H 2 dissociation on individual Pd atoms deposited on Cu(111)

• Autores: Ramos Acevedo, Maximiliano; Martinez, Alejandra Elisa; Busnengo, Heriberto Fabio
• Año de publicación: 2012
• Idioma: inglés
• Tipo de recurso: artículo
• Materia: Aleaciones; Dinámica Molecular; DFT
• Institución: Consejo Nacional de Investigaciones Científicas y Técnicas

We present a Molecular Dynamics (MD) study based on Density Functional Theory (DFT) calculations for H2 interacting with a Pd?Cu(111) surface alloy for low Pd coverages, ΘPd. Our results show, in line with recent experimental data, that single isolated Pd atoms evaporated on Cu(111) significantly increase the reactivity of the otherwise inert pure Cu surface. On top of substitutional Pd atoms in the Pd?Cu(111) surface alloy, the activation energy barrier for H2 dissociation is smaller than the lowest one found on Cu(111) by a factor of two: 0.25 eV vs. 0.46 eV. Also in agreement with experiments, our DFT-MD calculations show that a large fraction of the dissociating H atoms efficiently spillover from Pd (i.e. the active sites), thanks to their extra kinetic energy due to the 0.50 eV chemisorption exothermicity. Still, our DFT-MD calculations predict a dissociative sticking probability for low energy H2 molecules that is much smaller than the estimated value from scanning tunneling microscopy experiments. Thus, further theoretical and experimental investigations are required for a complete understanding of H2 dissociation on low-ΘPd Pd?Cu(111) surface alloys.
Fil: Ramos Acevedo, Maximiliano. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Martinez, Alejandra Elisa. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina
Fil: Busnengo, Heriberto Fabio. Consejo Nacional de Investigaciones Científicas y Técnicas. Centro Científico Tecnológico Conicet - Rosario. Instituto de Física de Rosario. Universidad Nacional de Rosario. Instituto de Física de Rosario; Argentina