Pegg, JT;
Shields, AE;
Storr, MT;
Scanlon, DO;
de Leeuw, NH;
(2019)
Interaction of hydrogen with actinide dioxide (111) surfaces.
Journal of Chemical Physics
, 150
(13)
, Article 134701. 10.1063/1.5087577.
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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.
| Type: | Article |
|---|---|
| Title: | Interaction of hydrogen with actinide dioxide (111) surfaces |
| Open access status: | An open access version is available from UCL Discovery |
| DOI: | 10.1063/1.5087577 |
| Publisher version: | https://doi.org/10.1063/1.5087577 |
| Language: | English |
| Additional information: | This version is the author accepted manuscript. For information on re-use, please refer to the publisher’s terms and conditions. |
| 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/10072727 |
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