Pegg, JT;
Shields, AE;
Storr, MT;
Scanlon, DO;
De Leeuw, NH;
(2020)
Interaction of hydrogen with actinide dioxide (011) surfaces.
The Journal of Chemical Physics
, 153
(1)
, Article 014705. 10.1063/5.0010200.
Preview |
Text (Article)
Scanlon_5.0010200.pdf - Published Version Download (10MB) | Preview |
Preview |
Text (Supplementary Information)
Scanlon_hydrogen_011_surfaceesi.pdf - Published Version Download (1MB) | Preview |
Abstract
The corrosion and oxidation of actinide metals, leading to the formation of metal-oxide surface layers with the catalytic evolution of hydrogen, impacts the management of nuclear materials. Here, the interaction of hydrogen with actinide dioxide (AnO2, An = U, Np, or Pu) (011) surfaces by Hubbard corrected density functional theory (PBEsol+U) has been studied, including spin–orbit interactions and non-collinear 3k anti-ferromagnetic behavior. The actinide dioxides crystalize in the fluorite-type structure, and although the (111) surface dominates the crystal morphology, the (011) surface energetics may lead to more significant interaction with hydrogen. The dissociative adsorption of hydrogen on the UO2 (0.44 eV), NpO2 (−0.47 eV), and PuO2 (−1.71 eV) (011) surfaces has been calculated. It is found that hydrogen dissociates on the PuO2 (011) surface; however, UO2 (011) and NpO2 (011) surfaces are relatively inert. Recombination of hydrogen ions is likely to occur on the UO2 (011) and NpO2 (011) surfaces, whereas hydroxide formation is shown to occur on the PuO2 (011) surface, which distorts the surface structure.
| Type: | Article |
|---|---|
| Title: | Interaction of hydrogen with actinide dioxide (011) surfaces |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1063/5.0010200 |
| Publisher version: | https://doi.org/10.1063/5.0010200 |
| Language: | English |
| Additional information: | This version is the version of record. For information on re-use, please refer to the publisher’s terms and conditions. |
| Keywords: | Spin-orbit interactions, Electronic bandstructure, Corrosion, Nuclear fuel Catalysis, Chemisorption, Hubbard U corrected density functional theory, Physisorption, Actinides |
| UCL classification: | UCL UCL > Provost and Vice Provost Offices > UCL BEAMS UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences UCL > Provost and Vice Provost Offices > UCL BEAMS > Faculty of Maths and Physical Sciences > Dept of Chemistry |
| URI: | https://discovery.ucl.ac.uk/id/eprint/10104204 |
Archive Staff Only
 |
View Item |
