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arXiv · 0801.1144

Alloy surface segregation in reactive environments: A first-principles atomistic thermodynamics study of Ag3Pd(111) in oxygen atmospheres

John Kitchin·Karsten Reuter·Matthias Scheffler
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Abstract

We present a first-principles atomistic thermodynamics framework to describe the structure, composition and segregation profile of an alloy surface in contact with a (reactive) environment. The method is illustrated with the application to a Ag3Pd(111) surface in an oxygen atmosphere, and we analyze trends in segregation, adsorption and surface free energies. We observe a wide range of oxygen adsorption energies on the various alloy surface configurations, including binding that is stronger than on a Pd(111) surface and weaker than that on a Ag(111) surface. This and the consideration of even small amounts of non-stoichiometries in the ordered bulk alloy are found to be crucial to accurately model the Pd surface segregation occurring in increasingly O-rich gas phases.

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John Kitchin, Karsten Reuter, Matthias Scheffler. 2008-01-08. Alloy surface segregation in reactive environments: A first-principles atomistic thermodynamics study of Ag3Pd(111) in oxygen atmospheres. https://doi.org/10.1103/physrevb.77.075437

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