TITLE

Metal nanoparticles as models of single crystal surfaces and supported catalysts: Density functional study of size effects for CO/Pd(111)

AUTHOR(S)
Yudanov, Ilya V.; Sahnoun, Riadh; Neyman, Konstantin M.; Rösch, Notker
PUB. DATE
December 2002
SOURCE
Journal of Chemical Physics;12/1/2002, Vol. 117 Issue 21, p9887
SOURCE TYPE
Academic Journal
DOC. TYPE
Article
ABSTRACT
Large octahedral and cuboctahedral palladium clusters, ranging from Pd[sub 55] to Pd[sub 146], have been investigated by means of all-electron relativistic density functional calculations. Adsorption of CO molecules on the (111) facets of these clusters was also studied. In particular, we focused on the interaction of CO (a single molecule per facet) with threefold hollow sites to inspect the variation of the calculated adsorption parameters with cluster size. We considered how observables calculated for that adsorption position on cluster facets relate to adsorption properties of the corresponding site at the single crystal surface Pd(111). We demonstrated for the first time that, with three-dimensional cluster models proposed here, one can reach cluster size convergence even for such a sensitive observable as the adsorption energy on a metal surface. We also addressed size effects on interatomic distances and the cohesive energy of bare Pd nanoclusters whose structure was fully optimized under the imposed Oh symmetry constraint. These quantities were found to correlate linearly with the average coordination number and the inverse of the cluster radius, respectively, allowing a rather accurate extrapolation to the corresponding values of Pd bulk. Finally, we considered the size convergence of adsorption properties of the optimized Pd clusters, as probed by CO adsorption. We also outlined implications of using these symmetric clusters for investigating adsorption and reactions on oxide-supported nanoparticles of model Pd catalysts.
ACCESSION #
7903364

 

Related Articles

  • Studies of nanocluster coalescence at high temperature. Liu, H.B.; José-Yacaman, M.; Perez, R.; Ascencio, J.A. // Applied Physics A: Materials Science & Processing;2003, Vol. 77 Issue 1, p63 

    Molecular Dynamics simulations and high resolution electron microscope observations were used to determine the mechanism of nanocluster coalescence in detail. In the simulations, the tight-binding second momentum approximation potential was used to describe the interatomic interactions. The...

  • Nanoparticles behaving oddly. Louie, Steven G. // Nature;12/19/1996, Vol. 384 Issue 6610, p612 

    Provides background and analysis of a report of a study of the electronic specific heat capacity and magnetic susceptibility of metal clusters of nanoparticles. The confirmation of predictions by Kubo and others about metal nanoparticles at low temperatures. The report by Voloktin and others...

  • NH3 Decomposition Kinetics on Supported Ru Clusters: Morphology and Particle Size Effect. Weiqing Zheng; Jian Zhang; Hengyong Xu; Wenzhao Li // Catalysis Letters;Dec2007, Vol. 119 Issue 3/4, p311 

    The supported Ru clusters with mean sizes ranging from 1.9 to 4.6 nm showed a high activity towards the NH3 decomposition reaction. The structural properties of catalysts were characterized by N2 adsorption/desorption, X-ray diffraction (XRD) and transmission electron micrograph (TEM)....

  • Generation of palladium clusters on Au(111) electrodes: Experiments and simulations. Del Popolo, M.; Leiva, E.; Kleine, H.; Meier, J.; Stimming, U.; Mariscal, M.; Schmickler, W. // Applied Physics Letters;9/30/2002, Vol. 81 Issue 14, p2635 

    The properties of palladium clusters, generated with the electrochemical scanning tunneling microscope, have been investigated both by experiments and by computer simulations. The clusters are found to be larger and more stable if the tip is moved further towards the electrode surface in the...

  • A hydrogen sensor based on tunneling between palladium clusters. van Lith, J.; Lassesson, A.; Brown, S. A.; Schulze, M.; Partridge, J. G.; Ayesh, A. // Applied Physics Letters;10/29/2007, Vol. 91 Issue 18, p181910 

    We describe nanocluster based tunneling sensors for detecting hydrogen. Pd clusters with diameters ranging from 3.5 to 6 nm are deposited between a pair of contacts until a predetermined resistance between the contacts is obtained. We demonstrate that the conduction through the cluster film is...

  • Measurement of nanoparticle temperature in a (CO2) N cluster beam using SF6 molecules as tiny probe thermometers. Makarov, G. N.; Petin, A. N. // Journal of Experimental & Theoretical Physics;Apr2010, Vol. 110 Issue 4, p568 

    A temperature measurement technique using SF6 molecules as tiny probe thermometers is described, and results are presented, for large (CO2) N van der Waals clusters (with N ≥ 102) in a cluster beam. The SF6 molecules captured by (CO2) N clusters in crossed cluster and molecular beams...

  • Homogeneous and heterogeneous clustering in the accretion regime. Feiden, P.; Leygnier, J.; Cahuzac, Ph.; Bréchignac, C. // European Physical Journal D -- Atoms, Molecules, Clusters & Opti;Jul2007, Vol. 43 Issue 1-3, p49 

    Condensation of nano-droplets in a supersaturating vapor decomposes in two steps: the formation of a nucleation center, also called critical nuclei or nucleation seed, and the growth sequence, by accretion of further atoms on the nucleation center. These two steps have been investigated...

  • Nanoscale SiO2 Particles at High Temperatures: Size Dependent Properties. Schweigert, I. V.; Lehtinen, K. E. J.; Carrier, M. J.; Zachariah, M. R. // AIP Conference Proceedings;2002, Vol. 649 Issue 1, p414 

    The properties of silica clusters at temperatures of 1500 to 2800 K have been investigated using classical molecular dynamics simulations for particles containing up to 1152 atoms. We found that the atoms in the cluster were arranged in a shell like structure at low temperatures and that the...

  • Structures of gas-phase Ag–Pd nanoclusters: A computational study. Negreiros, Fabio R.; Kuntová, Zdenka; Barcaro, Giovanni; Rossi, Giulia; Ferrando, Riccardo; Fortunelli, Alessandro // Journal of Chemical Physics;6/21/2010, Vol. 132 Issue 23, p234703 

    Gas-phase Ag–Pd clusters in the size range of 38–100 atoms are studied via a combined density-functional/empirical-potential (DF-EP) approach. Many-body EPs describing Pd–Pd, Ag–Ag, and Ag–Pd interactions are reparametrized and used in thorough global...

Share

Read the Article

Courtesy of VIRGINIA BEACH PUBLIC LIBRARY AND SYSTEM

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

Try another library?
Sign out of this library

Other Topics