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Catalytic Oxidation Activity of Pt3O4 Surfaces and Thin Films

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Institut für Werkstoffwissenschaft, Technische Universität Dresden, Hallwachsstrasse 3, 01069 Dresden, Germany, Theory of Condensed Matter Group, Cavendish Laboratory, University of Cambridge, J J Thomson Avenue, Cambridge CB3 0HE, United Kingdom, and Fraunhofer Institut für Werkstoffmechanik, Wöhlerstrasse 11, 79108 Freiburg, Germany
Cite this: J. Phys. Chem. B 2006, 110, 30, 14860–14869
Publication Date (Web):July 6, 2006
https://doi.org/10.1021/jp063281r
Copyright © 2006 American Chemical Society
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    Abstract

    The catalytic oxidation activity of platinum particles in automobile catalysts is thought to originate from the presence of highly reactive superficial oxide phases which form under oxygen-rich reaction conditions. Here we study the thermodynamic stability of platinum oxide surfaces and thin films and their reactivities toward oxidation of carbon compounds by means of first-principles atomistic thermodynamics calculations and molecular dynamics simulations based on density functional theory. On the Pt(111) surface the most stable superficial oxide phase is found to be a thin layer of α-PtO2, which appears not to be reactive toward either methane dissociation or carbon monoxide oxidation. A PtO-like structure is most stable on the Pt(100) surface at oxygen coverages of one monolayer, while the formation of a coherent and stress-free Pt3O4 film is favored at higher coverages. Bulk Pt3O4 is found to be thermodynamically stable in a region around 900 K at atmospheric pressure. The computed net driving force for the dissociation of methane on the Pt3O4(100) surface is much larger than that on all other metallic and oxide surfaces investigated. Moreover, the enthalpy barrier for the adsorption of CO molecules on oxygen atoms of this surface is as low as 0.34 eV, and desorption of CO2 is observed to occur without any appreciable energy barrier in molecular dynamics simulations. These results, combined, indicate a high catalytic oxidation activity of Pt3O4 phases that can be relevant in the contexts of Pt-based automobile catalysts and gas sensors.

    *

     Address correspondence to this author. E-mail:  nicola.seriani@ univie.ac.at.

    †

     Technische Universität Dresden.

    ⊥

     Present address:  Institut für Materialphysik, Universität Wien, Sensengasse 8, A-1090 Wien, Austria.

    ‡

     University of Cambridge.

    §

     Fraunhofer Institut für Werkstoffmechanik.

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