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Computational investigation of the adsorption of carbon dioxide onto zirconium oxide clusters

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Abstract

A theoretical investigation of the adsorption of CO2 onto ZrO2 is presented. Various cluster models were used to mimic different basic and acidic sites on the surface. The method used was the density functional theory with the generalized gradient approximation and including Grimme’s empirical model in order to properly describe the weak interactions that may occur between the adsorbate and the surface. We found that the adsorption at sites exhibiting two adjacent unsaturated zirconium atoms led to either the exothermic dissociation of CO2 or to a strongly physisorbed state. By contrast, on a single unsaturated zirconium, CO2 was adsorbed in an apical manner. In this case, the molecule is highly polarized and the adsorption energy amounts to −64.6 kJ mol−1. Finally, the weakest adsorption of CO2 occurred on the basic OH sites on the surface.

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Acknowledgments

The author P. Boulet is grateful to the Centre Informatique National de l’Enseignement Supérieur (CINES, Montpellier, France) and the Centre Régional de Compétences en Modélisation Moléculaire (CRCMM, Marseille, France) for providing access to their computer facilities. This work was granted access to the HPC resources of CINES under the allocation 2011085120 made by GENCI (Grand Equipement National de Calcul Intensif).

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  1. Christina Knöfel

    Present address: Risø National Laboratory for Sustainable Energy, Fuel Cells and Solid State Chemistry Division, ABF, P.O. Box 49, Frederiksborgvej 399, DK-4000, Roskilde, Denmark

Authors and Affiliations

  1. Laboratoire Matériaux Divisés Interfaces Réactivité Electrochimie, UMR 7246, Aix-Marseille Université et CNRS, Avenue de l’Escadrille Normandie-Niemen, 13397, Marseille Cedex, France

    Pascal Boulet, Christina Knöfel, Bogdan Kuchta, Virginie Hornebecq & Philip L. Llewellyn

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  1. Pascal Boulet
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Correspondence to Pascal Boulet.

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Boulet, P., Knöfel, C., Kuchta, B. et al. Computational investigation of the adsorption of carbon dioxide onto zirconium oxide clusters. J Mol Model 18, 4819–4830 (2012). https://doi.org/10.1007/s00894-012-1486-0

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  • DOI: https://doi.org/10.1007/s00894-012-1486-0

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