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Many-body potentials for aqueous Li+, Na+, Mg2+ and Al3+: Comparison of effective three-body potentials and poliarizable models
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry.
Uppsala University, Disciplinary Domain of Science and Technology, Chemistry, Department of Materials Chemistry.
2004 (English)In: Journal of Chemical Physics, ISSN 0021-9606, E-ISSN 1089-7690, Vol. 120, no 10, 4829-4843 p.Article in journal (Refereed) Published
Abstract [en]

Many-body potentials for the aqueous Li+, Na+, Mg2+, and Al3+ ions have been constructed from ab initio cluster calculations. Pure pair, effective pair, effective three-body, and effective polarizable models were created and used in subsequent molecular dynamics simulations. The structures of the first and second solvation shells were studied using radial distribution functions and angular-radial distribution functions. The effective three-body and polarizable potentials yield similar first-shell structures, while the contraction of the O–O distances between the first and second solvation shells is more pronounced with the polarizable potentials. The definition of the tilt angle of the water molecules around the ions is discussed. When a proper definition is used, it is found that for Li+, Mg2+, and Al3+ the water molecules prefer a trigonal orientation, but for Na+ a tetrahedral orientation (ion in lone-pair direction) is preferred. The self-diffusion coefficients for the water molecules and the ions were calculated; the ionic values follow the order obtained from experiment, although the simulated absolute values are smaller than experiment for Mg2+ and Al3+.

Place, publisher, year, edition, pages
2004. Vol. 120, no 10, 4829-4843 p.
National Category
Inorganic Chemistry
Identifiers
URN: urn:nbn:se:uu:diva-67824DOI: 10.1063/1.1641191OAI: oai:DiVA.org:uu-67824DiVA: diva2:95735
Available from: 2006-03-21 Created: 2006-03-21 Last updated: 2017-11-21Bibliographically approved
In thesis
1. Cation Solvation in Water and Acetonitrile from Theoretical Calculations
Open this publication in new window or tab >>Cation Solvation in Water and Acetonitrile from Theoretical Calculations
2003 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

Metal ions solvated in aqueous, non-aqueous, and mixtures of solvents occur in many chemical contexts, for example in electrochemical applications and solvent separation. Solvated ions appear in high concentration in the living organisms, where their presence or absence can fundamentally alter the functions of life. In many of these cases, understanding the selective solvation and the dynamics of the ions is essential for the understanding of the processes involved.

Computer simulation provides a molecular level of detail of the solvation process usually not available from experiments. The quality of the interaction models employed in the theoretical description is of particular importance, since even rather small changes in the interaction can lead to substantial and qualitative differences.

This thesis describes the development of a sequence of increasingly refined analytical ion-solvent potentials from ab initio calculations for the systems Li+(aq), Na+(aq), Mg2+(aq), Al3+(aq), Li+(MeCN), Na+(MeCN), Li+(aq, MeCN), and Na+(aq, MeCN). Molecular dynamics simulations using these potentials were subsequently performed, and some key-properties computed. The reliability of the computed thermodynamical, structural and dynamical properties was scrutinized.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2003. 45 p.
Series
Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1104-232X ; 892
Keyword
Inorganic chemistry, molecular dynamics, ab initio, lithium, sodium, magnesium, aluminum, metal ion, water, acetonitrile, solution, solvation, Oorganisk kemi
National Category
Inorganic Chemistry
Identifiers
urn:nbn:se:uu:diva-3598 (URN)91-554-5751-7 (ISBN)
Public defence
2003-10-24, 2001, The Ångström Laboratory, Uppsala, 10:15
Opponent
Supervisors
Available from: 2003-10-03 Created: 2003-10-03 Last updated: 2013-07-24Bibliographically approved

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Spångberg, DanielHermansson, Kersti

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