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Changes to the dissociation barrier of H2 due to buckling induced by a chemisorbed hydrogen on a doped graphene surface

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Abstract

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.

Hydrogen dissociation and adsorption process via buckling defect

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Acknowledgements

Part of this work was performed at the CNMS and the Oak Ridge National Laboratory Leadership Computing Facility which is a US DOE Office of Science User Facility at ORNL Supported under contract no. DE-AC05-00OR22725. F. Martínez-Farías was partially supported by grant UAEHPTC764, DSA /5116/178021.

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Authors and Affiliations

  1. Escuela Superior de Apan, Energetic Systems and Advanced Materials, Universidad Autónoma del Estado de Hidalgo, Carretera Apan-Calpulalpan Km. 8, Col. Chimalpa, C.P. 43920, Apan, Hidalgo, México

    A. Hernández-Hernández, E. Vallejo, F. Martínez-Farías, J. Jesus Pelayo, L. A. Hernández-Hernández, J. A. Pescador-Rojas, L. Tamayo-Rivera, A. Morales-Peñaloza, P. A. López-Pérez & E. Rangel Cortes

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  1. A. Hernández-Hernández
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  2. E. Vallejo
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  3. F. Martínez-Farías
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  4. J. Jesus Pelayo
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  5. L. A. Hernández-Hernández
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  6. J. A. Pescador-Rojas
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  7. L. Tamayo-Rivera
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  8. A. Morales-Peñaloza
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  9. P. A. López-Pérez
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  10. E. Rangel Cortes
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Correspondence to F. Martínez-Farías or E. Rangel Cortes.

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Hernández-Hernández, A., Vallejo, E., Martínez-Farías, F. et al. Changes to the dissociation barrier of H2 due to buckling induced by a chemisorbed hydrogen on a doped graphene surface. J Mol Model 24, 244 (2018). https://doi.org/10.1007/s00894-018-3763-z

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  • DOI: https://doi.org/10.1007/s00894-018-3763-z

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