Changes to the dissociation barrier of H 2 due to buckling induced by a chemisorbed hydrogen on a doped graphene surface

• Published in: Journal of molecular modeling 2018-09, Vol.24 (9), p.244
• Main Authors: Hernández-Hernández, A, Vallejo, E, Martínez-Farías, F, Pelayo, J Jesus, Hernández-Hernández, L A, Pescador-Rojas, J A, Tamayo-Rivera, L, Morales-Peñaloza, A, López-Pérez, P A, Cortes, E Rangel
• Format: Article
• Language: English
• ISSN: 0948-5023
• DOI: 10.1007/s00894-018-3763-z

An effectiveway of enhancing hydrogen storage on adsorbent materials can be induced by the hydrogen spill-over mechanism, although to date there is no general consensus which satisfactorily explains the mechanism. In this work, a possible reaction path to explain hydrogen adsorption is shown. Density-functional calculations were used to study the dissociation of molecular hydrogen near to a stressed region, as a consequence of chemisorbed hydrogen at the graphene-nitrogen surface. We found that as a result of the buckling induced by the chemisorbed hydrogen, the dissociation barrier of molecular hydrogen diminished by 0.84 eV. The chemisorbed hydrogen is the final state in the spill-over mechanism on a graphene-nitrogen decorated with palladium clusters. This effect helps to create hydrogen nanoislands that may change the diffusion and detrapping of H. An electronic structure analysis suggests that these systems occasionally present metallic or semiconductor behavior. Graphical Abstract Hydrogen dissociation and adsorption process via buckling defect.