Development and application of effective pairwise potentials for UO2n+, NpO2n+, PuO2n+, and AmO2n+ (n = 1, 2) ions with water

Pomogaev, Vladimir A.; Tiwari, Surya Prakash; Rai, Neeraj; Goff, George S.; Runde, Wolfgang; Schneider, William F.; Maginn, Edward J.

doi:10.1039/c3cp52444b

Cited by 47 publications

(73 citation statements)

References 84 publications

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“…All simulations were performed by using NAMD 2.10 program . The force field parameters used to describe uranyl were taken from a recent work . The proposed intramolecular parameters performed well for the description of uranyl in water system.…”

Section: Methodsmentioning

confidence: 99%

Study on the interaction of uranyl with sulfated beta‐cyclodextrin by affinity capillary electrophoresis and molecular dynamics simulation

Zhang

et al. 2016

Electrophoresis

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The study on sulfated beta-cyclodextrin binding to uranyl ion helps to get a better understanding of uranyl compounds' intermolecular interaction mechanism and facilitates the structure-based design of uranyl binding molecules. Here we investigated the electromigration of the inclusion complex by using affinity capillary electrophoresis in acidic solution. The binding constant was determined to be logK = 2.96 ± 0.02 (R = 0.996) through nonlinear regression approach. The possible configurations and structural features of the inclusion complex were further studied by molecular dynamics simulation. The results suggest the distinctions of coordination environment and hydration compared with bare uranyl ion in aqueous solution. Thus, two water oxygen atoms coordinated with uranyl in the first hydration shell at 2.55 angstrom instead of five in the same distance range. The binding free energy was calculated as -12.10 ± 1.46 kcal/mol by means of thermodynamic perturbation method. The negative value indicates that the process of S-β-CD capture uranyl ion in the aqueous media is spontaneous.

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Section: Methodsmentioning

confidence: 99%

Study on the interaction of uranyl with sulfated beta‐cyclodextrin by affinity capillary electrophoresis and molecular dynamics simulation

Zhang

et al. 2016

Electrophoresis

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“…Wipff and Guilbaud 33,79 and Keristi and Liu 34 from MD using empirical interaction potentials, and Siboulet et al 21 from QM computations found one hydrogen atom at around 1.8 Å from the uranyl oxygen forming typical hydrogen bonding. On the contrary, Roos et al 35 and Maginn et al 37,38 with classical MD using ab initio potentials; Bühl et al, 77 Frick et al, 42 and Nichols et al 41 using ab initio MD did not find preferential HB formation; furthermore, a low density number region is obtained, which led them to propose a rather hydrophobic behaviour in the uranyl axial region.…”

Section: B Hydration Structure Of Uranyl In Aqueous Solutionmentioning

confidence: 98%

“…In this work the importance of introducing charge transfer terms to describe the hydrate of a doubly charged ion in solution, such as uranyl, was shown. Maginn et al 37,38 considered the importance of polarization and other many-body effects in the binding of water molecules to the cation. They developed another firstprinciples force field for uranyl by parameterizing the interaction energies of the cation in the presence of four hydration water molecules.…”

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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“…All the actinyls of this study have open-shell electron configurations except uranyl. We will evaluate the goodness of the DFT mean field treatment of static electronic correlation effects to provide an accurate enough EXAFS spectrum prediction for open-shell actinyls, since DFT has shown the ability of our model to reproduce many other experimental properties [23,34,35]. To get insight into this question and check the EXAFS sensitivity to minute structural changes, multi-reference NEVPT2 [36][37][38] computations have been performed to build a [NpO 2 ] + −H 2 O interaction potential based on this quantum-mechanical level.…”

Section: Introductionmentioning

confidence: 99%

Combining EXAFS and Computer Simulations to Refine the Structural Description of Actinyls in Water

et al. 2020

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EXAFS spectroscopy is one of the most used techniques to solve the structure of actinoid solutions. In this work a systematic analysis of the EXAFS spectra of four actinyl cations, [UO2]2+, [NpO2]2+, [NpO2]+ and [PuO2]2+ has been carried out by comparing experimental results with theoretical spectra. These were obtained by averaging individual contributions from snapshots taken from classical Molecular Dynamics simulations which employed a recently developed [AnO2]2+/+ –H2O force field based on the hydrated ion model using a quantum-mechanical (B3LYP) potential energy surface. Analysis of the complex EXAFS signal shows that both An-Oyl and An-OW single scattering paths as well as multiple scattering ones involving [AnO2]+/2+ molecular cation and first-shell water molecules are mixed up all together to produce a very complex signal. Simulated EXAFS from the B3LYP force field are in reasonable agreement for some of the cases studied, although the k= 6–8 Å−1 region is hard to be reproduced theoretically. Except uranyl, all studied actinyls are open-shell electron configurations, therefore it has been investigated how simulated EXAFS spectra are affected by minute changes of An-O bond distances produced by the inclusion of static and dynamic electron correlation in the quantum mechanical calculations. A [NpO2]+−H2O force field based on a NEVPT2 potential energy surface has been developed. The small structural changes incorporated by the electron correlation on the actinyl aqua ion geometry, typically smaller than 0.07 Å, leads to improve the simulated spectrum with respect to that obtained from the B3LYP force field. For the other open-shell actinyls, [NpO2]2+ and [PuO2]2+, a simplified strategy has been adopted to improve the simulated EXAFS spectrum. It is computed taking as reference structure the NEVPT2 optimized geometry and including the DW factors of their corresponding MD simulations employing the B3LYP force field. A better agreement between the experimental and the simulated EXAFS spectra is found, confirming the a priori guess that the inclusion of dynamic and static correlation refine the structural description of the open-shell actinyl aqua ions.

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Development and application of effective pairwise potentials for UO2n+, NpO2n+, PuO2n+, and AmO2n+ (n = 1, 2) ions with water

Cited by 47 publications

References 84 publications

Study on the interaction of uranyl with sulfated beta‐cyclodextrin by affinity capillary electrophoresis and molecular dynamics simulation

Study on the interaction of uranyl with sulfated beta‐cyclodextrin by affinity capillary electrophoresis and molecular dynamics simulation

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

Combining EXAFS and Computer Simulations to Refine the Structural Description of Actinyls in Water

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