Alfredsson, M. and Catlow, C.R.A. (2001) Modelling of Pd and Pt Supported on the {111} and {011} Surfaces of Cubic-ZrO2. Physical Chemistry Chemical Physics, 3 (18). pp. 4129-4140. ISSN 1463-9076.
| The full text of this publication is not available from this repository. (Contact us about this Publication) | |
| Official URL http://dx.doi.org/10.1039/b102261j |
Abstract
The interaction of the noble metals Pd and Pt with the {111} and {011} surfaces of cubic-ZrO2 was examined by employing pseudo-potential plane-wave calculations within two Hamiltonians: the LDA and Perdew-Wang91 (GGA). The most favourable adsorption sites, adsorption energies, density of states and electron-charge density distributions are discussed, where the latter properties provide information on the bonding character between the ad-layer and the support, which is directly related to the catalytic activity. Owing to surface relaxation on the Pd/ZrO2{111} interface, we found a competition between the 1-fold and 3-fold oxygen sites; i.e. the differences in adsorption energies between the various adsorption sites are ca. 20 kJ mol(-1), which in addition suggests that the Pd-adlayer may have significant mobility. We anticipated the Pt-adlayer to be associated with lower surface mobility than the Pd-layer, due to the tendency to favour one particular adsorption site: DeltaE(ads) on top of O-S is similar to 100 kJ mol(-1), while on top of the 3-fold oxygen sites the energy is similar to 60 kJ mol(-1). Also, on the {011} surface, Pt is favoured by 1-fold oxygen coordination, while Pd exhibits higher oxygen coordination, and is adsorbed on the terraces of the {011} surface. Our calculations show the metal-support interactions to be mainly of an electrostatic nature, introduced by a polarisation of the metal ad-layers.
| Item Type: | Article |
|---|---|
| Additional information: | ISI Document Delivery No.: 477YG Times Cited: 14 Cited Reference Count: 51 |
| Uncontrolled keywords: | RAY-ABSORPTION SPECTROSCOPY AUGER-ELECTRON SPECTROSCOPY STRUCTURAL-PROPERTIES HIGH-TEMPERATURE FIRST-PRINCIPLES AB-INITIO ZIRCONIA CATALYSTS CLUSTERS PALLADIUM |
| Subjects: | Q Science |
| Divisions: | Faculties > Science Technology and Medical Studies > School of Physical Sciences > Functional Materials Group |
| Depositing User: | Maria Alfredsson |
| Date Deposited: | 14 Sep 2008 09:12 |
| Last Modified: | 14 Jan 2010 14:17 |
| Resource URI: | http://kar.kent.ac.uk/id/eprint/4760 (The current URI for this page, for reference purposes) |
- Depositors only (login required):
