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  • 1
    Online-Ressource
    Online-Ressource
    Informa UK Limited ; 2004
    In:  Nuclear Technology Vol. 147, No. 1 ( 2004-07), p. 157-170
    In: Nuclear Technology, Informa UK Limited, Vol. 147, No. 1 ( 2004-07), p. 157-170
    Materialart: Online-Ressource
    ISSN: 0029-5450 , 1943-7471
    Sprache: Englisch
    Verlag: Informa UK Limited
    Publikationsdatum: 2004
    ZDB Id: 2132500-5
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 2
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2004
    In:  MRS Proceedings Vol. 824 ( 2004)
    In: MRS Proceedings, Springer Science and Business Media LLC, Vol. 824 ( 2004)
    Kurzfassung: Heat generated by radioactive decay of spent fuel represents a potentially important barrier to water accumulation on commercial spent nuclear fuel in breached waste packages. In the absence of water, fuel degradation and radionuclide release will be negligible. Thermal models for the proposed Yucca Mountain Repository suggest that, after a period of approximately 1000-4000 years (depending on loadingand ventilation conditions), the repository drift walls may decline to sub-boiling temperatures, thus allowing humidity in the drift to increase. The question thus arises, is the thermal gradient between the fuel and the drift sufficient to prevent water accumulation in a humid drift environment throughout the regulatory period? The answer depends on the balance between processes that oppose water condensation ontothe fuel (decay heat) and those that promote condensation such as the deliquescence of hygroscopic phaseswithin the fuel. Our experimental results indicate that deliquescence could lead to the condensation of water onto spent fuel despite the thermal “self-drying”effect if the following criteria are met: (1) the fission product salt CsI is present in the fuel or in the fuel-cladding gap, (2) the relative humidity in the driftexceeds 80% while temperatures in the waste package are around 90 o C. Previous work suggests that these criteria may be met for some fuel pins within the proposed Yucca Mountain Repository. However,experiments that account for the role of U(VI) alteration phases suggest that deliquescence may be a self-limiting process in the sense that deliquescent components (e.g. Cs, Ba, Sr) may be incorporatedinto nondeliquescent U(VI) phases that form from the corrosion of spent fuel.
    Materialart: Online-Ressource
    ISSN: 0272-9172 , 1946-4274
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2004
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 3
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2006
    In:  MRS Proceedings Vol. 985 ( 2006)
    In: MRS Proceedings, Springer Science and Business Media LLC, Vol. 985 ( 2006)
    Kurzfassung: Performance assessment models of the U. S. repository at Yucca Mountain, Nevada suggest that neptunium from spent nuclear fuel is a potentially important dose contributor. A scientific understanding of how the UO 2 matrix of spent nuclear fuel impacts the oxidative dissolution and reductive precipitation of Np is needed to predict the behavior of Np at the fuel surface during aqueous corrosion. Neptunium would most likely be transported as aqueous Np(V) species, but for this to occur it must first be oxidized from the Np(IV) state found within the parent spent nuclear fuel. In this paper we present synchrotron x-ray absorption spectroscopy and microscopy findings that illuminate the resultant local chemistry of neptunium and plutonium within uranium oxide spent nuclear fuel before and after corrosive alteration in an air-saturated aqueous environment. We find the Pu and Np in unaltered spent fuel to have a +4 oxidation state and an environment consistent with solid-solution in the UO 2 matrix. During corrosion in an air-saturated aqueous environment, the uranium matrix is converted to uranyl (UO 2 2+ ) mineral assemblage that is depleted in Np and Pu relative to the parent fuel. The transition from U(IV) in the fuel to a fully U(VI) character across the corrosion front is not sharp, but occurs over a transition zone of ∼ 50 micrometers. We find evidence of a thin (∼ 20 micrometer) layer that is enriched in Pu and Np within a predominantly U(IV) environment on the fuel side of the transition zone. These experimental observations are consistent with available data for the standard reduction potentials for NpO 2 + /Np 4+ and UO 2 2+ /U 4+ couples, which indicate that Np(IV) may not be effectively oxidized to Np(V) at the corrosion potential of uranium dioxide spent nuclear fuel in air-saturated aqueous solutions.
