Dissociative chemisorption of H2 on Cu(100): A four-dimensional study of the effect of parallel translational motion on the reaction dynamics

Kroes, G. J.; Wiesenekker, G.; Baerends, E. J.; Mowrey, R. C.; Neuhauser, Daniel
October 1996
Journal of Chemical Physics;10/8/1996, Vol. 105 Issue 14, p5979
Academic Journal
Results are reported of a four-dimensional dynamics study on the dissociation of H2 on Cu(100). The potential-energy surface was taken from density functional calculations, which employed the generalized gradient approximation and a slab representation for the surface. Reaction occurs preferentially in impacts near the bridge and hollow sites. Collisions near top sites promote vibrational excitation. The conclusion that vibrationally inelastic scattering and reaction occur preferentially on different sites can be generalized to other low index Cu surfaces. Resonances affect the reaction in the 4D model through a mechanism in which the molecule, trapped by excitation of the molecular bond which is weakened at the surface near top sites, is allowed more time to tunnel through the barrier to reaction. The calculated dependence of the diffraction probabilities on incidence energy suggests that a measurement of low-order diffraction would be able to determine whether the minimum barrier to reaction occurs for impacts on the bridge sites (as theory predicts) or on the hollow or top sites. The calculated reaction probabilities are in good agreement with experiment, further improvement being expected from including the rotational degrees of freedom in the model. © 1996 American Institute of Physics.


Related Articles

  • Optical model of dissociative chemisorption: H2 on the (111), (110), and (100) faces of copper. Farrelly, David; Levine, R. D. // Journal of Chemical Physics;8/1/1992, Vol. 97 Issue 3, p2139 

    The recently developed optical model of gas-surface scattering is applied to dissociative chemisorption of a hydrogen molecule on different faces of a copper crystal. In each case, a potential of mean force is employed to describe the real part of the scattering potential. The probability of...

  • Alignment of D2(v, J) desorbed from Cu(111): Low sensitivity of activated dissociative chemisorption to approach geometry. Gulding, S. J.; Wodtke, A. M.; Hou, H.; Rettner, C. T.; Michelsen, H. A.; Auerbach, D. J. // Journal of Chemical Physics;12/1/1996, Vol. 105 Issue 21, p9702 

    We have determined the alignment of D2(v,J) desorbed from Cu(111). The measurements reveal a small preference for ‘‘helicoptering’’ motion that increases with increasing J. At low J, the alignments are much smaller than predicted by recent calculations. We believe that...

  • Dissociative adsorption of H2 on Cu(110): A mixed quantum-classical study. Kumar, Sudershan; Jackson, Bret // Journal of Chemical Physics;4/15/1994, Vol. 100 Issue 8, p5956 

    A mixed quantum-classical approach is used to study the dissociative sticking of H2 on Cu(110). The method includes all six molecular degrees of freedom: three quantum mechanically and three classically. Dissociation probabilities are computed as a function of translational energy for several...

  • Hydrogen dissociation on copper: Importance of dimensionality in calculations of the sticking coefficient. Engdahl, Christer; Nielsen, Ulrik // Journal of Chemical Physics;3/1/1993, Vol. 98 Issue 5, p4223 

    The dissociative adsorption of H2 on copper is studied using classical trajectory and quantum wave-packet calculations. A multidimensional effective-medium potential is used which takes the molecular orientation as well as the surface structure into account. The emphasis in this work is on the...

  • The kinetics of H2 dissociative chemisorption: The role of transients. Chakravarty, Charusita; Metiu, Horia // Journal of Chemical Physics;6/1/1995, Vol. 102 Issue 21, p8643 

    The Lee–DePristo model for the dissociative chemisorption of H2 on Ni(100) has an interesting behavior. The potential energy surface has a minimum corresponding to a molecular, physisorbed state. This minimum is shallow and at 300 K the lifetime of physisorbed H2 is extremely short. One...

  • Dissociative chemisorption of H2 on Ni surface: Time-dependent quantum dynamics calculation and comparison with experiment. Sheng, Jia; Zhang, John Z. H. // Journal of Chemical Physics;3/1/1992, Vol. 96 Issue 5, p3866 

    A time-dependent quantum wave packet method has been applied to studying the process of activated dissociative chemisorption of H2 on Ni(100) surface. The Ni surface is treated as static and the effect of weak surface correlation is neglected in our dynamics calculation. The three-dimensional...

  • A critical examination of data on the dissociative adsorption and associative desorption of hydrogen at copper surfaces. Michelsen, H. A.; Auerbach, D. J. // Journal of Chemical Physics;6/1/1991, Vol. 94 Issue 11, p7502 

    We examine experimental data on the activated dissociative adsorption and associative recombination of hydrogen at copper surfaces with respect to the role played by molecular vibrational states. We use models describing the variation of the adsorption probability with the vibrational state,...

  • Dissociation of H2 on Cu(100): Dynamics on a new two-dimensional potential energy surface. Wiesenekker, G.; Kroes, G. J.; Baerends, E. J.; Mowrey, R. C. // Journal of Chemical Physics;3/1/1995, Vol. 102 Issue 9, p3873 

    A two-dimensional (2-D) potential energy surface (PES) has been calculated for H2 interacting with the (100) face of copper. The PES is for H2 approaching with its internuclear axis parallel to the surface and dissociating over a bridge site into neighboring hollow sites. The density functional...

  • Ti-decorated C60 as catalyst for hydrogen generation and storage. Liping Huang; Ying-Chun Liu; Gubbins, Keith E.; Nardelli, Marco Buongiorno // Applied Physics Letters;2/8/2010, Vol. 96 Issue 6, p063111 

    First-principles calculations were carried out to study Ti–C60 nanostructures as catalysts for water dissociation to generate hydrogen and elucidate the influence of water moisture in the air on hydrogen storage capability of such systems. Our results show that both Ti atoms and dimers on...


Read the Article


Sorry, but this item is not currently available from your library.

Try another library?
Sign out of this library

Other Topics