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X-ray absorption spectroscopy on electrochemically oxidized Cu exposed to Na2S
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Soft X-Ray Physics.
Department of Chemistry, The University of Western Ontario, London, Ontario N6A 5B7, Canada.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Soft X-Ray Physics.
Uppsala University, Disciplinary Domain of Science and Technology, Physics, Department of Physics and Astronomy, Soft X-Ray Physics.
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2011 (English)In: Corrosion Science, ISSN 0010-938X, E-ISSN 1879-0496, Vol. 54, p. 85-89Article in journal (Refereed) Published
Abstract [en]

Copper surfaces have been investigated by X-ray absorption spectroscopy after electrochemical oxidation and subsequent exposure to sulfide solution. Oxide surface layers on bulk copper surfaces were electrochemically grown in anaqueous NaOH solution at two different potentials and the resulting chemical composition was investigated using X-ray absorption spectroscopy. At both potentials the resulting surfaces consisted largely of Cu2O. At the more strongly oxidizing potential, an admixture of Cu2+-containing phases – mostly Cu(OH)2 – was detected. Sulfide exposure of both surfaces was found to completely reduce the surface from Cu2+ to Cu1+ and resulted in the formation of Cu2S with an admixture of Cu2O.

Place, publisher, year, edition, pages
Amsterdam: Elsevier , 2011. Vol. 54, p. 85-89
Keywords [en]
Copper, AFS (EXAFS & XANES), Sulphidation
National Category
Atom and Molecular Physics and Optics
Research subject
Physics with spec. in Atomic, Molecular and Condensed Matter Physics
Identifiers
URN: urn:nbn:se:uu:diva-149328DOI: 10.1016/j.corsci.2011.09.001ISI: 000297894000012OAI: oai:DiVA.org:uu-149328DiVA, id: diva2:404561
Available from: 2011-03-17 Created: 2011-03-17 Last updated: 2017-12-11Bibliographically approved
In thesis
1. Redox Reactions in Li-ion Battery Cycling and in Cu Corrosion Studied by Soft X-ray Spectroscopy
Open this publication in new window or tab >>Redox Reactions in Li-ion Battery Cycling and in Cu Corrosion Studied by Soft X-ray Spectroscopy
2011 (English)Doctoral thesis, comprehensive summary (Other academic)
Abstract [en]

The topic of this thesis is redox reactions in two technologically important contexts: firstly, in Li-ion battery electrodes during cycling, and secondly, in copper corrosion in oxygen-free ground water containing sulfide. In an attempt to expand the understanding of the charge uptake process in battery electrodes and the chemical reactions on copper surfaces upon sulfide exposure, soft X-ray spectroscopy has been used to study the electronic structure of these systems.

To ascertain the changes in electron density at different atomic sites in a battery electrode material, both X-ray absorption spectroscopy (XAS) and resonant inelastic X-ray scattering (RIXS) have been applied to different electrode materials. This thesis explains in detail the assembling procedure, cycling, and situ sample preparation of the battery materials. Furthermore, two different designs used in in situ experiments for study of batteries during cycling are also discussed.

The main result from the Li-ion battery materials is the justification to abandon the view of valences as integers. This is true for all battery electrodes examined in this thesis. Generally, oxygen plays a more important role in the charge uptake than commonly assumed, but also the transition metals and other species apart from expected behavior. In LiMnPO4, even the notion of Li as strictly Li+ must be questioned.

Copper is intended to act as a corrosion barrier in a nuclear waste repository. In the corrosion experiments presented in this thesis, different copper oxides were exposed to the conditions present at the planned repository site, with exception for the concentration of sulfide, which was greatly increased.

The conclusion from these experiments is that sulfide effectively reduces Cu(II) oxide to Cu(I) compounds and possibly forms a compound containing both oxygen and sulfur. Also, the thickness and inhomogeneity of the copper oxide surface layers are of great importance for the corrosion mechanisms, including passivation.

Place, publisher, year, edition, pages
Uppsala: Acta Universitatis Upsaliensis, 2011. p. 69
Series
Digital Comprehensive Summaries of Uppsala Dissertations from the Faculty of Science and Technology, ISSN 1651-6214 ; 812
National Category
Physical Sciences
Identifiers
urn:nbn:se:uu:diva-148396 (URN)978-91-554-8036-3 (ISBN)
Public defence
2011-05-06, room 2001, Ångströmlaboratoriet, Lägerhyddsvägen 1, Uppsala, 13:15 (English)
Opponent
Supervisors
Available from: 2011-04-14 Created: 2011-03-05 Last updated: 2011-05-05Bibliographically approved

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Hollmark, HåkanVegelius, JohanWerme, LarsDuda, Laurent

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