Molecular beam study of the apparent activation barrier associated with adsorption and desorption of hydrogen on copper

Balooch, M.; Cardillo, M. J.; Miller, David R.; Stickney, R. E.

doi:10.1016/0039-6028(74)90315-x

Cited by 411 publications

(65 citation statements)

References 17 publications

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“…Many previous researches showed that the catalytic properties of clusters are structure dependent, leading to different adsorption energies and sites for different structures of clusters [1][2][3][4][5][6]. Hydrogen is employed in many modern technologies [7][8][9][10][11][12][13][14][15][16][17][18][19][20][21], so surface reactions of hydrogen molecules in transition metals have been carried out over the adsorption and desorption of hydrogen and deuterium molecules on well-defined single crystal metals. Axel Pramann et al [22] studied hydrogen chemisorption rates and electronic structures of small Nb n Al -clusters by photoelectron spectroscopic method.…”

Section: Introductionmentioning

confidence: 99%

Theoretical Study of Hydrogen Adsorption on Ruthenium Clusters

Yan

Jing

et al. 2011

J Clust Sci

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The geometries, stabilities, electronic, and magnetic properties of hydrogen adsorption on Ru n clusters have been systematically investigated by using density functional theory with generalized gradient approximation. The result indicates the absorbed species does not lead to a rearrangement of the basic cluster. For n [ 2, three different adsorption patterns are found for the Ru n H 2 complexes: One H atom binds to the Ru top site, and another H binds to the bridge site for n = 3, 5, 6, 8; bridge site adsorption for n = 4; hollow site and top site adsorption for n = 7. The adsorption energies display oscillation and reach the peak at n = 2, 4, 7, implying their high chemical reactivity. The small electron transferred number between H atoms and Ru n clusters indicates that the interaction between H atoms and Ru n clusters is small. When H 2 is absorbed on the Ru n clusters, the chemical activity of corresponding clusters is dramatically increased. The absorbed H 2 can lead to an oscillatory behavior of the magnetic moments, and this behavior is rooted in the electronic structure of the preceding cluster and the changes in the magnetic moment are indicative of the relative ordering of the majority and minority LUMO's. The second order difference indicates 5 is magic number in Ru n H 2 and Ru n clusters.

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Section: Introductionmentioning

confidence: 99%

Theoretical Study of Hydrogen Adsorption on Ruthenium Clusters

Yan

Jing

et al. 2011

J Clust Sci

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“…In favorable cases, the state distributions of the gaseous products of thermally driven associative desorption (the time reversal of dissociative chemisorption) can provide information about dissociative sticking through the principle of detailed balance. 3,4 For hydrogen dissociative chemisorption on Cu(111), detailed balance applied to associative desorption has shown that molecular vibrational energy and rotational energy are not as efficacious in promoting dissociative chemisorption as either molecular translational energy directed along the surface normal, 5,6 or surface thermal energy. 7 Studies of methane dissociative chemisorption on metals have also shown that energy from both the incident molecules 8,9 and the surface 10 can promote reactivity.…”

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confidence: 99%

Communication: Angle-resolved thermal dissociative sticking of CH4 on Pt(111): Further indication that rotation is a spectator to the gas-surface reaction dynamics

Navin

Donald

Tinney

et al. 2012

The Journal of Chemical Physics

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Effusive molecular beam measurements of angle-resolved thermal dissociative sticking coefficients for CH4 impinging on a Pt(111) surface, at a temperature of 700 K, are reported and compared to theoretical predictions. The reactivity falls off steeply as the molecular angle of incidence increases away from the surface normal. Successful modeling of the thermal dissociative sticking behavior, consistent with existent CH4 supersonic molecular beam experiments involving rotationally cold molecules, required that rotation be treated as a spectator degree of freedom.

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“…The results of experiments measuring the dependence of the dissociation probability on the incidence angle, translational energy, and the rovibrational state of the molecule [1][2][3][4][5][6][7][8][9][10][11][12][13] are available as benchmarks to which the results of computational models can be compared. To date, a full six-dimensional ͑6D͒ quantum mechanical description of activated dissociation of H 2 has not yet been carried out but low-dimensional models treating the most important coordinates have successfully explained many experimental observations.…”

Section: Introductionmentioning

confidence: 99%

Dissociative adsorption of H2 on Cu(100): A four-dimensional study of the effect of rotational motion on the reaction dynamics

Mowrey

Kroes

Wiesenekker

et al. 1997

The Journal of Chemical Physics

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The reaction of H 2 on Cu͑100͒ is investigated using a four-dimensional ͑4D͒ quantum dynamical fixed-site model to assess the influence of molecular rotation on dissociation over the most reactive ͑the bridge͒ site. The potential energy surface ͑PES͒ is a fit to the results of density functional calculations performed using a generalized gradient approximation treating a Cu slab with a periodic overlayer of H 2 . Dissociation probabilities for molecules with ''helicoptering'' (m j ϭ j) and ''cartwheeling'' ͑m j ϭ0͒ rotational motions are here found to be comparable because of the strong corrugation in the azimuthal coordinate. The calculations indicate that reaction is accompanied by significant rotationally inelastic scattering. Surprisingly, vibrational excitation is also found to be an efficient process in collisions with the reactive bridge site. In these collisions, the molecular axis is tilted away from the orientation parallel from the surface. Considering the approximate nature of the 4D model used, the calculated reaction probabilities are in good agreement with experiment, indicating that the PES that was used is accurate.

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Molecular beam study of the apparent activation barrier associated with adsorption and desorption of hydrogen on copper

Cited by 411 publications

References 17 publications

Theoretical Study of Hydrogen Adsorption on Ruthenium Clusters

Theoretical Study of Hydrogen Adsorption on Ruthenium Clusters

Communication: Angle-resolved thermal dissociative sticking of CH4 on Pt(111): Further indication that rotation is a spectator to the gas-surface reaction dynamics

Dissociative adsorption of H2 on Cu(100): A four-dimensional study of the effect of rotational motion on the reaction dynamics

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