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

• Published in: Journal of molecular modeling Vol. 20; no. 10; p. 2471
• Main Authors: Marjolin, Aude, Gourlaouen, Christophe, Clavaguéra, Carine, Ren, Pengyu Y., Piquemal, Jean-Philip, Dognon, Jean-Pierre
• Format: Journal Article
• Language: English
• Published: Berlin/Heidelberg Springer Berlin Heidelberg 01-10-2014; Springer Verlag (Germany)
• Subjects: Actinoid Series Elements - chemistry; Cations; Characterization and Evaluation of Materials; Chemical Sciences; Chemistry; Chemistry and Materials Science; Computer Appl. in Life Sciences; Computer Applications in Chemistry; Coordination chemistry; Energy Transfer; Lanthanoid Series Elements - chemistry; Molecular Dynamics Simulation; Molecular Medicine; Molecular Structure; Original Paper; Solvents - chemistry; Structure-Activity Relationship; Theoretical and Computational Chemistry; Topical Collection QUITEL 2013; Water - chemistry; Polarizable force fields; Hydration free energy; Actinides; Lanthanides; f-elements
• ISSN: 1610-2940; 0948-5023
• DOI: 10.1007/s00894-014-2471-6

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