Leaching Behavior and α-Decay Damage Accumulation of UO2 Containing Short-Lived Actinides

2000 ◽  
Vol 663 ◽  
Author(s):  
V.V. Rondinella ◽  
J. Cobos ◽  
Hj. Matzke ◽  
T. Wiss ◽  
P. Carbol ◽  
...  
Keyword(s):  
Redox Potential ◽  
Sample Surface ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Experimental Conditions ◽  
Α Decay ◽  
Level Of Activity ◽  
Congruent Dissolution ◽  
High Concentrations ◽  
Α Activity

ABSTRACTUO2 containing short-lived α-emitters, the so-called α-doped UO2, can simulate type (i.e. α- decay) and level of activity of spent fuel at the time when it might become exposed to groundwater in a geologic repository during storage. This allows studying α-radiolysis effects on the dissolution of the fuel matrix. Additionally, UO2 with high concentrations of α-emitters accumulate, during experimentally acceptable short times, the amount of decays, hence of property modifications, corresponding to long storage times for spent fuel. UO2 containing ∼10 and ∼0.1 wt% 238Pu was fabricated and tested. Leaching experiments in deionized water under unaerated conditions, with continuous monitoring of the evolution of the redox potential and pH in the leaching solutions, were performed. The Eh measurements showed a fast increase of the redox potential in the case of the material with the highest α-activity, while the UO2 containing ∼0.1 wt% 238Pu increased its potential more slowly. The redox potential for undoped UO2 decreased steadily during the experiment. As previously observed, higher fractions of U were released in the case of α-doped UO2 compared to undoped UO2. The fractions of U and Pu released during leaching from the α-doped materials were very similar, suggesting that congruent dissolution occurred. After leaching times longer than 10 h, only dissolved species were present in the solutions. Under these experimental conditions, characterized by relatively low values of the ratio sample surface/leachant volume, a dependence of the released amounts on the α-activity of the samples was observed. Periodical measurements of parameters like hardness, showed a rapid buildup of radiation damage in the material with the high α-activity. After more than two years, noticeable changes, namely an increase of the hardness, have begun to be observed also for the material with the low concentration of 238Pu.

Studies on Spent Fuel Alterations During Storage and Radiolysis Effects on Corrosion Behaviour Using Alpha-Doped UO2

2003 ◽  
Author(s):  
V. V. Rondinella ◽  
T. Wiss ◽  
J.-P. Hiernaut ◽  
J. Cobos
Keyword(s):  
Corrosion Behaviour ◽  
Alpha Decay ◽  
Lattice Parameter ◽  
Dislocation Loops ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Experimental Conditions ◽  
Dose Rate Effects ◽  
Radiolytic Process ◽  
Microstructure Examination

UO2 containing different fractions of short-lived alpha-emitters, the so-called alpha-doped UO2 simulates the level of activity of spent fuel after different storage times, and can be used to study the effects of radiolysis on the corrosion behaviour of aged spent fuel exposed to groundwater in a geologic repository. Furthermore, the integral over time of the alpha-decay in alpha-doped UO2 can simulate the decay damage accumulated in spent fuel during storage. This allows investigating property modifications occurring to the fuel during storage periods of interest (e.g. in view of spent fuel retrieval or in view of final disposal) within a laboratory-acceptable timescale. Periodical measurements of lattice parameter are performed on high activity alpha-doped UO2 to investigate the build-up of radiation damage and evaluate possible dose rate effects. Additionally, annealing tests combined with He-release measurements using a Knudsen cell and with microstructure examination using TEM are performed to establish a correlation among the annealing of damage in the microstructure (mainly characterized by dislocation loops) and the release behaviour of He. The effects on the microstructure due to the accumulation of He and α-decay damage are of interest as they may considerably affect the mechanical integrity of the fuel rods, by causing e.g. swelling or cracking in the fuel and/or overpressurization of the cladding. Alpha-doped UO2 with specific activities spanning over three orders of magnitude and undoped UO2 were used in static leaching experiments at room temperature in deionized water under nominally anoxic conditions. Under these experimental conditions (single effect studies) a clear dissolution enhancing effect of alpha-radiolysis was observed coupled with the establishment of higher redox potential due to the radiolytic process. An alpha-activity dependence of the dissolution behaviour was observed.

