skip to main content

Title: A first-principles study of Pt thin films on SrTiO{sub 3}(100): Support effects on CO adsorption

Density functional theory was used to study CO adsorption on thin Pt metal films supported on SrO- and TiO{sub 2}-terminated SrTiO{sub 3}(100) surfaces. Regardless of substrate-termination, significant enhancement in CO binding occurred on the Pt monolayer compared to the bulk Pt(100) surface. We also observed CO-coverage dependent shifting of Pt atoms, influenced by the nature of underlying oxide atoms. These oxide-induced effects become negligible after depositing more than 2 monolayers of Pt. Evaluating the electronic structures of oxide-supported Pt showed that the interaction of filled Pt d{sub xz+yz} and empty Pt d{sub z{sup 2}} states with CO molecular orbitals can be directly related to CO adsorption on the Pt/SrTiO{sub 3}(100) surface. A hybrid d-band model is able to capture the CO adsorption trends for systems that do not show large lateral distortion except for the case of Pt adsorbed above the Sr atom on the SrO-termination. For this case, charge transfer from adjacent Pt atoms leads to a large filled d{sub z{sup 2}} peak below the Fermi level that weakens the Pt–CO σ bonding due to Pauli repulsion.
Authors:
;  [1]
  1. William G. Lowrie Department of Chemical and Biomolecular Engineering, The Ohio State University, Columbus, Ohio 43210 (United States)
Publication Date:
OSTI Identifier:
22415578
Resource Type:
Journal Article
Resource Relation:
Journal Name: Journal of Chemical Physics; Journal Volume: 142; Journal Issue: 12; 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; 75 CONDENSED MATTER PHYSICS, SUPERCONDUCTIVITY AND SUPERFLUIDITY; ADSORPTION; ATOMS; CARBON MONOXIDE; COMPARATIVE EVALUATIONS; DENSITY FUNCTIONAL METHOD; ELECTRONIC STRUCTURE; FERMI LEVEL; PLATINUM; STRONTIUM OXIDES; STRONTIUM TITANATES; SUBSTRATES; SURFACES; THIN FILMS; TITANIUM OXIDES