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Interaction of hydrogen with actinide dioxide (111) surfaces

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. Green open access

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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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