Computational analysis of the early stage of cuprous oxide sulphidation: a top-down process. (28th April 2017)

• Record Type: Journal Article
• Authors: Stenlid, J. H.; Johansson, A. J.; Leygraf, C.; Brinck, T.
• Is Part Of: Corrosion engineering, science, and technology. Volume 52(2017)Supplement 1
• Page Start: 50
• Page End: 53
• Publication Date: 2017-04-28
• Subjects: Density functional theory -- sulphidation -- cuprite (Cu2O) -- corrosion -- water (H2O) -- hydrogen sulphide (H2S) -- nuclear waste disposal -- chalcocite (Cu2S); Corrosion and anti-corrosives -- Periodicals; 620.11223
• DOI: 10.1080/1478422X.2017.1284393
• Languages: English
• ISSNs: 1478-422X

Abstract

ABSTRACT: The initial steps of Cu2 O sulphidation to Cu2 S have been studied using plane-wave density functional theory at the PBE-D3+U level of sophistication. Surface adsorption and dissociation of H2 S and H2 O, as well as the replacement reaction of lattice oxygen with sulphur, have been investigated for the most stable (111) and (100) surface facets under oxygen-lean conditions. We find that the (100) surface is more susceptible to sulphidation than the (111) surface, promoting both H2 S adsorption, dissociation and the continued oxygen–sulphur replacement. The results presented in this proceeding bridge previous results from high-vacuum experiments on ideal surface to more realistic corrosion conditions and set the grounds for future mechanistic studies. Potential implications on the long-term final disposal of spent nuclear fuel are discussed. This paper is part of a supplement on the 6th International Workshop on Long-Term Prediction of Corrosion Damage in Nuclear Waste Systems . GRAPHICAL ABSTRACT: