title: Growth of Stable Surface Oxides on Pt(111) at Near-Ambient Pressures.
abstract: Detailed knowledge of the structure and degree of oxidation of platinum surfaces under operando conditions is essential for understanding catalytic performance. However, experimental investigations of platinum surface oxides have been hampered by technical limitations, preventing in situ investigations at relevant pressures. As a result, the time-dependent evolution of oxide formation has only received superficial treatment. In addition, the amorphous structures of many surface oxides have hindered realistic theoretical studies. Using near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS) we show that a time scale of hours (t≥4 h) is required for the formation of platinum surface oxides. These experimental observations are consistent with ReaxFF grand canonical Monte Carlo (ReaxFF-GCMC) calculations, predicting the structures and coverages of stable, amorphous surface oxides at temperatures between 430-680 K and an O2partial pressure of 1 mbar.
authors.affiliation: Institute of Electrochemistry, Ulm University, Albert-Einstein-Allee 47, 89069, Ulm, Germany.|Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage, 89081, Ulm, Germany.|Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021, Karlsruhe, Germany.
authors.forename: Donato
authors.initials: D
authors.lastname: Fantauzzi
authors.affiliation: Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058, Erlangen, Germany.
authors.forename: Sandra
authors.initials: S
authors.lastname: Krick Calderón
authors.affiliation: Institute of Electrochemistry, Ulm University, Albert-Einstein-Allee 47, 89069, Ulm, Germany.|Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage, 89081, Ulm, Germany.|Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021, Karlsruhe, Germany.
authors.forename: Jonathan E
authors.initials: JE
authors.lastname: Mueller
authors.affiliation: Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058, Erlangen, Germany.
authors.forename: Mathias
authors.initials: M
authors.lastname: Grabau
authors.affiliation: Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058, Erlangen, Germany.
authors.forename: Christian
authors.initials: C
authors.lastname: Papp
authors.affiliation: Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058, Erlangen, Germany.
authors.forename: Hans-Peter
authors.initials: HP
authors.lastname: Steinrück
authors.affiliation: Department of Mechanical and Aereospace Engineering, Princeton University, Princeton, NJ, 08544-5263, USA.
authors.forename: Thomas P
authors.initials: TP
authors.lastname: Senftle
authors.affiliation: Department of Mechanical and Nuclear Engineering, Pennsylvania State University, University Park, PA, 16801, USA.
authors.forename: Adri C T
authors.initials: AC
authors.lastname: van Duin
authors.affiliation: Institute of Electrochemistry, Ulm University, Albert-Einstein-Allee 47, 89069, Ulm, Germany.|Helmholtz Institute Ulm (HIU) Electrochemical Energy Storage, 89081, Ulm, Germany.|Karlsruhe Institute of Technology (KIT), P.O. Box 3640, 76021, Karlsruhe, Germany.
authors.forename: Timo
authors.initials: T
authors.lastname: Jacob
keywords: interfaces; kinetics; oxidation; phase transitions; surface chemistry