Measurement of Soluble Nuclide Dissolution Rates from Spent Fuel

1989 ◽  
Vol 176 ◽  
Author(s):  
C. N. Wilson ◽  
W. J. Gray
Keyword(s):  
Yucca Mountain ◽  
Water Soluble ◽  
Spent Fuel ◽  
Release Rates ◽  
Dissolution Rates ◽  
Advantages And Disadvantages ◽  
Water Composition ◽  
The Matrix ◽  
Flow Through

ABSTRACTGaining a better understanding of the potential release behavior of water-soluble radionuclides is the focus of new laboratory spent fuel dissolution studies being planned in support of the Yucca Mountain Project. Previous studies have suggested that maximum release rates for actinide nuclides, which account for most of the long-term radioactivity in spent fuel, should be solubility-limited and should not depend on the characteristics or durability of the spent fuel waste form. Maximum actinide concentrations should be sufficiently low to meet the NRC annual release limits. Potential release rates for soluble nuclides such as 99Tc, 135Cs, 14C and 129I, which account for about 1-2% of the activity in spent fuel at 1000 years, are less certain and may depend on processes such as oxidation of the fuel in the repository air environment.Dissolution rates for several soluble nuclides have been measured from spent fuel specimens using static and semi-static methods. However, such tests do not provide a direct measurement of fuel matrix dissolution rates that may ultimately control soluble-nuclide release rates. Flow-through tests are being developed as a potential supplemental method for determining the matrix component of soluble-nuclide dissolution. Advantages and disadvantages of both semi-static and flow-through methods are discussed. Tests with fuel specimens representing a range of potential fuel states that may occur in the repository, including oxidized fuel, are proposed. Preliminary results from flow-through tests with unirradiated UO2 suggesting that matrix dissolution rates are very sensitive to water composition are also presented.

Spent Fuel Corrosion Behavior in Salt Solution in the Presence of Hydrogen Overpressure

2001 ◽  
Author(s):  
Andreas Loida ◽  
Bernd Grambow ◽  
Horst Geckeis
Keyword(s):  
Gas Phase ◽  
Spent Fuel ◽  
Nacl Solution ◽  
Release Rates ◽  
Corrosion Rates ◽  
The Matrix ◽  
Matrix Bound ◽  
Safety Assessments ◽  
Container Material

Abstract The simultaneous corrosion of spent fuel and Fe-based container material is characterized by the formation of large amounts of hydrogen, which control the composition of the gas phase. Various experimental data indicate that the matrix dissolution rate and the release rates of important radionuclides decrease, if the H2 overpressure increases. To quantify to what extent the hydrogen overpressure may counteract radiolysis enhanced matrix dissolution rates, and to take credit from the effect of hydrogen overpressure in long-term safety assessments of the repository, a detailed experimental investigation has been initiated. High burnup spent fuel is being corroded under anoxic conditions in the absence of carbonate in 5m NaCl solution under an external H2 overpressure of 3.3 bar. This pressure is in the same range as observed in a long-term test using spent fuel and Fe-powder. Results obtained after 117 days of testing show that due to constant or decreasing concentrations of Sr and other matrix bound radionuclides, corrosion rates were not measurable indicating a stop of matrix dissolution or very low long-term rates. Grain boundary release of Cs and fission gases was found to continue under hydrogen overpressure. Compared to tests in the absence of hydrogen solution concentrations decreased by about ca. 1.5 orders of magnitude for U (10−8 M), Am, Eu (10−10 M), whereas the decrease of Np (3×10−10 M), Tc (5×10−9 M) and Pu (4×10−9 M) concentrations was found to be less significant.

The Effect of Nearfield Constraints on the Corrosion Behavior of High Burnup Spent Fuel

2006 ◽  
Vol 932 ◽  
Author(s):  
Andreas Loida ◽  
Manfred Kelm ◽  
Bernhard Kienzler ◽  
Horst Geckeis ◽  
Andreas Bauer
Keyword(s):  
Host Rock ◽  
Near Field ◽  
Experimental Studies ◽  
Spent Fuel ◽  
Mutual Support ◽  
Significant Extent ◽  
Dissolution Rates ◽  
The Matrix ◽  
Container Material

ABSTRACTThe long-term immobilization for individual radioelements released from the waste form “spent fuel” in solid phases upon groundwater contact depends strongly on the (geo)chemical constraints prevailing in the repository. Related experimental studies comprise effects induced by the presence of Fe based container material, and near field materials other than Fe for a rock salt environment. The effect of the presence of an argillaceous host rock containing organic matter and pyrite on fuel alteration was studied in addition. The results have shown that oxidative radio-lysis products were found to be consumed at a significant extent by the metallic Fe and by the argillaceous host rock. Under these conditions a decrease at a factor of ca.100 for both the matrix dissolution rates and the solution concentrations of U and Pu was found. There is mutual support between the matrix dissolution rates, the solution concentrations and the amounts of oxygen encountered during the experiments under various conditions controlled by the presence of near field materials under study.

Constraints by Experimental Data for Modeling of Radionuclide Release from Spent Fuel

1989 ◽  
Vol 176 ◽  
Author(s):  
Bernd Grambow ◽  
L.O. Werme ◽  
R.S. Forsyth ◽  
J. Bruno
Keyword(s):  
Experimental Data ◽  
Product Layer ◽  
Spent Fuel ◽  
Upper Limits ◽  
The Matrix ◽  
The Usa ◽  
Oxidant Production ◽  
Release Data ◽  
Radionuclide Release

ABSTRACTComparison of spent fuel corrosion data from nuclear waste management projects in Canada, Sweden and the USA strongly suggests that the release of 90Sr to the leachant can be used as a measure of the degradation (oxidation/dissolution) of the fuel matrix. A surprisingly quantitative similarity in the 90 Sr release data for fuel of various types (BWR, PWR, Candu), linear power ratings and burnups leached under oxic conditions was observed in the comparison. After 1000 days of leachant contact, static or sequential, the fractional release rates for 90Sr (and for cesium nuclides) were of the order of 10−7/d.The rate of spent fuel degradation (alteration) under oxic conditions can be considered to be controlled either by the growth rates of secondary alteration products, by oxygen diffusion through a product layer, by the rate of formation of radiolytic oxidants or by solubility-controlled dissolution of the matrix. These processes are discussed. Methods for determining upper limits for long-term 90Sr release, and hence fuel degradation, have been derived from the experimental data and consideration of radiolytic oxidant production.

On the Role of H2 as an Inhibitor of UO2 Matrix Dissolution

2007 ◽  
Author(s):  
Juan Merino ◽  
Xavier Gaona ◽  
Lara Duro ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza
Keyword(s):  
Chemical Composition ◽  
Partial Pressure ◽  
Water Radiolysis ◽  
Water Interface ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Term Stability ◽  
Long Term Stability

The study of spent fuel behaviour under disposal conditions is usually based on conservative approaches assuming oxidising conditions produced by water radiolysis at the fuel/water interface. However, the presence of H2 from container corrosion can inhibit the dissolution of the UO2 matrix and enhance its long-term stability. Several studies have confirmed the decrease in dissolution rates when H2 is present in the system, although the exact mechanisms of interaction have not been fully established. This paper deals with a radiolytic modelling exercise to explore the consequences of the interaction of H2 with radicals generated by radiolysis in the homogeneous phase. The main conclusion is that in all the modelled cases the presence of H2 in the system leads to a decrease in matrix dissolution. The extent of the inhibition, and the threshold partial pressure for the inhibition to take place, both depend in a complex way on the chemical composition of the water and the type of radiation present in the system.

Histopathological effects of crude oil on Atlantic cod following chronic exposure

1984 ◽  
Vol 62 (10) ◽  
pp. 2038-2043 ◽  
Author(s):  
R. A. Khan ◽  
J. Kiceniuk
Keyword(s):  
Gadus Morhua ◽  
Atlantic Cod ◽  
Giant Cells ◽  
Water Soluble ◽  
Similar Concentration ◽  
Long Term Effect ◽  
Flow Through ◽  
Kidney Lesions ◽  
Histopathological Effects

To assess the long-term effect on the tissues of marine fish, Atlantic cod, Gadus morhua L., were exposed to water-soluble fractions of Venezuelan and Hibernia crude oils at concentrations of 50–300 ppb for 12–13 weeks in a flow-through seawater system. Histopathological changes in oil-exposed fish included increased numbers of mucus-producing epithelial cells, capillary dilation, lamellar hyperplasia, and fusion of adjacent filaments in gills, microvesicular formation in hepatocytes, delayed spermatogenesis with intratubular multinucleated giant cells, and an increase of melanomacrophage centers in the spleen and kidney. Lesions were more prevalent and severe in fish exposed to Hibernia crude than to Venezuelan crude at a similar concentration.

A Comparison and Abstraction of the Commercial Spent Fuel Corrosion Experiments in the U.S.

2002 ◽  
Vol 757 ◽  
Author(s):  
Eric R. Siegmann
Keyword(s):  
Corrosion Rate ◽  
Spent Fuel ◽  
Release Rates ◽  
Water Contact ◽  
Contact Mode ◽  
Corrosion Rates ◽  
Single Temperature ◽  
Flow Through ◽  
Distribution Sensitivity ◽  
Temperature Dependent Model

ABSTRACTThis paper compares the results of three different fuel corrosion experiments by taking the existing corrosion data reported for various temperatures and recalculating corrosion rates at a single temperature of 25°C using a temperature dependent model developed elsewhere. Three types of light water reactor fuel corrosion tests (sometimes called dissolution or alteration tests) were performed in support of Yucca Mountain Project. The tests used three water contact modes and various fuel burnups. All measurements were adjusted for temperature differences and then compared. Five different isotopes (cesium, technetium, iodine, strontium, and, in the flow-through tests, uranium) were considered as a measure of corrosion. The data used represent over ten years of experiments with about nine different fuel types. Most experiments were with repository type fluids, containing dissolved constituents such as carbonate, calcium and silicon. The results show that all of the experiments predict similar fuel corrosion rates. Small differences in the isotope release rates are observed and incorporated in the abstracted uncertainty. Water contact mode (flow-through, batch, or drip) does not seem to be very important although the drip tests introduced larger variations. In developing a corrosion abstraction, all of the isotope measurements were considered equally. The distribution of release rates was used directly to develop the uncertainty. The mean corrosion rate was 1.8 × 10-4 fraction/year at 25°C (5%-95% range = 5.7 × 10-5 to 1.7 × 10-3). Using the derived corrosion rate for 25°C, and considering rapid axial splitting of the cladding, the CSNF fuel rod is expected to corrode in less than 2,000 years. The abstraction uses all the available experiments performed with water containing carbonates, silicon, or calcium and irradiated fuel to produce a corrosion rate distribution. Sensitivity studies using this corrosion rate abstraction in the TSPA-SR analysis show very small changes in dose (3%) in response to changes in the UO2 corrosion abstraction.

Static dissolution tests of α-doped UO2 under repository relevant conditions: Influence of Boom Clay and α-activity on fuel dissolution rates

2006 ◽  
Vol 932 ◽  
Author(s):  
Sonia Salah ◽  
Christelle Cachoir ◽  
Karel Lemmens ◽  
Norbert Maes
Keyword(s):  
Clay Fraction ◽  
Dissolution Kinetics ◽  
Spent Fuel ◽  
Dissolution Rates ◽  
Retention Capacity ◽  
Boom Clay ◽  
Dissolution Tests ◽  
Clay Formation ◽  
Α Activity

ABSTRACTSince reprocessing is no longer the reference policy in Belgium, studies on the direct disposal of spent fuel in a clay formation have gained increased interest in the last years. In order to determine to what extent the clay properties and the α-activity influence the dissolution kinetics of spent fuel for the long term disposal, static dissolution tests have been performed on 5 different types of α-doped UO2, representing a PWR fuel with a burn-up of 45 or 55 GWd · tHM−1 and fuel ages ranging between 150 and 90,000 years, in different Boom Clay (BC) media at room temperature and in an anoxic atmosphere for 90 to 720 days. The uranium activity in the clay fraction over time was found to be much higher than the U-activity in the leachates, which has been mainly ascribed to the high retention capacity of the BC. The average dissolution rate between 0 and 90 days obtained for the 5 types of α-doped UO2 were all found to be high and quite similar at ~263 µg · m−2 · d−1and a “longer-term” rate (181 to 720 days) ranging between zero and 15 µg · m−2· d−1. These results suggest that the activity of the fuels does not seem to have an effect on the UO2 dissolution rates under the considered test conditions. In order to study the partition/redistribution of U during UO2dissolution, sequential extraction experiments were performed. Results of the latter have provided a better mechanistic understanding of BC/spent fuel interaction processes as well as information on the role of the different minerals controlling the U-retention/immobilization.

UO2 dissolution in high pH conditions of the Belgian Supercontainer

2012 ◽  
Vol 1475 ◽  
Author(s):  
Th. Mennecart ◽  
C. Cachoir ◽  
K. Lemmens
Keyword(s):  
Spent Fuel ◽  
Dissolution Rates ◽  
High Ph ◽  
Neutral Ph ◽  
Dissolution Tests ◽  
Alkaline Conditions ◽  
Ph Conditions ◽  
Ph Range ◽  
Long Term Behavior

ABSTRACTTo assess the long-term behavior of spent fuel in alkaline conditions representative for the Belgian Supercontainer design, static and dynamic dissolution tests were performed with depleted and Pu-doped UO2 , simulating medium burn-up UOX fuels of different fuel ages. The experiments were performed under argon atmosphere at 25 – 30°C in cement waters in the pH range 11.7 – 13.5 and at different SA/V ratios. This paper presents the observed UO2 matrix dissolution rates based on the (238U or 233U) release, and proposes a selection of reference dissolution rates for performance assessment. We demonstrate that the dissolution rates at high pH are equivalent to the dissolution rates reported in the literature for neutral pH conditions. The α-activity threshold below which radiolytical fuel oxidation becomes negligible, seems to be close to the threshold reported for anoxic media at neutral pH.

Measures of Geologic Isolation

2004 ◽  
Vol 824 ◽  
Author(s):  
William M. Murphy
Keyword(s):  
Scientific Basis ◽  
Yucca Mountain ◽  
Radiation Doses ◽  
Spent Fuel ◽  
Carbon 14 ◽  
Decay Series ◽  
Regulatory Measures ◽  
Geologic Setting ◽  
High Level

AbstractIsolation in a geologic setting has been the generally favored solution to the high-level radioactive waste (HLW) problem since a scientific basis for nuclear waste management began to be formulated over half a century ago. Although general features of suitable settings have been enumerated, quantitative measures of the safety of geologic isolation of HLW are challenging to devise and to implement. Some regulatory measures of isolation for the proposed repository at Yucca Mountain, Nevada, have be devised and revised involving considerations of global releases, groundwater travel time, and time and space scales for isolation. In current Yucca Mountain specific regulations, the measure of long-term safety hinges on probabilistic estimates of radiation doses to the average member of a maximally exposed group of people living about 18 km down the groundwater flow gradient within 10,000 years after permanent closure of the repository. From another perspective, hydrogeochemical studies provide quantitative measures of system openness and the ability of geologic systems to isolate HLW. Hydrogeochemical data that bear on geologic isolation of HLW at Yucca Mountain include precipitation of radionuclides in stable mineralogical products of spent fuel alteration, ages of natural secondary mineralization in the mountain, uranium decay-series isotopic data for system openness, bomb-pulse isotope occurrences, and ambient carbon-14 distributions.

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