Document Type

Article

Publication Version

Published Version

Publication Date

11-24-2014

Journal or Book Title

Nano Letters

Volume

14

Issue

12

First Page

777

Last Page

7084

DOI

10.1021/nl503519m

Abstract

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.

Comments

Reprinted with permission from Nano Lett. 2014, 14(12), pp. 7077–7084, doi:10.1021/nl503519m. Copyright 2014 American Chemical Society.

Copyright Owner

American Chemical Society

Language

en

File Format

application/pdf

Share

COinS