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Hydration gibbs free energies of open and closed shell trivalent lanthanide and actinide cations from polarizable molecular dynamics

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Abstract

The hydration free energies, structures, and dynamics of open- and closed-shell trivalent lanthanide and actinide metal cations are studied using molecular dynamics simulations (MD) based on a polarizable force field. Parameters for the metal cations are derived from an ab initio bottom-up strategy. MD simulations of six cations solvated in bulk water are subsequently performed with the AMOEBA polarizable force field. The calculated first-and second shell hydration numbers, water residence times, and free energies of hydration are consistent with experimental/theoretical values leading to a predictive modeling of f-elements compounds.

Solvation free energy of the actinide (III) and lanthanide (III) cations in water: AMOEBA vs. reference data

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Acknowledgments

P. Y. R. thanks support by the National Institute of Health (R01GM106137). A.M. thanks the CEA for a PhD grant. J.-P. D. thanks the CEA nuclear energy division DEN/RBPCH for financial support. This work was granted access to the HPC resources of [CCRT/CINES/IDRIS] under the allocation c2013086146 made by GENCI (Grand Equipement National de Calcul Intensif).

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Authors and Affiliations

  1. Laboratoire de Chimie Théorique, Sorbonne Universités, UMPC, CNRS UMR 7616, CC 137 4 Place Jussieu, 75252, Paris, Cedex 05, France

    Aude Marjolin & Jean-Philip Piquemal

  2. Laboratoire de Chimie Moléculaire et de catalyse pour l’Energie, CEA, CNRS UMR 3299, CEA Saclay, 91191, Gif-sur Yvette, Cedex, France

    Aude Marjolin & Jean-Pierre Dognon

  3. Laboratoire de Chimie Quantique, Université de Strasbourg, CNRS UMR 7177, PB 296 1 Rue Blaise Pascal, 67008, Strasbourg, Cedex, France

    Christophe Gourlaouen

  4. Laboratoire de Chimie Moléculaire, Department of Chemistry, Ecole Polytechnique, CNRS, 91 128, Palaiseau, Cedex, France

    Carine Clavaguéra

  5. Department of Biomedical engineering, University of Texas at Austin, Austin, TX, 78712-1062, USA

    Pengyu Y. Ren

Authors
  1. Aude Marjolin
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  2. Christophe Gourlaouen
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  3. Carine Clavaguéra
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  4. Pengyu Y. Ren
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  5. Jean-Philip Piquemal
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  6. Jean-Pierre Dognon
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Corresponding authors

Correspondence to Carine Clavaguéra, Jean-Philip Piquemal or Jean-Pierre Dognon.

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This paper belongs to Topical Collection QUITEL 2013

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ESM 1

MRCI results; validation on metal-water cluster interaction energies; structural data from SBC 216 H2O and PBC 215 H2O MD; hydration Gibbs free energies. Supporting information for this article is available on the WWW under http://dx.doi.org/. (DOCX 34 kb)

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Marjolin, A., Gourlaouen, C., Clavaguéra, C. et al. Hydration gibbs free energies of open and closed shell trivalent lanthanide and actinide cations from polarizable molecular dynamics. J Mol Model 20, 2471 (2014). https://doi.org/10.1007/s00894-014-2471-6

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