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Title: Implicit solvent effects in the determination of Bronsted-Evans-Polanyi relationships for heterogeneously catalyzed reactions
Author: Gomes, Jose R. B.
Viñes Solana, Francesc
Illas i Riera, Francesc
Fajin, Jose L. C.
Keywords: Catàlisi heterogènia
Metalls de transició
Heterogeneus catalysis
Transition metals
Issue Date: 28-Aug-2019
Publisher: Royal Society of Chemistry
Abstract: Heterogeneous catalyzed reactions take place at the catalyst surface where, depending on the conditions and process, the reacting molecules are either in gas or liquid phase. In the latter case, computational heterogeneous catalysis studies usually neglect solvent effects. In this work, we systematically analyze how the electrostatic contribution to solvent effects influence the atomic structure of reactants and products as well as adsorption, activation and reaction energy for the dissociation of water on several planar and stepped transition metal surfaces. The solvent effects were accounted for through an implicit model that describes the effect of electrostatics, cavitation, and dispersion on the interaction between solute and solvent. The present study shows that activation energy barriers are only slightly influenced by the inclusion of the electrostatic solvent effects accounted for in a continuum solvent approach whereas the adsorption energies of reactants or products are significantly affected. Encouragingly, the linear equations corresponding to the Brønsted-Evans-Polanyi relationships (BEPs) relating the activation energies for the dissociation reaction with a suitable descriptor, e.g. the adsorption energies of the products of reaction on the difference surfaces, are similar in the presence or in the absence of the solvent. This suggests that BEP relationships derived without the implicit consideration of the solvent are still valid for predicting activation energy barriers of catalytic reactions from a reaction descriptor.
Note: Versió postprint del document publicat a:
It is part of: Physical Chemistry Chemical Physics, 2019, vol. 21, num. 32, p. 17687-17695
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ISSN: 1463-9076
Appears in Collections:Articles publicats en revistes (Ciència dels Materials i Química Física)

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