Uranyl ion interaction at the water/NiO(100) interface: A predictive investigation by first-principles molecular dynamic simulations

Journal Article · Sun Oct 28 00:00:00 EDT 2012 · Journal of Chemical Physics

DOI:https://doi.org/10.1063/1.4759506· OSTI ID:22099069

Sebbari, Karim ^[1]; Roques, Jerome; Simoni, Eric ^[2]; Domain, Christophe ^[1]

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1. EDF-R and D, Departement Materiaux et Mecanique des Composants, Les Renardieres, Ecuelles, 77818 Moret Sur Loing (France)
2. Institut de Physique Nucleaire d'Orsay, Universite Paris-Sud, CNRS UMR 8608, 15 rue Georges Clemenceau, Batiment 100, 91406 Orsay Cedex (France)

The behavior of the UO{sub 2}{sup 2+} uranyl ion at the water/NiO(100) interface was investigated for the first time using Born-Oppenheimer molecular dynamic simulations with the spin polarized DFT +U extension. A water/NiO(100) interface model was first optimized on a defect-free five layers slab thickness, proposed as a reliable surface model, with an explicit treatment of the solvent. Water molecules are adsorbed with a well-defined structure in a thickness of about 4 A above the surface. The first layer, adsorbed on nickel atoms, remains mainly in molecular form but can partly dissociate at 293 K. Considering low acidic conditions, a bidentate uranyl ion complex was characterized on two surface oxygen species (arising from water molecules adsorption on nickel atoms) with d{sub U-O{sub a{sub d{sub s{sub o{sub r{sub p{sub t{sub i{sub o{sub n}}}}}}}}}}}=2.39 A. This complex is stable at 293 K due to iono-covalent bonds with an estimated charge transfer of 0.58 electron from the surface to the uranyl ion.

• OSTI ID: 22099069
• Journal Information: Journal of Chemical Physics, Vol. 137, Issue 16; Other Information: (c) 2012 American Institute of Physics; Country of input: International Atomic Energy Agency (IAEA); ISSN 0021-9606
• Country of Publication: United States
• Language: English

Related Subjects

37 INORGANIC
ORGANIC
PHYSICAL AND ANALYTICAL CHEMISTRY
75 CONDENSED MATTER PHYSICS
SUPERCONDUCTIVITY AND SUPERFLUIDITY
ADSORPTION
BORN-OPPENHEIMER APPROXIMATION
CHEMICAL BONDS
DISSOCIATION
INTERFACES
ION-MOLECULE COLLISIONS
IONS
MOLECULAR DYNAMICS METHOD
NICKEL OXIDES
SIMULATION
SPIN ORIENTATION
SURFACES
TEMPERATURE RANGE 0273-0400 K
URANYL COMPOUNDS
WATER