Structure and alteration kinetics of rare-earth rich borosilicate glasses with (64 – 2x) SiO2 / 18 B2O3 / 18 Na2O / x RE2O3 composition (RE = Y or Eu+ La)

2010 ◽  
Vol 1265 ◽  
Author(s):  
Odile Majerus ◽  
Daniel Caurant ◽  
Ning Li ◽  
Jean-Baptiste Baudouin ◽  
Gabriela Manolescu ◽  
...  

AbstractThe high level nuclear waste load is likely to increase in the future containment glasses, rising new questions about their long-term chemical durability. In this study sodium borosilicate compositions with Si substituted for RE (RE = rare earth) are altered under static conditions at fixed pH (8.5). The Na and B leached fractions reached just after the rate drop increase with the RE2O3 content. Part of the RE ions remain in the altered layer which is significantly de-polymerised (IR-ATR and NMR results). Their environment is reorganized and adopts a more centrosymetrical character. The higher leached fractions are attributed to rapid hydrolysis of Si/B-O-RE bonds with respect to Si-O-Si bonds.

Author(s):  
Kenneth R. Trethewey

It is well known that some metals suffer damage caused by the evolution of hydrogen in certain conditions in nuclear applications. Of particular current interest is the use of alloys for use in containers for the long-term storage of high level nuclear waste. Calculations for the rates of corrosion of metals where hydrogen evolution is possible rely upon measurements of the reaction kinetics, but it is difficult to obtain reliable and accurate values for the kinetic constants. Standard electrochemical tests can be used, but the analysis of the results is complex because of the need to deconvolute the curves. This paper presents a computer model for the analysis of the data that is checked by its use on experimental data from a number of nuclear materials.


2003 ◽  
Vol 807 ◽  
Author(s):  
Adam Duddridge ◽  
Moinul Islam ◽  
Diane Holland ◽  
Charlie R. Scales

ABSTRACTA mixed-alkali modified borosilicate base glass used in the vitrification of high-level nuclear waste (HLW) has been doped with a number of waste simulants to between 2 and 12 mol%. The simulants have been chosen to give two distinct series of glasses: one consisting of trivalent ions having the form M2O3(where M is La, Bi, Al or Fe) and the other consisting of divalent simulants of the form MO (where M is Pb, Zn or Ba). An international standard Soxhlet leach test procedure was performed on each glass to study the effect of prolonged, moderate-temperature, dynamic water corrosion. Results of these studies show that, except for BaO, as the amount of simulant is increased, the amount of Na and Li leached decreases showing them to become more chemically resistant. These corrosion tests have been correlated to ionic (D.C.) conductivity measurements, which show a decrease in the conductivity of the glass as the amount of waste simulant is increased, and 11B magic-angle spinning nuclear magnetic resonance (MAS-NMR) studies, which have shown that, as more waste-simulant is loaded into the glasses the rate of conversion of [BO4] to [BO3] units increases. All of the data from these studies reflect the different network forming abilities of the divalent and trivalent cations.


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.


2002 ◽  
Vol 757 ◽  
Author(s):  
Maureen Alai ◽  
Susan Carroll

ABSTRACTWe are investigating the evaporation of pore water representative of the designated high-level-nuclear-waste repository at Yucca Mountain, NV to predict the range of brine compositions that may contact waste containers. These brines could form potentially corrosive thin films on the containers and impact their long-term integrity. Here we report the geochemistry of a relatively complex synthetic Topopah Spring Tuff pore water that was progressively evaporated in a series of experiments. The experiments were conducted in a vented vessel in which HEPA filtered air flowed over the 95°C solution. Samples of the evaporating solution and the condensed vapor were taken and analyzed to determine the evolving water chemistry and gas volatility. The final solid was analyzed by X-ray diffraction.The synthetic Topopah Spring Tuff water evolved towards a complex brine that contained about 45 mol % Cl, 7 mol% NO3, 43 mol% Na, 4 mol % K, and less than 1 mol % each of SO4, Ca, Mg, HCO3 and Si. Trends in the solution data and identification of CaSO4 solids suggest that fluorite, carbonate, sulfate, and Mg-silicate precipitation minimize the corrosion potential of “sulfate type pore water” by removing F, Ca, and Mg during the early stages of evaporation.


1988 ◽  
Vol 127 ◽  
Author(s):  
I. L. Pegg ◽  
E. E. Saad ◽  
X. Feng ◽  
R. B. Adiga ◽  
W. P. Freeborn ◽  
...  

ABSTRACTProperty models have been developed for the major properties that need to be controlled in the production of borosilicate glasses for West Valley high-level nuclear waste immobilization. The chemical durability is the most important parameter for product performance, while melt viscosity is the most critical parameter in assuring the processability of the glass. Simple models for these properties are described that are based on data from numerous glasses which were prepared with compositions in the region around the West Valley reference glass. A scheme for optimization of the target glass and for predicting the acceptability of glasses resulting from natural process variations is illustrated. This involves integration of the product models with a process model that was described previously. This approach has guided the present placement of the West Valley reference glass.


Author(s):  
Jerzy Narbutt

<p>Recycling of actinides from spent nuclear fuel by their selective separation followed by transmutation in fast reactors will optimize the use of natural uranium resources and minimize the long-term hazard from high-level nuclear waste. This paper describes solvent extraction processes recently developed, aimed at the separation of americium from lanthanide fission products as well as from curium present in the waste. Depicted are novel poly-N-heterocyclic ligands used as selective extractants of actinide ions from nitric acid solutions or as actinide-selective hydrophilic stripping agents.</p>


2019 ◽  
Vol 9 (12) ◽  
pp. 2437 ◽  
Author(s):  
Sebastian Wegel ◽  
Victoria Czempinski ◽  
Pao-Yu Oei ◽  
Ben Wealer

The nuclear industry in the United States of America has accumulated about 70,000 metric tons of high-level nuclear waste over the past decades; at present, this waste is temporarily stored close to the nuclear power plants. The industry and the Department of Energy are now facing two related challenges: (i) will a permanent geological repository, e.g., Yucca Mountain, become available in the future, and if yes, when?; (ii) should the high-level waste be transported to interim storage facilities in the meantime, which may be safer and more cost economic? This paper presents a mathematical transportation model that evaluates the economic challenges and costs associated with different scenarios regarding the opening of a long-term geological repository. The model results suggest that any further delay in opening a long-term storage increases cost and consolidated interim storage facilities should be built now. We show that Yucca Mountain’s capacity is insufficient and additional storage is necessary. A sensitivity analysis for the reprocessing of high-level waste finds this uneconomic in all cases. This paper thus emphasizes the urgency of dealing with the high-level nuclear waste and informs the debate between the nuclear industry and policymakers on the basis of objective data and quantitative analysis.


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