Electrochemical Measurements during the Anaerobic Corrosion of Steel

2000 ◽  
Vol 663 ◽  
Author(s):  
N.R. Smart ◽  
P.A.H. Fennell ◽  
R. Peat ◽  
K. Spahiu ◽  
L. Werme
Keyword(s):  
Redox Potential ◽  
Silver Chloride ◽  
Steel Wire ◽  
Reference Electrode ◽  
Glass Electrode ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Steel Electrode ◽  
Anaerobic Corrosion ◽  
Corrosion Of Steel

ABSTRACTIn Sweden, it is proposed that spent fuel should be encapsulated in sealed cylindrical canisters for disposal in a geologic repository. The canisters would consist of a thick ferrous inner container and a copper overpack. If mechanical failure of the copper overpack occurred, allowing water to enter, the ferrous inner container would corrode anaerobically and liberate hydrogen. The rate of hydrogen generation due to the anaerobic corrosion of steel in anoxic groundwater has been measured using barometric cells. The aim of the work presented in this paper was to measure the redox potential, Eh and pH in the presence of anaerobically corroding steel, in a barometric cell. Two specially designed barometric cells were constructed. They were equipped with a silver chloride or calomel reference electrode, a gold Eh electrode, a glass electrode, and a steel electrode. The electrodes were allowed to stabilize in anoxic artificial groundwater and then a mass of pickled steel wire was introduced into the test cell. As the wires were added, the redox potential rapidly became more negative due to the rapid consumption of the residual oxygen. The corrosion potential of the steel was stable and a slow drift in pH was observed. The results are compared with the results of geochemical modelling. Extension of the work to investigate the electrochemical parameters in the presence of dissolved uranium species is discussed.

Testing of Uranium Dioxide Containing Different Levels of Alpha Activity Under Anaerobic and Reducing Conditions

2008 ◽  
Vol 1104 ◽  
Author(s):  
Arvid Ödegaard-Jensen ◽  
Virginia Oversby
Keyword(s):  
Uranium Dioxide ◽  
Alpha Decay ◽  
Sample Surface ◽  
Hydrogen Atmosphere ◽  
Nitrogen Atmosphere ◽  
Alpha Activity ◽  
Dissolution Behavior ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Radiolysis Products

AbstractSweden plans to dispose of spent nuclear reactor fuel in a deep geologic repository in granitic rock. The conditions in the repository in the long term will be reducing and water is not expected to contact the fuel until after more than 1000 years. At that time, most of the beta- and gamma-active nuclides will have decayed away and the radiation will be dominated by alpha decay. In order to simulate the radiolysis field for dissolution of spent fuel with age more than 1000 years we have used uranium dioxide containing 5% U-235 and 0, 5, or 10% U-233. The 10% U-233 gives an alpha activity appropriate to about 3000 years after disposal. Samples were testied in a synthetic groundwater with low ionic strength and with the chemical composition dominated by sodium bicarbonate and calcium chloride. Tests were run in triplicate using an atmosphere of nitrogen (1atm), hydrogen (10 bar), hydrogen (10 bar) plus an iron strip in the solution, nitrogen (1 atm) plus an iron strip in the solution, hydrogen (10 bar) plus an iron strip in the solution, hydrogen (10 bar) without the iron strip. Each of these test conditions was run for 2 consecutive periods of at least 21 days. The results showed that the dissolution behavior of the samples was the same for both nitrogen atmosphere and hydrogen atmosphere. The amount of U dissolved under these conditions clearly showed the enhancement of dissolution due to oxidation of the sample surface by radiolysis products. When an iron strip was added to the solution, the amount of dissolution decreased dramatically indicating that the Fe(II) ions released from the corroding iron were able to react with most of the radiolysis products before they could oxidize the uranium dioxide surface.

scholarly journals Adsorption Studies on Magnetic Nanoparticles Functionalized with Silver to Remove Nitrates from Waters

Water ◽  
2021 ◽  
Vol 13 (13) ◽  
pp. 1757
Author(s):  
Yesica Vicente-Martínez ◽  
Manuel Caravaca ◽  
Antonio Soto-Meca ◽  
Miguel Ángel Martín-Pereira ◽  
María del Carmen García-Onsurbe
Keyword(s):  
Magnetic Nanoparticles ◽  
Nitrate Content ◽  
Adsorption Efficiency ◽  
Experimental Conditions ◽  
Dependent Behavior ◽  
Before And After ◽  
Naoh Solution ◽  
High Concentrations ◽  
Interference Studies

