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Issue 39, 2014
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Segregation effects on the properties of (AuAg)147

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Abstract

AuAg nanoclusters are promising supported co-catalysts for photocatalytic hydrogen reduction. However, beyond the quantum regime (N > 100) little is known about how the electronic properties of these nanoparticles are affected by chemical ordering. We investigate the effects of chemical ordering on the properties of 147-atom cuboctahedral AuAg nanoclusters, using empirical potentials coupled with an atomic-swap basin-hopping search to optimise the elemental distribution, with the lowest energy arrangements then reminimised using Density Functional Theory (DFT). Force-field calculations show Au atoms preferentially occupy sub-surface positions in the bimetallic structures, which results in the formation of a pseudo-onion structure for Ag-rich compositions. At the DFT-level, however, an Ag core surrounded by an Au shell (Ag@Au) is energetically favoured, as electron density can be drawn more readily when Au atoms are positioned on the nanocluster surface, thus resulting in a partial negative charge. Core@shell configurations are analogous to structures that can be chemically synthesised, and further detailed electronic analysis is discussed in the context of nanocluster applications to co-catalysed photocatalysis.

Graphical abstract: Segregation effects on the properties of (AuAg)147

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Publication details

The article was received on 20 Feb 2014, accepted on 14 Apr 2014 and first published on 15 Apr 2014


Article type: Paper
DOI: 10.1039/C4CP00753K
Citation: Phys. Chem. Chem. Phys., 2014,16, 21049-21061
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    Segregation effects on the properties of (AuAg)147

    A. L. Gould, C. J. Heard, A. J. Logsdail and C. R. A. Catlow, Phys. Chem. Chem. Phys., 2014, 16, 21049
    DOI: 10.1039/C4CP00753K

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