    Materialart: Online-Ressource
    ISSN: 0272-9172 , 1946-4274
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2006
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  • 4
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2019
    In:  npj Materials Degradation Vol. 3, No. 1 ( 2019-08-29)
    In: npj Materials Degradation, Springer Science and Business Media LLC, Vol. 3, No. 1 ( 2019-08-29)
    Kurzfassung: Borosilicate waste glass degradation models must quantify the effects of the solution composition on the dissolution rate. Here, we present results of modified ASTM C1285 tests conducted at 90 °C with AFCI and LRM glasses to determine whether dependencies of dissolution rates on the pH, Al, and Si concentrations must be included. Solution compositions were modified from those generated by glass dissolution alone by adding small amounts of K 4 SiO 4 glass, Al(OH) 3 •2H 2 O, and a concentrated NaOH solution when the tests were initiated. Results show rate laws for the initial and resumption regimes must include pH dependences, but the residual rate can be modeled independent of the pH, Al, and Si concentrations. Triggering the resumption rate probably depends on the pH, Si, and Al concentrations and perhaps other aspects of the glass composition. A waste glass degradation model using is being parameterized using tests with a range of waste glass compositions to quantify these dependencies.
    Materialart: Online-Ressource
    ISSN: 2397-2106
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2019
    ZDB Id: 2925488-7
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 5
    Online-Ressource
    Online-Ressource
    Elsevier BV ; 2003
    In:  Applied Geochemistry Vol. 18, No. 6 ( 2003-6), p. 823-843
    In: Applied Geochemistry, Elsevier BV, Vol. 18, No. 6 ( 2003-6), p. 823-843
    Materialart: Online-Ressource
    ISSN: 0883-2927
    Sprache: Englisch
    Verlag: Elsevier BV
    Publikationsdatum: 2003
    ZDB Id: 1499242-5
    SSG: 13
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 6
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2006
    In:  MRS Proceedings Vol. 985 ( 2006)
    In: MRS Proceedings, Springer Science and Business Media LLC, Vol. 985 ( 2006)
    Kurzfassung: A mineralogical and geochemical study of soils developed from the unmined Coles Hill uranium deposit (Virginia) was undertaken to determine how phosphorous influences the speciation of uranium in an oxidizing soil/saprolite system typical of the eastern US. This paper presents mineralogical and geochemical results that identify and quantify the processes by which uranium has been sequestered in these soils. It was found that uranium is not leached from the saturated soil zone (saprolites) overlying the deposit due to the formation of a sparingly soluble uranyl phosphate mineral of the meta-autunite group. The concentration of uranium in the saprolites is approximately 1000 mg uranium per kg of saprolite. It was also found that a significant amount of uranium was retained in the unsaturated soil zone overlying uranium-rich saprolites. The uranium concentration in the unsaturated soils is approximately 200 mg uranium per kg of soil (20 times higher than uranium concentrations in similar soils adjacent to the deposit). Mineralogical evidence indicates that uranium in this zone is sequestered by a barium-strontium-calcium aluminum phosphate mineral of the crandallite group (gorceixite). This mineral is intimately inter-grown with iron and manganese oxides that also contain uranium. The amount of uranium associated with both the aluminum phosphates (as much as 1.4 weight percent) has been measured by electron microprobe microanalyses and the geochemical conditions under which these minerals formed has been studied using thermodynamic reaction path modeling. The geochemical data and modeling results suggests the meta-autunite group minerals present in the saprolites overlying the deposit are unstable in the unsaturated zone soils overlying the deposit due to a decrease in soil pH (down to a pH of 4.5) at depths less than 5 meters below the surface. Mineralogical observations suggest that, once exposed to the unsaturated environment, the meta-autunite group minerals react to form U(VI)-bearing aluminum phosphates.
    Materialart: Online-Ressource
    ISSN: 0272-9172 , 1946-4274
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2006
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  • 7
    Online-Ressource
    Online-Ressource
    Elsevier BV ; 2006
    In:  Journal of Geochemical Exploration Vol. 91, No. 1-3 ( 2006-10), p. 56-70
    In: Journal of Geochemical Exploration, Elsevier BV, Vol. 91, No. 1-3 ( 2006-10), p. 56-70
    Materialart: Online-Ressource
    ISSN: 0375-6742
    Sprache: Englisch
    Verlag: Elsevier BV
    Publikationsdatum: 2006
    ZDB Id: 1494778-X
    SSG: 13
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 8
    Online-Ressource
    Online-Ressource
    Elsevier BV ; 2015
    In:  Journal of Nuclear Materials Vol. 462 ( 2015-07), p. 135-146
    In: Journal of Nuclear Materials, Elsevier BV, Vol. 462 ( 2015-07), p. 135-146
    Materialart: Online-Ressource
    ISSN: 0022-3115
    RVK:
    Sprache: Englisch
    Verlag: Elsevier BV
    Publikationsdatum: 2015
    ZDB Id: 2001279-2
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 9
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2002
    In:  MRS Proceedings Vol. 757 ( 2002)
    In: MRS Proceedings, Springer Science and Business Media LLC, Vol. 757 ( 2002)
    Kurzfassung: The dissolution behavior and fission-product release from irradiated thoria-urania fuel was studied by immersing fuel samples in J-13 well water at 90°C. The samples are from the Shippingport Light Water Breeder Reactor and consist of binary solid solutions of (U,Th)O 2 with UO 2 contents varying from 2.0 to 5.2 Wt.%. The post-irradiation U isotopic composition of the samples used in our experiments is: 87.3% 233 U, 10.4% 234 U, 1.8% 235 U, and 〈 0.5% 238 U, 236 U, 232 U. Burn up values for the samples range from 22.3 to 40.9 megawatt-days per kg-metal. Our tests were performed on polished disks and on crushed and sieved samples in stainless-steel reaction vessels with air-filled head-space. After 196 days of reaction, samples showed no evidence for corrosion at the micrometer scale. Concentration ranges (μgL -1 ) of key radionuclides in filtered (∼5 nm pore size) leachates were: 0.1 – 15 90 Sr, 0.9 – 7.0 99 Tc, 0.1 – 35.2 137 Cs, 〈 0.2 – 0.8 233 U, 〈 0.1 – 0.7 232 Th. Concentrations of 237 Np, 239 Pu, 240 Pu and 241 Am were all 〈 0.2 μgL -1 . The relatively high concentrations of the fission products 90 Sr and 137 Cs occur early during leaching and decrease for later samplings. Matrix dissolution rates for the irradiated thoria-urania samples range from ∼3x10 -3 to 〈 3×10 -5 mg m -2 day -1 and are at least two orders of magnitude lower than those measured for UO 2 spent fuels under similar experimental conditions.
    Materialart: Online-Ressource
    ISSN: 0272-9172 , 1946-4274
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2002
    Bibliothek Standort Signatur Band/Heft/Jahr Verfügbarkeit
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  • 10
    Online-Ressource
    Online-Ressource
    Springer Science and Business Media LLC ; 2002
    In:  MRS Proceedings Vol. 757 ( 2002)
    In: MRS Proceedings, Springer Science and Business Media LLC, Vol. 757 ( 2002)
    Kurzfassung: The unmined Coles Hill U deposit in the Virginia Piedmont represents a unique natural laboratory for studying the long-term containment of U by phosphate minerals. The primary ore assemblage consists of coffinite and apatite and is hosted in foliated granite. Geochemical and mineralogical studies of the weathered bedrock and soils developed over the primary ore body indicate that U transport is inhibited by the precipitation of meta-autunite group minerals. The lower part of the profile, which consists of ground water saturated saprolite, contains 1400 mg/kg U (in the solid). This concentration is 1.5 times greater than the mean ore grade of the deposit, indicating that the saprolites are enriched in U relative to the underlying primary ore. Uranium within the saprolite is dominantly associated with 10 to 500 μm long, tabular crystals of (Ba, Ca, Sr) meta-autunite. Ground waters from this zone contain less than 14 μg/L dissolved U suggesting that the U(VI) phosphate minerals present are capable of controlling dissolved U concentrations at values lower than the US-EPA maximum contaminant level (30 μg/L). Mineralogical characterization of the unsaturated soil horizons indicate that geochemical conditions in these zones are not conducive to U stabilization by meta-autunite mineralization. In the vadose zone U is primarily associated with Al phosphate (crandallite) and with P adsorbed or coprecipitated with iron oxide mineral coatings. Geochemical gradients suggest that significant amounts of U have been leached from the vadose zone by infiltrating fluids and reprecipitated below the water table, where the activity ratio of dissolved phosphate to carbonate increases. Based on regional weathering rates, the processes responsible for stabilization of U within the Coles Hill system are estimated to have been active for hundreds of thousands of years.
    Materialart: Online-Ressource
    ISSN: 0272-9172 , 1946-4274
    Sprache: Englisch
    Verlag: Springer Science and Business Media LLC
    Publikationsdatum: 2002
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