Relativistic density functional investigation of Pu(H2O)n3+ clusters

Blaudeau, Jean‐Philippe; Zygmunt, Stan; Curtiss, L.A.; Reed, Donald T.; Bursten, Bruce E.

doi:10.1016/s0009-2614(99)00784-8

Cited by 29 publications

(40 citation statements)

References 21 publications

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“…A series of XAFS and theoretical studies indicated that An(III) seemed to be eight‐ or nine‐coordinate in aqueous solution . Wiebke et al reported the QM study of An(III) hydration for all actinide elements.…”

Section: Actinide Computational Chemistry Associated With Exafs and Xmentioning

confidence: 99%

Exploring Actinide Materials Through Synchrotron Radiation Techniques

et al. 2014

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Synchrotron radiation (SR) based techniques have been utilized with increasing frequency in the past decade to explore the brilliant and challenging sciences of actinide‐based materials. This trend is partially driven by the basic needs for multi‐scale actinide speciation and bonding information and also the realistic needs for nuclear energy research. In this review, recent research progresses on actinide related materials by means of various SR techniques were selectively highlighted and summarized, with the emphasis on X‐ray absorption spectroscopy, X‐ray diffraction and scattering spectroscopy, which are powerful tools to characterize actinide materials. In addition, advanced SR techniques for exploring future advanced nuclear fuel cycles dealing with actinides are illustrated as well.

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Section: Actinide Computational Chemistry Associated With Exafs and Xmentioning

confidence: 99%

Exploring Actinide Materials Through Synchrotron Radiation Techniques

et al. 2014

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“…This analogy is usually attributed to the hardness of the Ln 3+ ions: their coordinations mainly depend upon the steric and electrostatic nature of the ligand interactions 19 . For the same reason, the 4f-block lanthanide elements are also chemical analogues of the 5f-block actinide elements, when at the same oxidation state 20,21,22,23,24,25 . Actually, in the nuclear fuel cycle industry, it is a challenge to separate the Am and Cm actinide activation products from (light) lanthanide fission products in an attempt to eliminate long live radionuclides from radioactive wastes.…”

Section: Introductionmentioning

confidence: 97%

Pair interaction potentials with explicit polarization for molecular dynamics simulations of La3+ in bulk water

Duvail

Souaille

Spezia

et al. 2007

The Journal of Chemical Physics

108

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Pair interaction potentials (IPs) were defined to describe the La(3+)-OH(2) interaction for simulating the La(3+) hydration in aqueous solution. La(3+)-OH(2) IPs are taken from the literature or parametrized essentially to reproduce ab initio calculations at the second-order Moller-Plesset level of theory on La(H(2)O)(8) (3+). The IPs are compared and used with molecular dynamics (MD) including explicit polarization, periodic boundary conditions of La(H(2)O)(216) (3+) boxes, and TIP3P water model modified to include explicit polarization. As expected, explicit polarization is crucial for obtaining both correct La-O distances (r(La-O)) and La(3+) coordination number (CN). Including polarization also modifies hydration structure up to the second hydration shell and decreases the number of water exchanges between the La(3+) first and second hydration shells. r(La-O) ((1))=2.52 A and CN((1))=9.02 are obtained here for our best potential. These values are in good agreement with experimental data. The tested La-O IPs appear to essentially account for the La-O short distance repulsion. As a consequence, we propose that most of the multibody effects are correctly described by the explicit polarization contributions even in the first La(3+) hydration shell. The MD simulation results are slightly improved by adding a-typically negative 1r(6)-slightly attractive contribution to the-typically exponential-repulsive term of the La-O IP. Mean residence times are obtained from MD simulations for a water molecule in the first (1082 ps) and second (7.6 ps) hydration shells of La(3+). The corresponding water exchange is a concerted mechanism: a water molecule leaving La(H(2)O)(9) (3+) in the opposite direction to the incoming water molecule. La(H(2)O)(9) (3+) has a slightly distorded "6+3" tricapped trigonal prism D(3h) structure, and the weakest bonding is in the medium triangle, where water exchanges take place.

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“…[15][16][17] Since the early studies, solvent effects were recognized as an important factor to be considered. They were accounted either by a discrete model of one or two solvation shells, [18][19][20][21][22] or by the inclusion of the hydrated ion within a a) Electronic mail: sanchez@us.es dielectric continuum, [23][24][25][26][27][28][29] as had previously been proposed for other metal cation hydrations. 30,31 The powerful QM approach must be completed with a statistical mechanical picture of the dynamic hydration phenomenon.…”

Section: Introductionmentioning

confidence: 99%

A hydrated ion model of [UO2]2+ in water: Structure, dynamics, and spectroscopy from classical molecular dynamics

Pérez-Conesa

Torrico

Martı́nez

et al. 2016

The Journal of Chemical Physics

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A new ab initio interaction potential based on the hydrated ion concept has been developed to obtain the structure, energetics, and dynamics of the hydration of uranyl in aqueous solution. It is the first force field that explicitly parameterizes the interaction of the uranyl hydrate with bulk water molecules to accurately define the second-shell behavior. The [UO(HO)] presents a first hydration shell U-O average distance of 2.46 Å and a second hydration shell peak at 4.61 Å corresponding to 22 molecules using a coordination number definition based on a multisite solute cavity. The second shell solvent molecules have longer mean residence times than those corresponding to the divalent monatomic cations. The axial regions are relatively de-populated, lacking direct hydrogen bonding to apical oxygens. Angle-solved radial distribution functions as well as the spatial distribution functions show a strong anisotropy in the ion hydration. The [UO(HO)] solvent structure may be regarded as a combination of a conventional second hydration shell in the equatorial and bridge regions, and a clathrate-like low density region in the axial region. Translational diffusion coefficient, hydration enthalpy, power spectra of the main vibrational modes, and the EXAFS spectrum simulated from molecular dynamics trajectories agree fairly well with the experiment.

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Relativistic density functional investigation of Pu(H2O)n3+ clusters

Cited by 29 publications

References 21 publications

Exploring Actinide Materials Through Synchrotron Radiation Techniques

Exploring Actinide Materials Through Synchrotron Radiation Techniques

Pair interaction potentials with explicit polarization for molecular dynamics simulations of La3+ in bulk water

A hydrated ion model of [UO2]2+ in water: Structure, dynamics, and spectroscopy from classical molecular dynamics

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