The study also shows that the V₂₂₂ structure is mechanically more stable than the defective graphene structure without chemically adsorbed hydrogen atoms. The current fundamental study, thus, reveals the efficient recovery mechanism of adsorbed hydrogen from V₂₂₂ and paves the way for the engineering of structural defects in graphene for H₂ storage.