This paper presents a novel procedure for the treatment of contaminated water with high concentrations of nitrates, which are considered as one of the main causes of the eutrophication phenomena. For this purpose, magnetic nanoparticles functionalized with silver (Fe3O4@AgNPs) were synthesized and used as an adsorbent of nitrates. Experimental conditions, including the pH, adsorbent and adsorbate dose, temperature and contact time, were analyzed to obtain the highest adsorption efficiency for different concentration of nitrates in water. A maximum removal efficiency of 100% was reached for 2, 5, 10 and 50 mg/L of nitrate at pH = 5, room temperature, and 50, 100, 250 and 500 µL of Fe3O4@AgNPs, respectively. The characterization of the adsorbent, before and after adsorption, was performed by energy dispersive X-ray spectroscopy, scanning electron microscopy, Brunauer-Emmett-Teller analysis and Fourier-transform infrared spectroscopy. Nitrates can be desorbed, and the adsorbent can be reused using 500 µL of NaOH solution 0.01 M, remaining unchanged for the first three cycles, and exhibiting 90% adsorption efficiency after three regenerations. A deep study on equilibrium isotherms reveals a pH-dependent behavior, characterized by Langmuir and Freundlich models at pH = 5 and pH = 1, respectively. Thermodynamic studies were consistent with physicochemical adsorption for all experiments but showed a change from endothermic to exothermic behavior as the temperature increases. Interference studies of other ions commonly present in water were carried out, enabling this procedure as very selective for nitrate ions. In addition, the method was applied to real samples of seawater, showing its ability to eliminate the total nitrate content in eutrophized waters.

The Effect of Bromide on Oxygen Yields in Homogeneous α-radiolysis

MRS Advances ◽  
2017 ◽  
Vol 2 (13) ◽  
pp. 711-716 ◽  
Author(s):  
Lovisa Bauhn ◽  
Christian Ekberg ◽  
Patrik Fors ◽  
Kastriot Spahiu
Keyword(s):  
Radiation Field ◽  
Spent Nuclear Fuel ◽  
Radiation Doses ◽  
Deep Geological Repository ◽  
Spent Fuel ◽  
Mass Spectrometric Measurement ◽  
Α Decay ◽  
Geological Repository ◽  
Dissolved Ions ◽  
Dissolved Hydrogen

ABSTRACTIn a scenario where ground water enters a canister for spent nuclear fuel in a deep geological repository, the presence of dissolved ions in the water could possibly influence the fuel dissolution due to effects on radiolysis yields. One species of particular interest in this context is bromide, which has a proven ability to scavenge hydroxyl radicals much faster than molecular hydrogen does. As a result, bromide could inhibit the beneficial effect of dissolved hydrogen, which has been shown in γ-radiolysis experiments. However, already a few hundred years after repository closure, α-decay starts to dominate in the radiation field from the spent fuel. Hence, the effects of α-radiolysis are expected to govern the fuel dissolution over the geological timeframes of the repository. In the present work, α-radiolysis experiments have been performed to determine the effect of bromide ions on the yield of hydrogen peroxide by mass spectrometric measurement of its decomposition product oxygen. The use of high activity 238Pu solutions has made it possible to study this effect during pure α-radiolysis from a homogeneously distributed radiation field. To simulate deep bedrock repository conditions, and to minimize the influence of in-leaking O2 from air, the studies were performed using graphite sealed stainless steel autoclaves with an initial atmosphere of 10 bar H2. The results show that addition of 1 mM Br- to the solution gives no significant effect on the O2 yield for radiation doses up to 2 MGy. This lack of effect is most likely explained by the limited radical escape yields from radiation tracks in pure α-radiolysis.

scholarly journals Activation of human platelets by immune complexes prepared with cationized human IgG

