UCL Discovery
UCL home » Library Services » Electronic resources » UCL Discovery

Interaction of hydrogen with actinide dioxide (011) surfaces

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. Green open access

[thumbnail of Article]
Preview
Text (Article)
Scanlon_5.0010200.pdf - Published Version

Download (10MB) | Preview
[thumbnail of Supplementary Information]
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
Downloads since deposit
111Downloads
Download activity - last month
Download activity - last 12 months
Downloads by country - last 12 months

Archive Staff Only

View Item View Item