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  • 1.
    Bjorkbacka, Asa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Johnson, C. Magnus
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Role of the Oxide Layer in Radiation-Induced Corrosion of Copper in Anoxic Water2016In: The Journal of Physical Chemistry C, ISSN 1932-7447, E-ISSN 1932-7455, Vol. 120, no 21, p. 11450-11455Article in journal (Refereed)
    Abstract [en]

    The influence of a pregrown copper oxide layer on radiation-induced corrosion of polished copper in pure anoxic water has been explored. The resulting amount of copper oxide formed during corrosion was measured with cathodic reduction, and the concentration of dissolved copper in solution was measured with inductively coupled plasma atomic emission spectroscopy. The identity of corrosion products and their topography was determined with Raman spectroscopy and scanning electron microscopy, respectively. Nonirradiated reference samples were analyzed for comparison. The results show that radiation-induced corrosion of copper in anoxic water is significantly more effective on preoxidized copper compared to polished copper. The total amount of oxidized copper exceeds the amount expected solely from radiation chemistry of water by more than 3 orders of magnitude. To explain this discrepancy a mechanism is suggested where the hydroxyl radical (HO center dot) is the main radiolytic oxidative species driving the corrosion process. If the thermodynamic driving force would be large enough (such as for the hydroxyl radical or its precursor, H2O+), the oxide layer could conduct electrons from the metal to the hydroxyl radicals formed at oxide surfaces. The formation of an oxide layer will then result in an increased reactive surface area partly accounting for the observed discrepancy.

  • 2.
    Björkbacka, Åsa
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Radiation induced corrosion of copper2015Doctoral thesis, comprehensive summary (Other academic)
    Abstract [en]

    The process of radiation induced corrosion of copper is not well understood. The most obvious situation where the knowledge of this process is crucial is in a deep repository for high level spent nuclear fuel where the fuel will be sealed inside copper canisters. The radiation will penetrate the canisters and be absorbed by the surrounding environment. In this study gamma irradiations of polished and pre-oxidized copper cubes in anoxic pure water, air of 60-100 % RH and in humid argon were performed. The copper surfaces were examined using IRAS, XPS, cathodic reduction, SEM, AFM, and Raman spectroscopy. The concentration of copper in the reaction solutions was measured using ICP-OES.  Also the formation of oxidative species caused by radiation absorption of water was studied by numerical simulations using MAKSIMA software. The corrosion of copper during gamma irradiation vastly exceeds what is expected. The production of oxidative species caused by radiation absorption of water is hundreds of times too low to explain the amount of oxidized copper. A possible explanation for this mismatch is an enhanced radiation chemical yield of HO· on the copper surface. Another one is an increased surface area due to oxidation of copper. One speculation is that HO· interacting with the copper oxide can cause oxidation of the metal. If the thermodynamic driving force is large enough then electrons can be conducted from the metal through the oxide to the oxidant. A dramatic increase in surface area together with an increased interfacial yield of HO· might explain the radiation enhanced corrosion process.   

  • 3.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Hosseinpour, S.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Leygraf, Christopher
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Jonsson, M.
    KTH, School of Chemical Science and Engineering (CHE), Chemical Engineering and Technology.
    Erratum to: Radiation Induced Corrosion of Copper in Anoxic Aqueous Solution (vol 15, pg C5, 2012)2012In: Electrochemical and solid-state letters, ISSN 1099-0062, E-ISSN 1944-8775, Vol. 15, no 6, p. S5-S5Article in journal (Refereed)
  • 4.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Hosseinpour, Saman
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Johnson, Magnus
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Radiation induced corrosion of copper for spent nuclear fuel storage2013In: Radiation Physics and Chemistry, ISSN 0969-806X, E-ISSN 1879-0895, Vol. 92, p. 80-86Article in journal (Refereed)
    Abstract [en]

    The long term safety of repositories for radioactive waste is one of the main concerns for countries utilizing nuclear power. The integrity of engineered and natural barriers in such repositories must be carefully evaluated in order to minimize the release of radionuclides to the biosphere. One of the most developed concepts of long term storage of spent nuclear fuel is the Swedish KBS-3 method. According to this method, the spent fuel will be sealed inside copper canisters surrounded by bentonite clay and placed 500 m down in stable bedrock. Despite the importance of the process of radiation induced corrosion of copper, relatively few studies have been reported. In this work the effect of the total gamma dose on radiation induced corrosion of copper in anoxic pure water has been studied experimentally. Copper samples submerged in water were exposed to a series of total doses using three different dose rates. Unirradiated samples were used as reference samples throughout. The copper surfaces were examined qualitatively using IRAS and XPS and quantitatively using cathodic reduction. The concentration of copper in solution after irradiation was measured using ICP-AES. The influence of aqueous radiation chemistry on the corrosion process was evaluated based on numerical simulations. The experiments show that the dissolution as well as the oxide layer thickness increase upon radiation. Interestingly, the evaluation using numerical simulations indicates that aqueous radiation chemistry is not the only process driving the corrosion of copper in these systems.

  • 5.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. Show more KTH Royal Inst Technol, Sch Chem Sci & Engn, SE-10044 Stockholm, Sweden..
    Hosseinpour, Saman
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science. Show more KTH Royal Inst Technol, Sch Chem Sci & Engn, SE-10044 Stockholm, Sweden..
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science. Show more KTH Royal Inst Technol, Sch Chem Sci & Engn, SE-10044 Stockholm, Sweden..
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry. Show more KTH Royal Inst Technol, Sch Chem Sci & Engn, SE-10044 Stockholm, Sweden..
    Radiation Induced Corrosion of Copper in Anoxic Aqueous Solution2012In: Electrochemical and solid-state letters, ISSN 1099-0062, E-ISSN 1944-8775, Vol. 15, no 5, p. C5-C7Article in journal (Refereed)
    Abstract [en]

    The effect of gamma radiation on corrosion of copper under anoxic conditions in pure water has been studied experimentally. Copper samples submerged in water were exposed to dose rates of 0.37 or 0.77 kGy/h. Reference samples were used throughout. The copper surfaces have been examined using the techniques of SEM-EDS, IRAS, CR spectroscopy and AFM. Dissolution of copper was measured using ICP-OES. The results show that irradiated samples are more corroded than corresponding reference samples. This is also reflected by the increased concentration of copper in water after irradiation. Surface examination also reveals local corrosion features.

  • 6.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Johnson, C. Magnus
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Radiation Induced Corrosion of Copper in Humid Air and Argon Atmospheres2017In: Journal of the Electrochemical Society, ISSN 0013-4651, E-ISSN 1945-7111, Vol. 164, no 4, p. C201-C206Article in journal (Refereed)
    Abstract [en]

    Corrosion of copper is a key-issue in the safety assessment of deep geological repositories for spent nuclear fuel utilizing copper coated canisters to isolate the spent nuclear fuel from the surrounding environment. Of particular interest is the radiation induced corrosion attributed to the inherent radioactivity of the spent nuclear fuel. In this work we have studied the radiation induced corrosion of copper in humid air and argon atmospheres. Polished copper cubes were gamma irradiated in the environments mentioned above at ambient temperature. Reference samples, not irradiated but otherwise treated under the exact same conditions as the irradiated samples, were used throughout the study. The oxide layers formed during radiation exposure were studied using cathodic reduction, infrared reflection/absorption spectroscopy, and the surfaces were examined using scanning electron microscopy. When possible, the concentration of copper in solution was measured using inductively coupled plasma atomic emission spectroscopy. The experimental results clearly show that radiation induced corrosion of copper in humid air as well as in humid argon is significantly more extensive than the corresponding process in anaerobic water. This is well in line with the recently proposed mechanism for radiation-induced corrosion of copper in anaerobic water. The very similar behavior of copper irradiated in humid air and in humid argon implies that the radiolytically formed HNO3 in the case of humid air has negligible impact on the radiation-induced corrosion compared to the radiolytically formed hydroxyl radical.

