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Influence of the exchange–correlation potential on the description of the molecular mechanism of oxygen dissociation by Au nanoparticles

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Abstract

The effect of the exchange–correlation functional on the molecular mechanism of dioxygen dissociation by Au nanoparticles is investigated using three Au nanoparticles of increasing size (Au25, Au38 and Au79) and various exchange–correlation functionals (local density approach, PW91, PBE and RevPBE. The effect of the exchange–correlation functional on the calculated adsorption energies is quite large and systematic whereas the effect on the calculated energy barriers is much smaller. Implications for the molecular mechanism of O2 dissociation, involving a competition between desorption and dissociation, are analyzed and discussed in detail.

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Acknowledgments

Alberto Roldán thanks Universitat Rovira i Virgili, for supporting his pre-doctoral research. Financial support has been provided by the Spanish Ministry of Science and Innovation (MICINN) (grants FIS2008-02238/FIS and CTQ2008-06549-C02-01) and, in part, by the Generalitat de Catalunya (Grants 2005SGR00697, 2005SGR-00104 and 2005 PEIR 0051/69). Computational time on the Marenostrum supercomputer of the Barcelona Supercomputing Center is gratefully acknowledged.

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Authors and Affiliations

  1. Departament de Química Física i Institut de Química Teòrica i Computacional (IQTCUB), Universitat de Barcelona, C/Martí i Franquès 1, 08028, Barcelona, Spain

    Alberto Roldán & Francesc Illas

  2. Departament de Química Física i Inorgànica, Universitat Rovira i Virgili, C/Marcel·lí Domingo s/n, 43007, Tarragona, Spain

    Alberto Roldán & Josep Manel Ricart

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  1. Alberto Roldán
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  2. Josep Manel Ricart
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  3. Francesc Illas
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Correspondence to Francesc Illas.

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Dedicated to Professor Santiago Olivella on the occasion of his 65th birthday and published as part of the Olivella Festschrift Issue.

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Roldán, A., Ricart, J.M. & Illas, F. Influence of the exchange–correlation potential on the description of the molecular mechanism of oxygen dissociation by Au nanoparticles. Theor Chem Acc 123, 119–126 (2009). https://doi.org/10.1007/s00214-009-0540-1

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