scholarly journals Laser Photoacoustic Spectroscopy for Trace Level Detection of Actinides in Groundwater

1986 ◽  
Vol 84 ◽  
Author(s):  
Mark M. Doxtader ◽  
Victor A. Maroni ◽  
James V. Beitz ◽  
Michael Heaven

The Basalt Waste Isolation Project (Rockwell Hanford Operations- BWIP) is investigating the feasibility of building a repository in the Columbia River Basalts for the permanent disposal of high-level nuclear waste. One aspect of this effort is to develop an understanding of the chemical behavior of radionuclides in the near-field environment of the waste container. Such information is needed to determine radionuclide release rates from the waste package and to make long-term projections of repository performance. To accomplish this task, ultrasensitive laser- based techniques, such as laser photoacoustic spectroscopy (LPAS) and laser induced fluorescence (LIF), are being developed as analytical methods for the trace-level detection and speciation of actinides in solutions typical of those encountered in groundwaters near the BWIP repository.

Author(s):  
Lara Duro ◽  
Alba Valls ◽  
Olga Riba ◽  
Jordi Bruno ◽  
Aurora Marti´nez-Esparza

The application of probabilistic approaches to the performance of underground repositories for long-lived radioactive waste has received special attention in the last years. Numerous exercises have been developed in order to elicit the Probability Distribution Functions (PDFs) of the several parameters needed for these developments. Several integrated models allow the implementation of PDFs in the long-term simulations needed for Performance Assessment. In this work we present how the deterministic compartmental model for a repository of high level nuclear waste (HLNW) located in a crystalline host-rock has been modified to include PDFs for some of the parameters. The implementation of probabilistic approaches gives also information on the most influencing parameter on the migration of the different radionuclides from a deep repository concept.


2012 ◽  
Vol 76 (8) ◽  
pp. 2911-2918 ◽  
Author(s):  
G. Deissmann ◽  
S. Neumeier ◽  
G. Modolo ◽  
D. Bosbach

AbstractSeparated stocks of UK civil plutonium are currently held as a zero value asset in storage, as there is no final decision about whether they should be treated as a resource for future use as nuclear fuel or as waste. Irrespective of future UK government strategies regarding plutonium, at least a portion of the UK civil plutonium inventory will be designated for geological disposal. In this context, we performed a high-level review of the performance of potential wasteforms for the disposal of separated civil plutonium. The key issues considered were the durability and chemical reactivity of the wasteforms in aqueous environments and the long-term radionuclide release under conditions relevant to geological disposal. The major findings of the review, relevant not only to the situation in the UK but to plutonium disposal in general, are summarized in this paper. The review showed that, in the event of a decision being taken to declare plutonium as a waste for disposal, more systematic studies would be required to constrain the wasteform performance under repository conditions in order to derive realistic source terms for a safety case.


1994 ◽  
Vol 353 ◽  
Author(s):  
Narasi Sridhar ◽  
Darrell Dunn ◽  
Gustavo Cragnolino

AbstractLocalized corrosion in aqueous environments forms an important bounding condition for the performance assessment of high-level waste (HLW) container materials. A predictive methodology using repassivation potential is examined in this paper. It is shown, based on long-term (continuing for over 11 months) testing of alloy 825, that repassivation potential of deep pits or crevices is a conservative and robust parameter for the prediction of localized corrosion. In contrast, initiation potentials measured by short-term tests are non-conservative and highly sensitive to several surface and environmental factors. Corrosion data from various field tests and plant equipment performance are analyzed in terms of the applicability of repassivation potential. The applicability of repassivation potential for predicting the occurrence of stress corrosion cracking (SCC) and intergranular corrosion in chloride containing environments is also examined.


1993 ◽  
Vol 333 ◽  
Author(s):  
John C. Walton ◽  
Narasi Sridhar ◽  
Gustavo Cragnolino ◽  
Tony Torng ◽  
Prasad Nair

ABSTRACTOne of the requirements for the performance of waste packages prescribed in 10CFR 60.113 is that the high level waste must be “substantially completely” contained for a minimum period of 300 to 1000 years. During this period, the radiation and thermal conditions in the engineered barrier system and the near-field environment are dominated by fission product decay. In the present U.S design of the engineered barrier system, the outer container plays a dominant role in maintaining radionuclide containment. A quantitative methodology for analyzing the performance of the container is described in this paper. This methodology enables prediction of the evolution of the waste package environment in terms of temperature fields, stability of liquid water on the container surface, and concentration of aggressive ions such as chloride. The initiation and propagation of localized corrosion is determined by the corrosion potential of the container material and critical potentials for localized corrosion. The coiTOsion potential is estimated from the kinetics of the anodic and cathodic reactions including oxygen diffusion through scale layers formed on the container surface. The methodology described is applicable to a wide range of metals, alloys and environmental conditions.


1982 ◽  
Vol 15 ◽  
Author(s):  
T. M. Ahn ◽  
B. S. Lee ◽  
J. Woodward ◽  
R. L. Sabatini ◽  
P. Soo

ABSTRACTThe corrosion behavior of TiCode-12 (Ti-0.3 Mo-0.8 Ni) high level nuclear waste container alloy has been studied for a simulated WIPP brine at a temperature of 150°C or below. Crevice corrosion was identified as a potentially important failure mode for this material. Within a mechanical crevice, a thick oxide film was found and shown to be the rutile form of TiO2, with a trace of lower oxide also present. Acidic conditions were found to cause a breakdown of the passive oxide layer. Solution aeration and increased acidity accelerate the corrosion rate. In hydrogen embrittlement studies, it was found that hydrogen causes a significant decrease in the apparent stress intensity level in fracture mechanics samples. Hydride formation is thought to be responsible for crack initiation. Stress corrosion cracking under static loads was not observed. Attention has also been given to methods for extrapolating short term uniform corrosion rate data to extended times.


2004 ◽  
Vol 824 ◽  
Author(s):  
Mark Sutton ◽  
Maureen Alai ◽  
Susan Carroll

AbstractThe evaporation of a range of synthetic pore water solutions representative of the potential high-level-nuclear-waste repository at Yucca Mountain, NV is being investigated. The motivation of this work is to understand and predict the range of brine compositions that may contact the wastecontainers from evaporation of pore waters, because these brines could form corrosive thin films on the containers and impact their long-term integrity. A relatively complex synthetic Topopah Spring Tuff pore water was progressively concentrated by evaporation in a closed vessel, heated to 95°C in a series of sequential experiments. Periodic samples of the evaporating solution were taken to determine the evolving water chemistry. According to chemical divide theory at 25°C and 95°C our starting solution should evolve towards a high pH carbonate brine. Results at 95°C show that this solution evolves towardsa complex brinethat contains about 99 mol% Na+for the cations, and 71 mol% Cl-, 18 mol% ΣCO2(aq), 9 mol% SO42- for the anions. Initial modeling ofthe evaporating solution indicates precipitation of aragonite, halite, silica, sulfate and fluoride phases. The experiments have been used to benchmark the use of the EQ3/6 geochemical code in predicting the evolution of carbonate-rich brines during evaporation.


1990 ◽  
Vol 212 ◽  
Author(s):  
D. E. Grandstaff ◽  
V. J. Grassi ◽  
A. C. Lee ◽  
G. C. Ulmer

ABSTRACTSystematic differences in pH, cation/proton ion activity ratios, and redox have been observed between solutions produced in rock-water hydrothermal experiments with tuff, granite, and basalt. Stable pH values in tuff-water experiments may be as much as 1.5 pH units more acidic than basalt-water experiments at the same temperature and ionic strength. Redox (log fO2) values in 300°C tuff experiments are 4–7 orders of magnitude more oxidizing than basalt experiments and ca. 4 log units more oxidizing than the magnetite-hematite buffer. Such fluid differences could significantly affect the performance of a high-level nuclear waste repository and should be considered in repository design and siting.


1990 ◽  
Vol 212 ◽  
Author(s):  
N. Sridhar ◽  
G. Cragnolino ◽  
W. Machowski

ABSTRACTThe effect of environmental variables on the localized corrosion behavior of alloy 825 is examined in this paper. Cyclic, potentiodynamic polarization tests based on a two-level, full factorial experimental design were conducted. An index incorporating both the visual and scanning electron microscope examinations of localized corrosion and the electrochemical parameters was used for the statistical analysis. The analysis showed that chloride is the single most important promoter of localized corrosion, while nitrate was the single most important inhibitor. Fluoride was a weak inhibitor, especially at low chloride levels. Sulfate was a weak promoter, especially at high chloride levels. Temperature did not have a significant effect within the chloride levels examined. Separate experiments indicated that silicon, added as metasilicate, did not have any significant effect on localized corrosion. The adverse effect of chloride was observed at concentrations as low as 100 ppm. Addition of H2O2 increased the corrosion potential of alloy 825 to a value above the repassivation potential observed in the 300 ppm chloride solution.


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