skip to main content

SciTech ConnectSciTech Connect

Title: Size and structure effects of Pt{sub N} (N = 12 − 13) clusters for the oxygen reduction reaction: First-principles calculations

Size and structure effects on the oxygen reduction reaction on Pt{sub N} clusters with N = 12–13 atoms have been investigated using periodic density functional theory calculations with the generalized gradient approximation. To describe the catalytic activity, we calculated the O and OH adsorption energies on the cluster surface. The oxygen binding on the 3-fold hollow sites on stable Pt{sub 12−13} cluster models resulted more favorable for the reaction with O, compared with the Pt{sub 13}(I{sub h}) and Pt{sub 55}(I{sub h}) icosahedral particles, in which O binds strongly. However, the rate-limiting step resulted in the removal of the OH species due to strong adsorptions on the vertex sites, reducing the utility of the catalyst surface. On the other hand, the active sites of Pt{sub 12−13} clusters have been localized on the edge sites. In particular, the OH adsorption on a bilayer Pt{sub 12} cluster is the closest to the optimal target; with 0.0-0.2 eV weaker than the Pt(111) surface. However, more progress is necessary to activate the vertex sites of the clusters. The d-band center of Pt{sub N} clusters shows that the structural dependence plays a decisive factor in the cluster reactivity.
Authors:
 [1] ;  [2]
  1. Instituto Potosino de Investigación Científica y Tecnológica, San Luis Potosí 78216 (Mexico)
  2. Instituto de Física, Universidad Autónoma de San Luis Potosí, San Luis Potosí 78000 (Mexico)
Publication Date:
OSTI Identifier:
22493226
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 143; Journal Issue: 18; Other Information: (c) 2015 AIP Publishing LLC; Country of input: International Atomic Energy Agency (IAEA)
Country of Publication:
United States
Language:
English
Subject:
37 INORGANIC, ORGANIC, PHYSICAL AND ANALYTICAL CHEMISTRY; ADSORPTION; ATOMIC CLUSTERS; ATOMS; CATALYSTS; CHEMICAL BONDS; COMPARATIVE EVALUATIONS; DENSITY FUNCTIONAL METHOD; EV RANGE; HYDROXYL RADICALS; LAYERS; OXYGEN; PERIODICITY; REACTIVITY; REDUCTION; SURFACES