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Configurational Thermodynamics of Alloyed Nanoparticles with Adsorbates

TitleConfigurational Thermodynamics of Alloyed Nanoparticles with Adsorbates
Publication TypeJournal Article
Year of Publication2014
AuthorsWang, LL, Tan, TL, Johnson, DD
JournalNano Letters
Date Published12
Type of ArticleArticle
ISBN Number1530-6984
Accession NumberWOS:000346322800050
Keywords1st-principles, calculation, catalysts, Cluster expansion, co, core-shell, effective cluster interactions, first principles, nanoalloy, nanoparticle, O, oxidation, Pd, phase-diagram, Rh, rh nanoparticles, shape changes, transformations, variation formalism

Changes in the chemical configuration of alloyed nanoparticle (NP) catalysts induced by adsorbates under working conditions, such as reversal in core-shell preference, are crucial to understand and design NP functionality. We extend the cluster expansion method to predict the configurational thermodynamics of alloyed NPs with adsorbates based on density functional theory data. Exemplified with PdRh NPs having O-coverage up to a monolayer, we fully detail the core-shell behavior across the entire range of NP composition and O-coverage with quantitative agreement to in situ experimental data. Optimally fitted cluster interactions in the heterogeneous system are the key to enable quantitative Monte Carlo simulations and design.

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