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Interaction of hydrogen with actinide dioxide (111) surfaces
Authors:
James T.
Pegg
(University College London; Atomic Weapons Establishment (AWE) Plc)
,
Ashley E.
Shields
(Oak Ridge National Laboratory)
,
Mark T.
Storr
(Atomic Weapons Establishment (AWE) Plc)
,
David O.
Scanlon
(University College London; Diamond Light Source)
,
Nora H.
De Leeuw
(University College London; Cardiff University)
Co-authored by industrial partner:
Yes
Type:
Journal Paper
Journal:
The Journal Of Chemical Physics
, VOL 150
State:
Published (Approved)
Published:
April 2019
Abstract: The interaction of atomic and molecular hydrogen with actinide dioxide (AnO2, An = U, Np, Pu) (111) surfaces has been investigated by DFT+U, where noncollinear 3k antiferromagnetic behaviour and spin-orbit interactions are considered. The adsorption of atomic hydrogen forms a hydroxide group, coupled to the reduction of an actinide ion. The energy of atomic hydrogen adsorption on the UO2 (0.82 eV), NpO2 (−0.10 eV), and PuO2 (−1.25 eV) surfaces has been calculated. The dissociation of molecular hydrogen is not observed, shown to be due to kinetic rather than thermodynamic factors. As a barrier to the formation of a second hydroxyl group, an unusual charge distribution has been shown. This could be a limitation of a (1·1) unit cell method or an artefact of the systems. The recombination of hydrogen ions on the AnO2 (111) surfaces is favoured over hydroxide formation.
Journal Keywords: Metal oxides; Corrosion; Adsorption; Spin-orbit interactions; Chemical elements; Chemisorption; Physisorption; Chemical compounds
Diamond Keywords: Antiferromagnetism
Subject Areas:
Materials,
Chemistry,
Physics
Technical Areas:
Added On:
04/02/2020 15:48
Discipline Tags:
Quantum Materials
Physics
Physical Chemistry
Hard condensed matter - structures
Chemistry
Corrosion
Materials Science
Technical Tags: