Electrochemical Interface during Corrosion of Copper in Anoxic Sulfide-Containing Groundwater—A Computational Study
Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
Standard
Electrochemical Interface during Corrosion of Copper in Anoxic Sulfide-Containing Groundwater—A Computational Study. / Stenlid, Joakim Halldin; Dos Santos, Egon Campos; Bagger, Alexander; Johansson, Adam Johannes; Rossmeisl, Jan; Pettersson, Lars G. M.
I: The Journal of Physical Chemistry Part C, Bind 124, Nr. 1, 2020, s. 469-481.Publikation: Bidrag til tidsskrift › Tidsskriftartikel › Forskning › fagfællebedømt
Harvard
APA
Vancouver
Author
Bibtex
}
RIS
TY - JOUR
T1 - Electrochemical Interface during Corrosion of Copper in Anoxic Sulfide-Containing Groundwater—A Computational Study
AU - Stenlid, Joakim Halldin
AU - Dos Santos, Egon Campos
AU - Bagger, Alexander
AU - Johansson, Adam Johannes
AU - Rossmeisl, Jan
AU - Pettersson, Lars G. M.
PY - 2020
Y1 - 2020
N2 - Corrosion of copper is an expensive degradation process of materials in engineered infrastructures and in various technical applications. It is also an important factor in the geological disposal of spent nuclear fuel, where sulfide-induced corrosion is expected to be the predominant chemical degradation process of copper canisters used for encapsulation and isolation of the radioactive material from the biosphere. One aspect of the corrosion process that is still under intense research is the corrosion morphology and how it might be affected by the composition of the groundwater. Using density functional theory, we investigate the electrochemical interface of corroding copper in aqueous solutions containing sulfides, with and without the presence of Cl–, HCO3–, and SO42– anions. Through state-of-the-art electrochemical models, we account for the effects of pH, concentrations, and potential on the interfacial structure and composition. Results are presented for the Cu(110) surface facet and compared to the (110) and (001) facets of chalcocite (Cu2S), i.e., the main product of sulfide-induced corrosion. It is found that at low potentials, H dominates on all surfaces, and at high potentials, sulfides. In the intermediate ranges, the surfaces differ with sulfides prevailing on Cu, while adsorbed H2O, Cl, or H dominate on Cu2S. The results are summarized as surface Pourbaix diagrams and are generally applicable in corrosion science and electrochemistry. The implications of the study are discussed in light of the expected conditions of planned spent nuclear fuel repositories in Sweden, Finland, and Canada.
AB - Corrosion of copper is an expensive degradation process of materials in engineered infrastructures and in various technical applications. It is also an important factor in the geological disposal of spent nuclear fuel, where sulfide-induced corrosion is expected to be the predominant chemical degradation process of copper canisters used for encapsulation and isolation of the radioactive material from the biosphere. One aspect of the corrosion process that is still under intense research is the corrosion morphology and how it might be affected by the composition of the groundwater. Using density functional theory, we investigate the electrochemical interface of corroding copper in aqueous solutions containing sulfides, with and without the presence of Cl–, HCO3–, and SO42– anions. Through state-of-the-art electrochemical models, we account for the effects of pH, concentrations, and potential on the interfacial structure and composition. Results are presented for the Cu(110) surface facet and compared to the (110) and (001) facets of chalcocite (Cu2S), i.e., the main product of sulfide-induced corrosion. It is found that at low potentials, H dominates on all surfaces, and at high potentials, sulfides. In the intermediate ranges, the surfaces differ with sulfides prevailing on Cu, while adsorbed H2O, Cl, or H dominate on Cu2S. The results are summarized as surface Pourbaix diagrams and are generally applicable in corrosion science and electrochemistry. The implications of the study are discussed in light of the expected conditions of planned spent nuclear fuel repositories in Sweden, Finland, and Canada.
U2 - 10.1021/acs.jpcc.9b08657
DO - 10.1021/acs.jpcc.9b08657
M3 - Journal article
VL - 124
SP - 469
EP - 481
JO - The Journal of Physical Chemistry Part C
JF - The Journal of Physical Chemistry Part C
SN - 1932-7447
IS - 1
ER -
ID: 234882566