Congruent and Incongruent Radionuclide Release During Matrix Dissolution of Partly Oxidized High Burnup Spent Fuel

2000 ◽  
Vol 663 ◽  
Author(s):  
A. Loida ◽  
B. Grambow ◽  
H. Geckeis
Keyword(s):  
Dissolution Rate ◽  
Masking Effect ◽  
Dissolution Behavior ◽  
Spent Fuel ◽  
Ph Values ◽  
Fe Powder ◽  
The Matrix ◽  
Order Of Magnitude ◽  
The Impact

ABSTRACTWith respect to the assessment of the long-term behavior of the waste form spent fuel it is of high importance to study in particular the UO2 matrix dissolution behavior and the associated release/retention of radionuclides in contact with groundwater. During long term fuel storage, fuel oxidation may not be avoided. Main issue of this work is to identify the impact on the corrosion of partly oxidized fuel of environmental conditions such as (1) the nature of solution contacting the matrix, the (2) presence/absence of CO2, (3) fixed pH values within a range between pH 7- pH 11, and (4) the presence/absence of corroding container material (Fe-powder). Dissolution tests with powdered oxidized spent fuel in various granite waters, and NaCl-brine resulted in matrix dissolution rates in the same order of magnitude for all investigated media (ca.5×10−4/d). The presence of CO2 and fixed pH values (pH 5 – 11) was without a distinct effect. The independence of the dissolution rate of the oxidized fuel matrix upon the nature of solution, pCO2, fixed pH values (5-11) can probably be explained by a masking effect of radiolysis. In presence of Fe powder the matrix dissolution rate was found to be slowed down by a factor of ca. 20, associated with strong retention effects of radionuclides.

Corrosion Behavior of Pre-oxidized High Burnup Spent Fuel in Salt Brine

2003 ◽  
Vol 807 ◽  
Author(s):  
Andreas Loida ◽  
Bernhard Kienzler ◽  
Horst Geckeis
Keyword(s):  
Dissolution Rate ◽  
Spent Fuel ◽  
Salt Solutions ◽  
Fuel Surface ◽  
Fuel Sample ◽  
Salt Brine ◽  
High Burnup ◽  
Interim Storage ◽  
The Impact

ABSTRACTDuring long-term interim storage of spent fuel, pre-oxidation of the UO2-matrix may not be ruled out completely. This can happen if air could find access to the fuel in the case of cladding failure. The aim of this work is to study the impact of pre-oxidation of the fuel surface on the UO2 matrix dissolution rate and the associated mobilization or retention of radionuclides in highly concentrated salt solutions. The tests were performed with samples that suffered pre-oxidation during up to seven years. The dissolution rate of a fuel sample contacted by small quantities of air-oxygen was found to be roughly a factor of 10 higher in comparison to non oxidized samples, but concentrations of radionuclides, especially Pu and U were hardly affected. The majority of dissolved radionuclides, especially Pu, U appear to have been reimmobilized on the fuel sample itself.

Mobilization/Retention of Radionuclides during Corrosion of High Burnup Spent Fuel and Backfill Materials in Salt Brines

2002 ◽  
Vol 757 ◽  
Author(s):  
Andreas Loida ◽  
Bernhard Kienzler ◽  
Horst Geckeis
Keyword(s):  
Near Field ◽  
Waste Form ◽  
Spent Fuel ◽  
The Matrix ◽  
Backfill Materials ◽  
Salt Brine ◽  
Solid Phases ◽  
Long Term Behavior ◽  
The Impact

ABSTRACTWith respect to the assessment of the long-term behavior of the waste form spent fuel it is of high importance to study the fuel alteration in contact with groundwater and near field materials. The aim of this work is to evaluate the impact of candidate backfill materials hydroxylapatite and magnetite on the overall corrosion behavior of this waste form in salt brine; both materials are used in corrosion tests together with spent fuel. The instant releases and the matrix dissolution rates appear to be similar in presence and in absence of any backfill material under study. However, Am,Np,Pu,U and Sr are retained at different ratios on the hydroxylapatite, on the magnetite and on the fuel sample, indicating possibly the formation of different radionuclide containing new solid phases.

Alteration Behavior of High Burnup Spent Fuel in Salt Brine Under Hydrogen Overpressure and in Presence of Bromide

2006 ◽  
Vol 985 ◽  
Author(s):  
Andreas Loida ◽  
Volker Metz ◽  
Bernhard Kienzler
Keyword(s):  
Dissolution Rate ◽  
Spent Fuel ◽  
Radiolysis Products ◽  
The Matrix ◽  
Matrix Bound ◽  
Salt Brine ◽  
High Burnup ◽  
Geological Formations ◽  
Α Activity

AbstractRecent studies have shown that in the presence of H2 overpressure, which forms due to the corrosion of the Fe based container, the dissolution rate of the spent fuel matrix is slowed down by a factor of about 10, associated with a distinct decrease of concentrations of important ra-dionuclides. However, in a natural salt environment as well as in geological formations with chloride rich groundwater the presence of radiation chemically active impurities such as bro-mide must be taken in consideration. Bromide is known to react with β/γ radiolysis products, thus counteracting the protective H2 effect. In the present experiments using high burnup spent fuel it is observed that during 212 days the matrix dissolution rate was enhanced by a factor of about10 in the presence of up to 10-3 M bromide and 3.2 bar H2 overpressure. However, concen-trations of matrix bound actinides were found at the same level or below as found under identical conditions, but in the absence of bromide. In the long-term it is expected that the effect of bro-mide becomes less important, because the decrease of β/γ-activity results in a decrease of oxida-tive radicals, which react with bromide, while α activity will dominate the radiation field.

Development of the Synthetic Rock Technique for the Immobilization of Iodine: Kinetics of the Alumina Matrix Dissolution under High Alkaline Conditions

2012 ◽  
Vol 1518 ◽  
pp. 79-84 ◽  
Author(s):  
Hideaki Miyakawa ◽  
Tomofumi Sakuragi ◽  
Hitoshi Owada ◽  
Osamu Kato ◽  
Kaoru Masuda
Keyword(s):  
Dissolution Rate ◽  
Rate Constant ◽  
Base Material ◽  
Dissolution Behavior ◽  
Treatment Technique ◽  
Release Behavior ◽  
Alumina Matrix ◽  
Synthetic Rock ◽  
The Matrix ◽  
Iodine Release

ABSTRACTIodine filters expended after nuclear fuel reprocessing contain radioactive iodine (I-129), almost all of which exists as silver iodide (AgI). The synthetic rock technique is a solidification treatment technique using hot isostatic press (HIP), in which the alumina adsorbent base material is synthesized to form a dense solidified material (synthetic rock), and I-129 is physically confined in the form of AgI in the alumina matrix. Thus, it is necessary to understand the matrix dissolution behavior to evaluate the iodine release behavior.Experiments involving the dissolution of the matrix were carried out under various temperatures (35–70 °C) and pH values (10–12.5) that reflect the disposal conditions. The results of the experiments showed that the dissolution rate of Al visibly increases with temperature and pH. The dissolution rate constant was calculated from the initial data assuming the dissolution of the matrix as a primary reaction. The logarithmic rate constant showed a good linear correlation with the pH and the reciprocal of temperature. The 27Al-NMR analysis of the solutions of the dissolved matrix showed that the major chemical species present in the solutions was Al(OH)4-. This indicated that the dissolution of the matrix can be described by the following equation: Al2O3 + 2OH- + 3H2O → 2Al(OH)4-. Subsequently, the empirical equation of the rate of dissolution of the matrix as a function of the temperature and pH was derived. It will be used to evaluate the iodine release behavior from the synthetic rock.

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.

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.

scholarly journals Consumers' Response to State Energy Efficient Appliance Rebate Programs

2017 ◽  
Vol 9 (4) ◽  
pp. 227-255 ◽  
Author(s):  
Sébastien Houde ◽  
Joseph E. Aldy
Keyword(s):  
Energy Efficiency ◽  
Energy Efficient ◽  
Energy Demand ◽  
State Energy ◽  
Government Expenditure ◽  
Order Of Magnitude ◽  
Term Energy ◽  
The Impact

Through an evaluation of the 2009 Recovery Act's State Energy Efficient Appliance Rebate Program, this paper examines consumers' response to energy efficiency rebates. The analysis shows that 70 percent of consumers claiming a rebate were inframarginal and an additional 15 percent–20 percent of consumers simply delayed their purchases by a few weeks. Consumers responded to rebates by upgrading to higher quality, but less energy-efficient models. Overall the impact of the program on long-term energy demand is likely to be small. Measures of government expenditure per unit of energy saved are an order of magnitude higher than estimates for other energy efficiency programs. (JEL D12, H31, H71, Q48)

Effects of pH and Uranium Valence State on the Aqueous Dissolution of Brannerite

2003 ◽  
Vol 807 ◽  
Author(s):  
Y. Zhang ◽  
E. Loi ◽  
M. Blackford ◽  
T. McLeod ◽  
H. Li ◽  
...  
Keyword(s):  
Dissolution Rate ◽  
Valence State ◽  
Ph Dependence ◽  
Aqueous Media ◽  
Matrix Elements ◽  
Atmospheric Conditions ◽  
Ph Values ◽  
Surface Alteration ◽  
Effects Of Ph ◽  
Order Of Magnitude

ABSTRACTThe dissolution of the thorium analogue of brannerite (ThTi2O6-I) and U(IV)/U(V) doped Th-brannerite (Th0.97U0.03Ti2O6-II and Th0.955U0.03Ca0.015Ti2O6-III) in aqueous media under atmospheric conditions has been studied to elucidate the effects of pH and uranium valence state on the dissolution rate.The dissolution of I is nearly stoichiometric but slightly preferential release of U occurs for II and preferential release of Ca and U occur for III. The V-shape pH dependence previously observed for U-brannerite only occurs for U (not other matrix elements) for II, indicating that the pH dependence is related to the U oxidation state upon dissolution. The normalised U dissolution rates of III are nearly an order of magnitude higher than those of II for pH values over 3, suggesting brannerite is less durable with U(V) doping. TEM examination of specimens after leaching revealed few surface alteration products, which is consistent with the nearly stoichiometric dissolution of thorium brannerite.

scholarly journals Large wood as a confounding factor in interpreting the width of spring-fed streams

2020 ◽  
Vol 8 (1) ◽  
pp. 195-210
Author(s):  
Dana Ariel Lapides ◽  
Michael Manga
Keyword(s):  
Unit Length ◽  
Channel Morphology ◽  
Large Wood ◽  
Climate Data ◽  
Stream Channels ◽  
Stream Width ◽  
Order Of Magnitude ◽  
High Resolution Satellite Imagery ◽  
The Impact

Abstract. Spring-fed streams throughout volcanic regions of the western United States exhibit larger widths than runoff-fed streams with similar discharge. Due to the distinctive damped hydrograph of spring-fed streams (as compared to large peaks visible in the hydrographs of runoff-fed streams), large wood is less mobile in spring-fed than runoff-fed stream channels, so wood is more likely to remain in place than form logjams as in runoff-fed streams. The consequent long residence time of wood in spring-fed streams allows wood to potentially have long-term impacts on channel morphology. We used high-resolution satellite imagery in combination with discharge and climate data from published reports and publicly available databases to investigate the relationship between discharge, wood length, and channel width in 38 spring-fed and 20 runoff-fed streams, additionally responding to a call for increased use of remote sensing to study wood dynamics and daylighting previously unpublished data. We identified an order of magnitude more logjams than single logs per unit length present in runoff-fed streams as compared to spring-fed streams. Histograms of log orientation in spring-fed streams additionally confirmed that single logs are immobile in the channel so that the impact of single logs on channel morphology could be pronounced in spring-fed streams. Based on these observed differences, we hypothesized that there should be a difference in channel morphology. A model for stream width in spring-fed streams based solely on length of wood is a better model than one derived from discharge or including both discharge and wood length. This study provides insights into controls on stream width in spring-fed streams.

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