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DFT-Computed trends in the properties of bimetallic precious-metal nanoparticles with Core@shell segregation

Logsdail, Andrew J. ORCID:, Paz-Borbon, Lauro Oliver and Downing, Christopher A. 2018. DFT-Computed trends in the properties of bimetallic precious-metal nanoparticles with Core@shell segregation. Journal of Physical Chemistry C 122 (10) , pp. 5721-5730. 10.1021/acs.jpcc.7b10614

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Bimetallic precious-metal nanoparticles (NPs) are promising as components of heterogeneous catalytic systems, however the synergistic effects that occur when combining multiple elements in these discrete systems are still being understood. Here, we present a systematic computational study that investigates the effect of geometry and compositional arrangements on the properties bimetallic core@shell precious-metal NPs. Combinations of the elements Ag, Au, Pd and Pt are considered and, for surface coverages of just one monolayer, we show that the electronic properties of the NP, such as the Fermi energy and d-band centre, are strongly correlated with the element occupying sites at the NP surface, in qualitative but not quantitative agreement with previous two-dimensional slab calculations. In contrast, strain effects from structural choices and elemental size mismatch play a minor role in altering energetic levels. Charge transfer between the core and shell regions of the NPs is a balance between the increased electronic degrees of freedom that implicitly exists at an NP surface and the electronegativity of the constituent elements, with Au and Ag respectively good and bad at retaining electron density. We use our results to rationalise recent experimental observations, and foresee that the outcomes will assist the rational atom-by-atom design of future nanoparticle catalysts.

Item Type: Article
Date Type: Published Online
Status: Published
Schools: Advanced Research Computing @ Cardiff (ARCCA)
Cardiff Catalysis Institute (CCI)
Publisher: ACS Publications
ISSN: 1932-7447
Date of First Compliant Deposit: 14 February 2018
Date of Acceptance: 8 February 2018
Last Modified: 06 Nov 2023 20:11

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