Development of a ReaxFF potential for Pt-O systems describing the energetics and dynamics of Pt-oxide formation

Donato Fantauzzi, Jochen Bandlow, Lehel Sabo, Jonathan E. Mueller, Adri Van Duin, Timo Jacob

Research output: Contribution to journalArticle

21 Citations (Scopus)

Abstract

ReaxFF force field parameters describing Pt-Pt and Pt-O interactions have been developed and tested. The Pt-Pt parameters are shown to accurately account for the chemical nature, atomic structures and other materials properties of bulk platinum phases, low and high-index platinum surfaces and nanoclusters. The Pt-O parameters reliably describe bulk platinum oxides, as well as oxygen adsorption and oxide formation on Pt(111) terraces and the (111) and (100) steps connecting them. Good agreement between the force field and both density functional theory (DFT) calculations and experimental observations is demonstrated in the relative surface free energies of high symmetry Pt-O surface phases as a function of the oxygen chemical potential, making ReaxFF an ideal tool for more detailed investigations of more complex Pt-O surface structures. Validation for its application to studies of the kinetics and dynamics of surface oxide formation in the context of either molecular dynamics (MD) or Monte Carlo simulations are provided in part by a two-part investigation of oxygen diffusion on Pt(111), in which nudged elastic band (NEB) calculations and MD simulations are used to characterize diffusion processes and to determine the relevant diffusion coefficients and barriers. Finally, the power of the ReaxFF reactive force field approach in addressing surface structures well beyond the reach of routine DFT calculations is exhibited in a brief proof-of-concept study of oxygen adsorbate displacement within ordered overlayers.

Original languageEnglish (US)
Pages (from-to)23118-23133
Number of pages16
JournalPhysical Chemistry Chemical Physics
Volume16
Issue number42
DOIs
StatePublished - Oct 8 2014

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Oxides
Oxygen
oxides
Platinum
Surface structure
field theory (physics)
Density functional theory
Molecular dynamics
oxygen
Diffusion barriers
Nanoclusters
Chemical potential
platinum
Adsorbates
platinum oxides
molecular dynamics
density functional theory
Free energy
Materials properties
nanoclusters

All Science Journal Classification (ASJC) codes

  • Physics and Astronomy(all)
  • Physical and Theoretical Chemistry

Cite this

Fantauzzi, Donato ; Bandlow, Jochen ; Sabo, Lehel ; Mueller, Jonathan E. ; Van Duin, Adri ; Jacob, Timo. / Development of a ReaxFF potential for Pt-O systems describing the energetics and dynamics of Pt-oxide formation. In: Physical Chemistry Chemical Physics. 2014 ; Vol. 16, No. 42. pp. 23118-23133.
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Development of a ReaxFF potential for Pt-O systems describing the energetics and dynamics of Pt-oxide formation. / Fantauzzi, Donato; Bandlow, Jochen; Sabo, Lehel; Mueller, Jonathan E.; Van Duin, Adri; Jacob, Timo.

In: Physical Chemistry Chemical Physics, Vol. 16, No. 42, 08.10.2014, p. 23118-23133.

Research output: Contribution to journalArticle

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