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Growth of Stable Surface Oxides on Pt(111) at Near‐Ambient Pressures
Author(s) -
Fantauzzi Donato,
Krick Calderón Sandra,
Mueller Jonathan E.,
Grabau Mathias,
Papp Christian,
Steinrück HansPeter,
Senftle Thomas P.,
van Duin Adri C. T.,
Jacob Timo
Publication year - 2017
Publication title -
angewandte chemie international edition
Language(s) - English
Resource type - Journals
SCImago Journal Rank - 5.831
H-Index - 550
eISSN - 1521-3773
pISSN - 1433-7851
DOI - 10.1002/anie.201609317
Subject(s) - reaxff , x ray photoelectron spectroscopy , platinum , amorphous solid , ambient pressure , oxide , materials science , catalysis , chemical physics , chemistry , chemical engineering , molecular dynamics , computational chemistry , thermodynamics , crystallography , metallurgy , organic chemistry , physics , interatomic potential , engineering
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 O 2 partial pressure of 1 mbar.