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Title: Solvation of the vanadate ion in seawater conditions from molecular dynamics simulations

Authors:
; ;
Publication Date:
Sponsoring Org.:
USDOE Office of Nuclear Energy (NE)
OSTI Identifier:
1416611
Grant/Contract Number:
NE0008397
Resource Type:
Journal Article: Publisher's Accepted Manuscript
Journal Name:
Inorganica Chimica Acta
Additional Journal Information:
Journal Volume: 458; Journal Issue: C; Related Information: CHORUS Timestamp: 2018-01-11 08:40:16; Journal ID: ISSN 0020-1693
Publisher:
Elsevier
Country of Publication:
Switzerland
Language:
English

Citation Formats

Priest, Chad, Zhou, Jingwei, and Jiang, De-en. Solvation of the vanadate ion in seawater conditions from molecular dynamics simulations. Switzerland: N. p., 2017. Web. doi:10.1016/j.ica.2016.12.027.
Priest, Chad, Zhou, Jingwei, & Jiang, De-en. Solvation of the vanadate ion in seawater conditions from molecular dynamics simulations. Switzerland. doi:10.1016/j.ica.2016.12.027.
Priest, Chad, Zhou, Jingwei, and Jiang, De-en. Wed . "Solvation of the vanadate ion in seawater conditions from molecular dynamics simulations". Switzerland. doi:10.1016/j.ica.2016.12.027.
@article{osti_1416611,
title = {Solvation of the vanadate ion in seawater conditions from molecular dynamics simulations},
author = {Priest, Chad and Zhou, Jingwei and Jiang, De-en},
abstractNote = {},
doi = {10.1016/j.ica.2016.12.027},
journal = {Inorganica Chimica Acta},
number = C,
volume = 458,
place = {Switzerland},
year = {Wed Mar 01 00:00:00 EST 2017},
month = {Wed Mar 01 00:00:00 EST 2017}
}

Journal Article:
Free Publicly Available Full Text
Publisher's Version of Record at 10.1016/j.ica.2016.12.027

Citation Metrics:
Cited by: 1work
Citation information provided by
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  • The raw single-ion solvation free energies computed from atomistic (explicit-solvent) simulations are extremely sensitive to the boundary conditions and treatment of electrostatic interactions used during these simulations. However, as shown recently [M. A. Kastenholz and P. H. Huenenberger, J. Chem. Phys. 124, 224501 (2006); M. M. Reif and P. H. Huenenberger, J. Chem. Phys. 134, 144103 (2010)], the application of appropriate correction terms permits to obtain methodology-independent results. The corrected values are then exclusively characteristic of the underlying molecular model including in particular the ion-solvent van der Waals interaction parameters, determining the effective ion size and the magnitude of itsmore » dispersion interactions. In the present study, the comparison of calculated (corrected) hydration free energies with experimental data (along with the consideration of ionic polarizabilities) is used to calibrate new sets of ion-solvent van der Waals (Lennard-Jones) interaction parameters for the alkali (Li{sup +}, Na{sup +}, K{sup +}, Rb{sup +}, Cs{sup +}) and halide (F{sup -}, Cl{sup -}, Br{sup -}, I{sup -}) ions along with either the SPC or the SPC/E water models. The experimental dataset is defined by conventional single-ion hydration free energies [Tissandier et al., J. Phys. Chem. A 102, 7787 (1998); Fawcett, J. Phys. Chem. B 103, 11181] along with three plausible choices for the (experimentally elusive) value of the absolute (intrinsic) hydration free energy of the proton, namely, {Delta}G{sub hyd} {sup O-minus} [H{sup +}]=-1100, -1075 or -1050 kJ mol{sup -1}, resulting in three sets L, M, and H for the SPC water model and three sets L{sub E}, M{sub E}, and H{sub E} for the SPC/E water model (alternative sets can easily be interpolated to intermediate {Delta}G{sub hyd} {sup O-minus} [H{sup +}] values). The residual sensitivity of the calculated (corrected) hydration free energies on the volume-pressure boundary conditions and on the effective ionic radius entering into the calculation of the correction terms is also evaluated and found to be very limited. Ultimately, it is expected that comparison with other experimental ionic properties (e.g., derivative single-ion solvation properties, as well as data concerning ionic crystals, melts, solutions at finite concentrations, or nonaqueous solutions) will permit to validate one specific set and thus, the associated {Delta}G{sub hyd} {sup O-minus} [H{sup +}] value (atomistic consistency assumption). Preliminary results (first-peak positions in the ion-water radial distribution functions, partial molar volumes of ionic salts in water, and structural properties of ionic crystals) support a value of {Delta}G{sub hyd} {sup O-minus} [H{sup +}] close to -1100 kJ{center_dot}mol{sup -1}.« less