Interaction of hydrogen with actinide dioxide (111) surfaces

Pegg, James T., Shields, Ashley E., Storr, Mark T., Scanlon, David O. and de Leeuw, Nora H. ORCID: https://orcid.org/0000-0002-8271-0545 2019. Interaction of hydrogen with actinide dioxide (111) surfaces. Journal of Chemical Physics 150 (13) , 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.

Item Type:	Article
Date Type:	Publication
Status:	Published
Schools:	Schools > Chemistry Research Institutes & Centres > Cardiff Catalysis Institute (CCI)
Publisher:	American Institute of Physics (AIP)
ISSN:	0021-9606
Funders:	EPSRC
Date of First Compliant Deposit:	9 May 2019
Date of Acceptance:	3 March 2019
Last Modified:	06 Nov 2024 12:45
URI:	https://orca.cardiff.ac.uk/id/eprint/122307

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