Development and Validation of an Integrated Computational Approach for the Study of Ionic Species in Solution by Means of Effective Two-Body Potentials. The Case of Zn2 +, Ni2 +, and Co2 + in Aqueous Solutions

Chillemi, Giovanni; D’Angelo, P.; Pavel, Nicolae Viorel; Sanna, Nico; Barone, Vincenzo

doi:10.1021/ja015686p

Cited by 93 publications

(133 citation statements)

References 37 publications

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“…2͒, predict 14 water molecules in the second shell region ͑3.5-4.7 Å͒ and nearly within the large range of values obtained from the analysis of the x-ray data, 45-50 7.6-13.2 waters. This number also agrees well with the results from several prior MD and QM/MM simulations 40,44,[51][52][53][54][55] and within the range of values of the conventional MD simulations. However, compared to these prior simulations our second shell maximum is found to be 5%-10% smaller.…”

Section: A the Hydration Shell Structuresupporting

confidence: 90%

Structure and dynamics of the hydration shells of the Zn2+ ion from ab initio molecular dynamics and combined ab initio and classical molecular dynamics simulations

Cauët

Bogatko

Weare

et al. 2010

The Journal of Chemical Physics

104

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Results of ab initio molecular dynamics ͑AIMD͒ simulations ͑density functional theory+ PBE96͒ of the dynamics of waters in the hydration shells surrounding the Zn 2+ ion ͑T Ϸ 300 K, Ϸ 1 gm/ cm 3 ͒ are compared to simulations using a combined quantum and classical molecular dynamics ͓AIMD/molecular mechanical ͑MM͔͒ approach. Both classes of simulations were performed with 64 solvating water molecules ͑ϳ15 ps͒ and used the same methods in the electronic structure calculation ͑plane-wave basis set, time steps, effective mass, etc.͒. In the AIMD/MM calculation, only six waters of hydration were included in the quantum mechanical ͑QM͒ region. The remaining 58 waters were treated with a published flexible water-water interaction potential. No reparametrization of the water-water potential was attempted. Additional AIMD/MM simulations were performed with 256 water molecules. The hydration structures predicted from the AIMD and AIMD/MM simulations are found to agree in detail with each other and with the structural results from x-ray data despite the very limited QM region in the AIMD/MM simulation. To further evaluate the agreement of these parameter-free simulations, predicted extended x-ray absorption fine structure ͑EXAFS͒ spectra were compared directly to the recently obtained EXAFS data and they agree in remarkable detail with the experimental observations. The first hydration shell contains six water molecules in a highly symmetric octahedral structure is ͑maximally located at 2.13-2.15 Å versus 2.072 Å EXAFS experiment͒. The widths of the peak of the simulated EXAFS spectra agree well with the data ͑8.4 Å 2 versus 8.9 Å 2 in experiment͒. Analysis of the H-bond structure of the hydration region shows that the second hydration shell is trigonally bound to the first shell water with a high degree of agreement between the AIMD and AIMD/MM calculations. Beyond the second shell, the bonding pattern returns to the tetrahedral structure of bulk water. The AIMD/MM results emphasize the importance of a quantum description of the first hydration shell to correctly describe the hydration region. In these calculations the full d 10 electronic structure of the valence shell of the Zn 2+ ion is retained. The simulations show substantial and complex charge relocation on both the Zn 2+ ion and the first hydration shell. The dipole moment of the waters in the first hydration shell is 3.4 D ͑3.3 D AIMD/MM͒ versus 2.73 D bulk. Little polarization is found for the waters in the second hydration shell ͑2.8 D͒. No exchanges were seen between the first and the second hydrations shells; however, many water transfers between the second hydration shell and the bulk were observed. For 64 waters, the AIMD and AIMD/MM simulations give nearly identical results for exchange dynamics. However, in the larger particle simulations ͑256 waters͒ there is a significant reduction in the second shell to bulk exchanges.

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Section: A the Hydration Shell Structuresupporting

confidence: 90%

Structure and dynamics of the hydration shells of the Zn2+ ion from ab initio molecular dynamics and combined ab initio and classical molecular dynamics simulations

Cauët

Bogatko

Weare

et al. 2010

The Journal of Chemical Physics

104

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“…However, exchange between second shell ligands and bulk take place much more readily: s res obtained by our simulation for Fe 2þ and Fe 3þ in the second hydration shell is 10 and 32 ps, respectively. For Fe 3þ , experimental data [18] for time binding are available with in the range 10 À10 to )10 À11 s, and are in fair agreement with our value, while for Fe 2þ only data for s res for hydrated Ni 2þ and Co 2þ with 10.3 and 4.5 ps are available from empirical potential simulations for comparison [32].…”

Section: Phasesupporting

confidence: 83%

Molecular dynamics simulation of the hydration of transition metal ions: the role of non-additive effects in the hydration shells of Fe2+ and Fe3+ ions

Remsungnen¹,

Rode²

2004

Chemical Physics Letters

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“…The corresponding force constants were taken from CHARMM22 force-field [23] which is based on high-level ab initio calculations. Ni(II)-water interactions were simulated with the potential proposed by Chillemi et al [24]. To our knowledge, there is no potential especially adapted to describe Ni(II)-glycerol interactions available in the literature.…”

Section: Methodsmentioning

confidence: 99%

Extensive NMRD studies of Ni(II) salt solutions in water and water–glycerol mixtures

Kowalewski

Egorov

Kruk

et al. 2008

Journal of Magnetic Resonance

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Development and Validation of an Integrated Computational Approach for the Study of Ionic Species in Solution by Means of Effective Two-Body Potentials. The Case of Zn^{2 +}, Ni^{2 +}, and Co^{2 +} in Aqueous Solutions

Cited by 93 publications

References 37 publications

Structure and dynamics of the hydration shells of the Zn2+ ion from ab initio molecular dynamics and combined ab initio and classical molecular dynamics simulations

Structure and dynamics of the hydration shells of the Zn2+ ion from ab initio molecular dynamics and combined ab initio and classical molecular dynamics simulations

Molecular dynamics simulation of the hydration of transition metal ions: the role of non-additive effects in the hydration shells of Fe2+ and Fe3+ ions

Extensive NMRD studies of Ni(II) salt solutions in water and water–glycerol mixtures

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