  • 7.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Johnson, Magnus
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Radiation induced corrosion of copper in humid air and argonManuscript (preprint) (Other academic)
  • 8.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Johnson, Magnus
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    The role of the oxide layerin radiation induced corrosion of copper in anoxic waterManuscript (preprint) (Other academic)
  • 9.
    Björkbacka, Åsa
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Yang, Miao
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Gasparrini, Claudia
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Leygraf, Christofer
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Surface and Corrosion Science.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Kinetics and mechanisms of reactions between H2O2 and copper and copper oxides2015In: Dalton Transactions, ISSN 1477-9226, E-ISSN 1477-9234, Vol. 44, no 36, p. 16045-16051Article in journal (Refereed)
    Abstract [en]

    One of the main challenges for the nuclear power industry today is the disposal of spent nuclear fuel. One of the most developed methods for its long term storage is the Swedish KBS-3 concept where the spent fuel is sealed inside copper canisters and placed 500 meters down in the bedrock. Gamma radiation will penetrate the canisters and be absorbed by groundwater thereby creating oxidative radiolysis products such as hydrogen peroxide (H2O2) and hydroxyl radicals (HO[radical dot]). Both H2O2 and HO[radical dot] are able to initiate corrosion of the copper canisters. In this work the kinetics and mechanism of reactions between the stable radiolysis product, H2O2, and copper and copper oxides were studied. Also the dissolution of copper into solution after reaction with H2O2 was monitored by ICP-OES. The experiments show that both H2O2 and HO[radical dot] are present in the systems with copper and copper oxides. Nevertheless, these species do not appear to influence the dissolution of copper to the same extent as observed in recent studies in irradiated systems. This strongly suggests that aqueous radiolysis can only account for a very minor part of the observed radiation induced corrosion of copper.

  • 10.
    Norrfors, K. Karin
    et al.
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Björkbacka, Åsa
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Kessler, Amanda
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Wold, Susanna
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    Jonsson, Mats
    KTH, School of Engineering Sciences in Chemistry, Biotechnology and Health (CBH), Chemistry, Applied Physical Chemistry.
    γ-radiation induced corrosion of copper in bentonite-water systems under anaerobic conditions2018In: Radiation Physics and Chemistry, ISSN 0969-806X, E-ISSN 1879-0895, Vol. 144, p. 8-12Article in journal (Refereed)
    Abstract [en]

    In this work we have experimentally studied the impact of bentonite clay on the process of radiation-induced copper corrosion in anoxic water. The motivation for this is to further develop our understanding of radiation-driven processes occurring in deep geological repositories for spent nuclear fuel where copper canisters containing the spent nuclear fuel will be embedded in compacted bentonite. Experiments on radiation-induced corrosion in the presence and absence of bentonite were performed along with experiments elucidating the impact irradiation on the Cu2+ adsorption capacity of bentonite. The experiments presented in this work show that the presence of bentonite clay has no or very little effect on the magnitude of radiation-induced corrosion of copper in anoxic aqueous systems. The absence of a protective effect similar to that observed for radiation-induced dissolution of UO2 is attributed to differences in the corrosion mechanism. This provides further support for the previously proposed mechanism where the hydroxyl radical is the key radiolytic oxidant responsible for the corrosion of copper. The radiation effect on the bentonite sorption capacity of Cu2+ (reduced capacity) is in line with what has previously been reported for other cations. The reduced cation sorption capacity is partly attributed to a loss of Al-OH sites upon irradiation.

  • 11.
    Norrfors, Karin
    et al.
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Kessler, Amanda
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Björkbacka, Åsa
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Wold, Susanna
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Jonsson, Mats
    KTH, School of Chemical Science and Engineering (CHE), Chemistry, Applied Physical Chemistry.
    Radiation induced corrosion of copper in bentonite-water systems under anaerobic conditionsManuscript (preprint) (Other academic)
1 - 11 of 11
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