On the combined use of discrete solvent ...
Type de document :
Compte-rendu et recension critique d'ouvrage
Titre :
On the combined use of discrete solvent models and continuum descriptions of solvent effects in ligand exchange reactions: a case study of the uranyl(VI) aquo ion
Auteur(s) :
Wåhlin, Pernilla [Auteur]
Schimmelpfennig, Bernd [Auteur]
Institut für Nukleare Entsorgung [INE]
Wahlgren, Ulf [Auteur]
Nordic Institute for Theoretical Physics [NORDITA]
Grenthe, Ingmar [Auteur]
Vallet, Valérie [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Schimmelpfennig, Bernd [Auteur]
Institut für Nukleare Entsorgung [INE]
Wahlgren, Ulf [Auteur]
Nordic Institute for Theoretical Physics [NORDITA]
Grenthe, Ingmar [Auteur]
Vallet, Valérie [Auteur]
Laboratoire de Physique des Lasers, Atomes et Molécules - UMR 8523 [PhLAM]
Titre de la revue :
Theoretical Chemistry Accounts: Theory, Computation, and Modeling
Pagination :
377
Éditeur :
Springer Verlag
Date de publication :
2009-09-16
ISSN :
1432-881X
Mot(s)-clé(s) :
quantum chemistry
actinide
solvent models
actinide
solvent models
Discipline(s) HAL :
Physique [physics]/Physique [physics]/Chimie-Physique [physics.chem-ph]
Résumé en anglais : [en]
Modeling of the solvent is important when using quantum chemical methods for the assignment of mechanisms from experimental studies of the exchange of water between metal aquo ions and the bulk solvent. In the present ...
Lire la suite >Modeling of the solvent is important when using quantum chemical methods for the assignment of mechanisms from experimental studies of the exchange of water between metal aquo ions and the bulk solvent. In the present study, we have investigated if and how the mechanisms for water exchange in the UO<sub>2</sub>(OH<sub>2</sub>)<sub>5</sub><sup>2+</sup>–H<sub>2</sub>O system is affected by the choice of chemical models for the second coordination sphere and physical models for describing the cavity in conductor-like polarizable continuum (CPCM) models. In the first case, we have compared models with one and five waters in the second coordination sphere. For both models, we have compared cavities in which each atom is assigned one spherical cavity and one in which the water molecules are described by a single spherical cavity (the United Atom model). There are significant differences in the relative energy of dissociative and associative intermediates; however, they are not large enough to affect the conclusion that the water exchange proceeds through an associative/interchange mechanism.Lire moins >
Lire la suite >Modeling of the solvent is important when using quantum chemical methods for the assignment of mechanisms from experimental studies of the exchange of water between metal aquo ions and the bulk solvent. In the present study, we have investigated if and how the mechanisms for water exchange in the UO<sub>2</sub>(OH<sub>2</sub>)<sub>5</sub><sup>2+</sup>–H<sub>2</sub>O system is affected by the choice of chemical models for the second coordination sphere and physical models for describing the cavity in conductor-like polarizable continuum (CPCM) models. In the first case, we have compared models with one and five waters in the second coordination sphere. For both models, we have compared cavities in which each atom is assigned one spherical cavity and one in which the water molecules are described by a single spherical cavity (the United Atom model). There are significant differences in the relative energy of dissociative and associative intermediates; however, they are not large enough to affect the conclusion that the water exchange proceeds through an associative/interchange mechanism.Lire moins >
Langue :
Anglais
Vulgarisation :
Non
Commentaire :
8 pages
Source :
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