a case study

Computer simulations have become increasingly popular in many different areas over the years, owing mainly to more effective and cheaper machines. In many cases, the trend seems to be that computer simulations are replacing experiments, at least in areas in which experiments are very difficult (expensive) or impossible. One such area is that of attempting to foresee what will happen in the future. Such analyses are very important for a durable construction such as a repository for spent nuclear fuel, for example. In the modelling effort, several computer codes are used and input data are often used without scrutiny. However, this work shows that even the rather simple task of calculating the solubility of a solid phase in a given water is encumbered with the effects of different uncertainties. These uncertainties may make the calculated solubility vary by several orders of magnitude. Thus the input to the more complex codes, simulating processes in connection with the repository, will also be affected. This report presents some computer programs for uncertainty and sensitivity analysis of solubility calculations. They are then illustrated by numerical simulations and estimation of uncertainty intervals for a case at the Äspö site in Sweden. Some of the input data treated as uncertain parameters are the stability constants for the reactions between the metal ion concerned and the elements present in the selected water or the rock. Stability constants and the enthalpies and entropies of reaction for the thoriumwater-acetylacetone-phosphate system have been determined experimentally. In addition to the values determined for these entities, uncertainty intervals are also estimated. A complexing mechanism for the thorium-phosphates at pH 8 is also suggested.researc

Potential tellurium deposits in the BWR containment during a severe nuclear accident

The release of fission products to the environment is one of the concerns with nuclear power. During an accident, the most likely released are the volatile fission products i.e., tellurium. To evaluate the behavior of tellurium in the event of an accident, it was heated under different conditions (oxidizing, inert, reducing; both dry and humidified). The formed vapor was transported to surfaces (aluminum, copper, zinc) at room temperature that can be found in the BWR-containment. All formed deposits were examined for morphology and species. Moreover, the content of sodium hydroxide liquid traps following the metal surfaces and filter was also investigated. In these traps, the highest amount of tellurium was found under humid-reducing followed by humid-oxidizing conditions. In the deposit removed from the zinc surface acquired under the latter conditions, elemental analysis observed zinc, indicating a possible reaction between tellurium and zinc. The corresponding trap showed significant amounts of zinc. (C) 2020 The Author(s). Published by Elsevier Ltd

Optimization of Indium Recovery and Separation from LCD Waste by Solvent Extraction with Bis(2-ethylhexyl) Phosphate (D2EHPA)

Indium tin oxide (ITO) is currently the choice of electrode material in liquid crystal displays (LCDs). D2EHPA is known to be an extractant that can be used to selectively recover indium from 1 M sulfuric acid. In order to optimize the extraction and separation of indium from LCD waste, the effects of pH, temperature, time, and extractant concentration on the distribution ratios of In(III) and the major impurities such as Al(III), Cu(II), Fe(III), and Zn(II) were investigated. Metal concentrations in the aqueous feed were based on the concentrations found in the leach liquor of LCD panel glass at 0.1 g/mL S/L ratio. This study showed that extraction of indium could be increased at <293 K and stripping of indium could be increased at >293 K. Furthermore, by increasing D2EHPA concentration from 0.1 M to 0.25 M, extraction of indium could be increased from 70% to >95%

Alpha dose rate calculations for UO2 based materials using stopping power models

Accurate dose rate models for UO2 based materials in contact with water are important in the modeling of the radiolytically promoted dissolution of spent fuel. Dose rates of α-doped UO2 and un-irradiated MOX fuel were modelled using the ASTAR and SRIM stopping power databases. Dose rates were calculated as a function of distance from the active surface. Comparisons with common dose rate calculation models and the combined Bethe-Bloch and Lindhard–Scharff (LS) equation were performed. It was shown that the ASTAR and SRIM databases could more accurately simulate an α-spectrum compared to the Bethe-Bloch-LS equation. A comparison between the continuous slowing down approximation (CSDA) and the radial projection algorithm in the SRIM program was performed, and it was shown that CSDA overestimates the range of the α-particles by a few percent. This leads to an overestimation of the α-dose rate at distances close to the maximum range of the α-particle in water. A relationship between the average dose rate to specific α-activity ratio as a function of α-energy was obtained from the calculations, which can easily be implemented in alpha dose rate calculations of a UO2 based materials

The aqueous chemistry of radium

Available literature data on the aqueous chemistry of radium are compiled. There are limited available experimental data and a significant portion of the data has been estimated using electrostatic techniques, typically based on the corresponding data of barium. The available data are compared with the corresponding data of barium (and strontium) and a methodology for estimating additional radium thermochemical data is described

Radiolytic degradation of dimethyl telluride in aqueous solutions

The formation of volatile radioactive species is a major concern in severe nuclear reactor accident scenarios. Release of radioactive material to the environment is highly governed by the volatility of the species and therefore it its crucial to understand the behavior of any such species during the accident and the days and weeks following. One of the volatile, yet highly understudied fission products is tellurium. Although tellurium has been released in significant amounts during the major nuclear accidents that have occurred, the knowledge of the behavior is still lacking. Here we present results on the radiolysis of dimethyl telluride, a highly volatile species shown to form in accident conditions. The behavior of dimethyl telluride was investigated under gamma irradiation in various aqueous solutions and conditions representative to severe nuclear reactor accident conditions. The results suggest that dimethyl telluride is relatively stable towards gamma irradiation and its degradation is highly affected by the amount of dissolved oxygen and competing species. It was found that dimethyl telluride degrades via oxidative processes by reacting with oxidizing radiolysis products e.g. •OH, O.-. In the absence of oxygen, several volatile telluride dimers were observed. The results presented here increase the interest in organic tellurides in severe accident conditions and highlight the need for further investigation of the re-volatilization and mitigation of volatile tellurium species

Determining Stability Constants Using the AKUFVE Technique

The AKUFVE techniques were developed by Rydberg and co-workers in the 1960s. The main aim was to be able to perform a series of liquid-liquid extraction data varying one or more parameters and at the same time achieve very pure phases. As such, this technique was later used for short-lived isotope studies in the SISAK system, but also as a standalone unit for a large number of thermodynamic studies of extraction systems both for fundamental understanding as well as more applied investigations. In this paper, the apparatus with modifications made over the decades is described. In addition, studies with stability constant determinations for the zirconium-water-acetylacetone system as well as lanthanide extraction using bromodecanoic acid are exemplified to demonstrate the potential use of the technique. The results shown clearly demonstrate the versatility and ability of the AKUFVE system

Organic Telluride Formation from Paint Solvents Under Gamma Irradiation

The interactions between tellurium and organic material during a nuclear reactor accident are critical to source term estimations because of the possible formation of volatile species. Reactions taking place in the containment sump are of interest since these can lead to re-volatilization and increase the fission product source term. This paper presents results from experiments investigating the interaction of tellurium dioxide with three paint solvents-texanol ester, methyl isobutyl ketone, and toluene-under containment sump conditions. The experiments were performed by irradiating a mixed solution of tellurium dioxide and paint solvents at a dose rate of 4 kGy/h up to 300 kGy. The resulting samples were analyzed for tellurium concentration and speciation. Tellurium(IV) was found to reduce to metallic tellurium under irradiation when paint solvents were present. More importantly, several volatile organic tellurides were identified in the irradiated samples, which suggests that tellurium can form volatile species in sump conditions when in contact with dissolved paint solvents. This paper provides novel evidence of organic telluride formation in the sump and raises further interest in tellurium chemistry during a severe nuclear reactor accident