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DFT study of the thermodynamic stability of Pd-Pt bulk oxide phases

Autor(en)
Arezoo Dianat, Nicola Seriani, Manfred Bobeth, Wolfgang Pompe, Lucio Colombi Ciacchi
Abstrakt

The catalytic combustion activity of PdPt bimetallic catalysts is

governed by oxide phases which form under oxygen-rich operation

conditions. We investigate the thermodynamic stability of mixed PdxPt1−xOy phases with the crystal structures of PdO, PtO2, and Pt3O4

within an ab initio thermodynamics framework based on

density-functional theory calculations. Our results suggest a complex

mixing−demixing behavior of the Pd−Pt−O system upon variations of

temperature and oxygen partial pressure. At atmospheric pressure mixed

oxides are predicted to be stable only at temperatures below 400−500 K,

whereby the presence of Pd4+ ions is stabilized with increasing Pt amount in a PdxPt1−xO2 phase. At intermediate temperatures a mixture of phases becomes stable where PdO coexists with PtO2 or Pt3O4.

At high temperatures the oxides decompose directly to form PdPt alloys,

except for Pd-rich systems, where PdO and metallic Pt coexist within a

small temperature window.

Organisation(en)
Computergestützte Materialphysik
Externe Organisation(en)
Fraunhofer-Institut für Werkstoffmechanik IWM, Karlsruher Institut für Technologie, Technische Universität Dresden
Journal
The Journal of Physical Chemistry Part C (Nanomaterials and Interfaces)
Band
112
Seiten
13623–13628
Anzahl der Seiten
6
ISSN
1932-7447
DOI
https://doi.org/10.1021/jp8035742
Publikationsdatum
2008
Peer-reviewed
Ja
ÖFOS 2012
103018 Materialphysik
Link zum Portal
https://ucrisportal.univie.ac.at/de/publications/4790eedd-f6bb-45d1-abd4-80b88b506d42