Adsorption of hydrogen atoms on a single graphite sheet (graphene) has been investigated by first-principles electronic structure means, employing plane-wave based, periodic density functional theory. A reasonably large 5x5 surface unit cell has been employed to study single and multiple adsorption of H atoms. Binding and barrier energies for sequential sticking have been computed for a number of configurations involving adsorption on top of carbon atoms. We find that binding energies per atom range from ~0.8 eV to ~1.9 eV, with barriers to sticking in the range 0.0-0.2 eV. In addition, depending on the number and location of adsorbed hydrogen atoms, we find that magnetic structures may form in which spin density localizes on a $\sqrt{3}{x}\sqrt{3}{R}30^{\circ}$ sublattice, and that binding (barrier) energies for sequential adsorption increase (decrease) linearly with the site-integrated magnetization. These results can be rationalized with the help of the valence-bond resonance theory of planar $\pi$ conjugated systems, and suggest that preferential sticking due to barrierless adsorption is limited to formation of hydrogen pairs.

Understanding adsorption of hydrogen atoms on graphene / S. Casolo, O.M. Løvvik, R. Martinazzo, G.F. Tantardini. - In: THE JOURNAL OF CHEMICAL PHYSICS. - ISSN 0021-9606. - 130:5(2009 Feb 07), pp. 054704.1-054704.10.

Understanding adsorption of hydrogen atoms on graphene

S. Casolo
Primo
;
R. Martinazzo
Penultimo
;
G.F. Tantardini
Ultimo
2009-02-07

Abstract

Adsorption of hydrogen atoms on a single graphite sheet (graphene) has been investigated by first-principles electronic structure means, employing plane-wave based, periodic density functional theory. A reasonably large 5x5 surface unit cell has been employed to study single and multiple adsorption of H atoms. Binding and barrier energies for sequential sticking have been computed for a number of configurations involving adsorption on top of carbon atoms. We find that binding energies per atom range from ~0.8 eV to ~1.9 eV, with barriers to sticking in the range 0.0-0.2 eV. In addition, depending on the number and location of adsorbed hydrogen atoms, we find that magnetic structures may form in which spin density localizes on a $\sqrt{3}{x}\sqrt{3}{R}30^{\circ}$ sublattice, and that binding (barrier) energies for sequential adsorption increase (decrease) linearly with the site-integrated magnetization. These results can be rationalized with the help of the valence-bond resonance theory of planar $\pi$ conjugated systems, and suggest that preferential sticking due to barrierless adsorption is limited to formation of hydrogen pairs.
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Utilizza questo identificativo per citare o creare un link a questo documento: http://hdl.handle.net/2434/66918
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