Growth of Stable Surface Oxides on Pt(111) at Near-Ambient Pressures
Dr. Donato Fantauzzi
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
These authors contributed equally to this work.
Search for more papers by this authorSandra Krick Calderón
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
These authors contributed equally to this work.
Search for more papers by this authorDr. Jonathan E. Mueller
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
Search for more papers by this authorMathias Grabau
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorCorresponding Author
Dr. Christian Papp
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorProf. Dr. Hans-Peter Steinrück
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorDr. Thomas P. Senftle
Department of Mechanical and Aereospace Engineering, Princeton University, Princeton, NJ, 08544-5263 USA
Search for more papers by this authorProf. Dr. Adri C. T. van Duin
Department of Mechanical and Nuclear Engineering, Pennsylvania State University, University Park, PA, 16801 USA
Search for more papers by this authorCorresponding Author
Prof. Dr. Timo Jacob
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
Search for more papers by this authorDr. Donato Fantauzzi
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
These authors contributed equally to this work.
Search for more papers by this authorSandra Krick Calderón
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
These authors contributed equally to this work.
Search for more papers by this authorDr. Jonathan E. Mueller
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
Search for more papers by this authorMathias Grabau
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorCorresponding Author
Dr. Christian Papp
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorProf. Dr. Hans-Peter Steinrück
Lehrstuhl für Physikalische Chemie II, Universität Erlangen-Nürnberg, Egerlandstr. 3, 91058 Erlangen, Germany
Search for more papers by this authorDr. Thomas P. Senftle
Department of Mechanical and Aereospace Engineering, Princeton University, Princeton, NJ, 08544-5263 USA
Search for more papers by this authorProf. Dr. Adri C. T. van Duin
Department of Mechanical and Nuclear Engineering, Pennsylvania State University, University Park, PA, 16801 USA
Search for more papers by this authorCorresponding Author
Prof. Dr. Timo Jacob
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
Search for more papers by this authorAbstract
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 O2 partial pressure of 1 mbar.
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