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

Authors
  • Sebbari, Karim
  • Roques, Jérôme
  • Domain, Christophe
  • Simoni, Eric
Type
Published Article
Journal
The Journal of Chemical Physics
Publisher
American Institute of Physics
Publication Date
Oct 28, 2012
Volume
137
Issue
16
Pages
164701–164701
Identifiers
DOI: 10.1063/1.4759506
PMID: 23126731
Source
Medline
License
Unknown

Abstract

The behavior of the UO(2)(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 Å 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(U-O(adsorption))=2.39 Å. 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.

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