title: Surface Buckling and Subsurface Oxygen: Atomistic Insights into the Surface Oxidation of Pt(111).
abstract: Platinum is a catalyst of choice in scientific investigations and technological applications, which are both often carried out in the presence of oxygen. Thus, a fundamental understanding of platinum's (electro)catalytic behavior requires a detailed knowledge of the structure and degree of oxidation of platinum surfaces in operando. ReaxFF reactive force field calculations of the surface energies for structures with up to one monolayer of oxygen on Pt(111) reveal four stable surface phases characterized by pure adsorbate, high- and low-coverage buckled, and subsurface-oxygen structures, respectively. These structures and temperature programmed desorption (TPD) spectra simulated from them compare favorably with and complement published scanning tunneling microscopy (STM) and TPD experiments. The surface buckling and subsurface oxygen observed here influence the surface oxidation process, and are expected to impact the (electro)catalytic properties of partially oxidized Pt(111) surfaces.
authors.affiliation: Institut für Elektrochemie, Universität Ulm, Albert-Einstein-Allee 47, 89069 Ulm (Germany).
authors.forename: Donato
authors.initials: D
authors.lastname: Fantauzzi
authors.affiliation: Institut für Elektrochemie, Universität Ulm, Albert-Einstein-Allee 47, 89069 Ulm (Germany).
authors.forename: Jonathan E
authors.initials: JE
authors.lastname: Mueller
authors.affiliation: Institut für Elektrochemie, Universität Ulm, Albert-Einstein-Allee 47, 89069 Ulm (Germany).
authors.forename: Lehel
authors.initials: L
authors.lastname: Sabo
authors.affiliation: Department of Mechanical and Nuclear Engineering, Pennsylvania State University, University Park, PA 16801 (USA).
authors.forename: Adri C T
authors.initials: ACT
authors.lastname: van Duin
authors.affiliation: Institut für Elektrochemie, Universität Ulm, Albert-Einstein-Allee 47, 89069 Ulm (Germany).
authors.forename: Timo
authors.initials: T
authors.lastname: Jacob
keywords: computational chemistry; heterogeneous catalysis; oxidation; platinum; surface chemistry