Journal
DALTON TRANSACTIONS
Volume 42, Issue 13, Pages 4570-4578Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/c3dt32536a
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Funding
- U.S. Department of Energy's National Nuclear Security Administration [DE-AC04-94AL85000]
- Used Fuel Disposition Campaign of the U. S. Department of Energy's Office of Nuclear Energy
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We report density functional calculations of the surface properties and chemistry of UO2(111) performed within the generalized gradient approximation corrected with an effective Hubbard parameter (GGA + U within Dudarev's formalism) to account for the strong on-site Coulomb repulsion between U 5f electrons. The variation of the properties of periodic slab models, with collinear ferromagnetic and antiferromagnetic arrangements of the uranium magnetic moments, was investigated while ramping up the effective Hubbard parameter from U-eff = 0 eV, corresponding to standard density functional theory, up to U-eff = 4 eV, the value that correctly reproduces the antiferromagnetic ground state of bulk UO2. The chemical interactions of molecular water, dissociated water, dissociated oxygen and co-adsorbed molecular water and monatomic oxygen with the UO2(111) surface were also studied as functions of the U-eff parameter. Calculations reveal that some of the key electronic and chemical properties controlling the surface reactivity are very sensitive to the value of this strong electron correlation parameter.
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