Artículo
A hydrated ion model of [UO2]2+ in water: Structure, dynamics, and spectroscopy from classical molecular dynamics
Autor/es | Pérez Conesa, Sergio
Torrico Perdomo, Francisco Miguel Martínez Fernández, José Manuel Rodríguez Pappalardo, Rafael Sánchez Marcos, Enrique |
Coordinador/Director | Sánchez Marcos, Enrique |
Departamento | Universidad de Sevilla. Departamento de Química Física |
Fecha de publicación | 2016-12 |
Fecha de depósito | 2020-04-23 |
Publicado en |
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Resumen | 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 ... 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 [UO2(H2O)5 ] 2+ 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 [UO2(H2O)5 ] 2+ 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. |
Agencias financiadoras | Junta de Andalucía |
Identificador del proyecto | P11-FQM 7607 |
Cita | Pérez Conesa, S., Torrico Perdomo, F.M., Martínez Fernández, J.M., Rodríguez Pappalardo, R. y Sánchez Marcos, E. (2016). A hydrated ion model of [UO2]2+ in water: Structure, dynamics, and spectroscopy from classical molecular dynamics. The Journal of Chemical Physics, 145 (22), 224502. |
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