Blood ◽  
1993 ◽  
Vol 82 (10) ◽  
pp. 3045-3051
Author(s):  
M Schattner ◽  
M Lazzari ◽  
AS Trevani ◽  
E Malchiodi ◽  
AC Kempfer ◽  
...  
Keyword(s):  
Platelet Aggregation ◽  
Platelet Activation ◽  
Immune Complexes ◽  
Platelet Rich Plasma ◽  
Human Platelets ◽  
Human Igg ◽  
Experimental Conditions ◽  
Induce Platelet Aggregation ◽  
Soluble Immune Complexes ◽  
High Concentrations

The present study shows that the ability of soluble immune complexes (IC), prepared with human IgG and rabbit IgG antibodies against human IgG, to trigger platelet activation was markedly higher for IC prepared with cationized human IgG (catIC) compared with those prepared with untreated human IgG (cIC). CatIC induced platelet aggregation and adenosine triphosphate release in washed platelets (WP), gel-filtered platelets (GFP), or platelet-rich plasma (PRP) at physiologic concentrations of platelets (3 x 10(8)/mL) and at low concentrations of catIC (1 to 30 micrograms/mL). On the contrary, under similar experimental conditions, cIC did not induce aggregation in PRP, WP, or GFP. Low aggregation responses were only observed using high concentrations of both WP (9 x 10(8)/mL) and cIC (500 micrograms/mL). Interestingly, catIC were also able to induce platelet activation under nonaggregating conditions, as evidenced by P-selectin expression. Cationized human IgG alone did not induce platelet aggregation in PRP but triggered either WP or GFP aggregation. However, the concentration needed to induce these responses, was about eightfold higher than those required for catIC. The responses induced either by catIC or cationized human IgG were completely inhibited by treatment with heparin, dextran sulphate, EDTA, prostaglandin E1, or IV3, a monoclonal antibody against the receptor II for the Fc portion of IgG (Fc gamma RII). The data presented in this study suggest that IgG charge constitutes a critical property that conditions the ability of IC to trigger platelet activation.

Chemical Durability of High Burnup Lwr-Spent Fuel in Concentrated Salt Solutions

1993 ◽  
Vol 333 ◽  
Author(s):  
A. Loida ◽  
B. Grambow ◽  
P. Dressier ◽  
K. Friese ◽  
H. Geckeis ◽  
...  
Keyword(s):  
Surface Area ◽  
Volume Ratio ◽  
Sample Surface ◽  
Solution Concentration ◽  
Reaction Rates ◽  
Spent Fuel ◽  
Intrinsic Dissolution ◽  
Fine Grained ◽  
High Burnup ◽  
Saturation Effects

ABSTRACTHigh-burnup (<50 MWd/kgU) spent fuel samples of various sizes were exposed to NaCl solutions under static, anaerobic and reducing conditions. The accumulated corrosion time was about 200 days. Gas phase and leach solutions were analyzed. By dissolving mm sized fragments in large volumes of solution, saturation effects were avoided and upper limits for intrinsic dissolution rates of about 5-20 mg/(m2d) were measured. Surface area normalized reaction rates were significantly lower when using fine grained fuel powder (estimated sample surface area to solution volume ratio S/V ca. 3000 m-1), indicating saturation effects. The maximum concentrations of Pu and Am in the tests are close to reported solubility limited concentrations in pure 5m NaCl solutions in the absence of radiolysis effects. The presence of iron effectively reduces the solution concentration of all measured radionuclides (except Cs).

Nonadrenergic bronchodilation induced by high concentrations of sulfur dioxide

1990 ◽  
Vol 69 (5) ◽  
pp. 1786-1791
Author(s):  
D. C. Thompson ◽  
J. L. Szarek ◽  
R. J. Altiere ◽  
L. Diamond
Keyword(s):  
Muscle Tone ◽  
Blocking Agent ◽  
Lung Compliance ◽  
Environmental Pollutant ◽  
Inhibitory System ◽  
Experimental Conditions ◽  
Bronchodilator Response ◽  
Cellular Source ◽  
High Concentrations ◽  
Dynamic Lung Compliance

SO2 is an environmental pollutant known to elicit bronchospasm in susceptible subjects. We observed that brief exposure of artificially bronchoconstricted cats to high concentrations of SO2 induces a bronchodilator response. This study assessed the characteristics of this response and examined various mechanisms that might underlie it. Cats were anesthetized with diallylbarbital-urethan, and airway smooth muscle tone, measured by lung resistance and dynamic lung compliance, was elevated with a continuous infusion of 5-hydroxytryptamine. Administration of 10 breaths of SO2 via a tracheostomy induced concentration-dependent bronchodilation in the range 100-1,000 parts/million. Only infrequently was bronchoconstriction observed before bronchodilation. SO2-induced bronchodilator responses were unaffected by pretreatment with intravenous atropine or propranolol, establishing them as nonadrenergic noncholinergic (NANC) in origin. Neither the ganglionic blocking agent hexamethonium nor the nerve toxin tetrodotoxin influenced the SO2-induced bronchodilation, thus excluding a role for central or local autonomic reflexes in the response. Efforts to modulate the response by pretreatment with the cyclooxygenase inhibitor indomethacin or the mediator release inhibitor cromolyn sodium also were unsuccessful. Administration of acidic aerosols failed to mimic the SO2-induced bronchodilator response. Although the mechanism whereby SO2 induces bronchodilation under these experimental conditions remains unclear, release of a NANC inhibitory transmitter from a neural, epithelial, or other cellular source via a mechanism insensitive to both tetrodotoxin and cromolyn is a distinct possibility. An intrinsic NANC inhibitory system may exist in feline airways functioning as a local regulator of bronchomotor tone and possibly serving to override responses to strong, potentially asphyxial bronchoconstrictive stimuli.

scholarly journals Methane-induced haemolysis of human erythrocytes

1995 ◽  
Vol 307 (2) ◽  
pp. 433-438 ◽  
Author(s):  
H Batliwala ◽  
T Somasundaram ◽  
E E Uzgiris ◽  
L Makowski
Keyword(s):  
Diffusion Rate ◽  
Human Erythrocytes ◽  
Experimental Conditions ◽  
Detergent Concentration ◽  
Partial Pressures ◽  
Temperature Diffusion ◽  
Wide Range ◽  
Gas Molecules ◽  
High Concentrations ◽  
Cell Leakage

Human erythrocytes were exposed to high concentrations of methane and nitrogen through the application of elevated partial pressures of these gas molecules. Cell leakage (haemolysis) was measured for cells exposed to these gases under a wide range of experimental conditions. Application of methane produces haemolysis at pressures far below the hydrostatic pressures known to disrupt membrane or protein structure. The effects of changes in buffer, temperature, diffusion rate and detergents were studied. Methane acts co-operatively with detergents to produce haemolysis at much lower detergent concentration than is required in the absence of methane or in the presence of nitrogen. At sufficiently high concentrations of methane, all cells are haemolysed. Increased temperature enhances the effect. Methane produces 50% haemolysis at a concentration of about 0.33 M compared with about 7.5 M methanol required for the same degree of haemolysis.

Phase Relations of the Uranyl Oxide Hydrates and their Relevance to the Disposal of Spent Fuel

1990 ◽  
Vol 212 ◽  
Author(s):  
R. J. Finch ◽  
R. C. Ewing
Keyword(s):  
General Formula ◽  
Phase Relations ◽  
Molecular Water ◽  
Spent Fuel ◽  
Geologic Repository ◽  
Structural Sheet ◽  
Natural Analogues ◽  
Ph Conditions ◽  
Image Position

ABSTRACTUranyl oxide hydrates, formed by the alteration of uraninite, are natural analogues for the long-term corrosion products of spent fuel in a geologic repository under oxidizing conditions. The uranyl oxide hydrates may be represented by the general formula:Pb-bearing hydrates require the addition of a neutral uranyl group into the structural sheet (UO2(OH)2) for each interlayer Pb ion. Distortion of the structure associated with the additional uranyl groups is reduced by replacing two structural hydroxyls with a structural oxygen and a molecular water. The general formula for the Pb-uranyl oxide hydrates is:This hypothesis explains the paragenetic sequences:1) schoepite ➛ billietite ➛ protasite ➛ bauranoite2) schoepite ➛ vandendriesscheite ➛ fourmarierite ➛ masuyite ➛ wölsendorfite3) schoepite ➛ vandendriesscheite ➛ fourmarierite ➛ ± masuyite ➛ sayrite ➛ curite, and indicates that, under relatively high pH conditions, schoepite will not be the long-term solubility-controlling phase for uranium in uranium-rich groundwaters.

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