Use of Archaeological Glass to Predict the Long-Term Behavior of HLW

2009 ◽  
Vol 1193 ◽  
Author(s):  
S. Gin ◽  
A. Verney-Carron ◽  
G. Libourel

AbstractThe predictability of models describing long-term nuclear glass behavior in a geological repository can be tested by means of natural or archaeological analogs. This study covers fractured archaeological glass blocks from a shipwreck discovered near the Mediterranean island of Embiez (France). The blocks were examined mainly because of their morphological analogy with nuclear glasses. Fractured after production (as in the case of nuclear glass), these blocks had been leached for 1800 years in seawater. The laboratory investigation led to the development and subsequent validation on archaeological objects of a geochemical model capable of accurately simulating the coupling between chemistry and transport to account for the alteration state of the cracks according to their geometric characteristics. Laboratory experiments allowed us to determine the kinetic and thermodynamic parameters for modeling glass alteration. The model was then tested against short-term experiments before simulating the crack alteration over 1800 years. We show that cracks in the outer regions of the block are the most severely altered because of rapid solution renewal, whereas internal cracks are very slightly altered because of a rate-limiting effect of water transport due to the formation of secondary phases. This study also establishes a direct link between data obtained at lab scale and the long-term evolution of a complex system in a natural environment, indicating that the key phenomena have been identified experimentally. The analogous behavior of archaeological and nuclear glass during leaching experiments and the similarities in their crack networks allow us to consider applying the model to nuclear glasses under geological repository conditions. This study clearly shows that the internal crack network does not play a major role in the overall long-term alteration of archeological glass blocks. The issue of the transposition studies will be to determine whether this conclusion can be generalized to nuclear glasses.

2014 ◽  
Vol 1665 ◽  
pp. 23-30 ◽  
Author(s):  
Guido Deissmann ◽  
Stefan Neumeier ◽  
Felix Brandt ◽  
Giuseppe Modolo ◽  
Dirk Bosbach

ABSTRACTVarious candidate waste matrices such as nuclear waste glasses, ceramic waste forms and low-specification “storage” MOX have been considered within the current UK geological disposal program for the immobilization of separated civilian plutonium, in the case this material is declared as waste. A review and evaluation of the long-term performance of potential plutonium waste forms in a deep geological repository showed that (i) the current knowledge base on the behavior and durability of plutonium waste forms under post-closure conditions is relatively limited compared to HLW-glasses from reprocessing and spent nuclear fuels, and (ii) the relevant processes and factors that govern plutonium waste form corrosion, radionuclide release and total systems behavior in the repository environment are not yet fully understood in detail on a molecular level. Bounding values for the corrosion rates of potential plutonium waste forms under repository conditions were derived from available experimental data and analogue evidence, taking into account that the current UK disposal program is in a generic stage, i.e. no preferred host rock type or disposal concept has yet been selected. The derived expected corrosion rates for potential plutonium waste forms under conditions relevant for a UK geological disposal facility are in the range of 10-4 to 10-2 g m-2 d-1 and 10-5 to 10-4 g m-2 d-1 for borosilicate glasses, and generic ceramic waste forms, respectively, and ∼5·10-6 g m-2 d-1 for storage MOX. More realistic assessments of the long-term behavior of the waste forms under post-closure conditions would require additional systematic studies regarding the corrosion and leaching behavior under more realistic post-closure conditions, to explore the safety margins of the various potential waste forms and to build confidence in long-term safety assessments for geological disposal.


Author(s):  
E. C. Buck ◽  
N. L. Dietz ◽  
J. K. Bates

When waste glass reacts with water, secondary phases may form, which will effect the distribution of radionuclides formally contained within the glass. In order to determine the long term behavior of waste glass, the secondary phases formed need to be identified. Analytical electron microscopy (AEM) is being used to characterize the secondary phases. Glasses have been reacted in test vessels at different surface areas to leachate volumes (S/V) and for periods in excess of 700 days. Increasing the S/V permits one to accelerate the reaction. Samples of the reacted waste forms are embedded in epoxy and thin sectioned by ultramicrotomy for observation in the transmission electron microscopy (TEM). Examinations were performed in a JEOL 2000FXII TEM operated at 200 kV. This abstract describes two types of glass tests, a high level waste sludge based glass and a low level waste glassy slag. Many hundreds of glass tests have been performed and examined by TEM to determine layer thickness, morphology of the leach layer, and identification of secondary phases.


2004 ◽  
Vol 824 ◽  
Author(s):  
S. Gin ◽  
N. Godon ◽  
I. Ribet ◽  
P. Jollivet ◽  
Y. Minet ◽  
...  

AbstractThis article reviews current knowledge of the long-term behavior of R7T7-type glass during the thermal phase and in geological repository conditions (aqueous alteration). In interim storage R7T7 glass can be considered to conserve its integrity over time. In geological repository conditions, the mechanisms of glass alteration by water have been identified and parameter values have been assigned to the reaction kinetics for wide variations of the influential factors (temperature, pH, flow rate, S/V ratio, etc.). CEA has developed an operational model to obtain robust and reasonably conservative predictions of the glass quantities altered after disposal. Examples of applications of the operational model are discussed, future research topics are also proposed to consolidate this approach.


2004 ◽  
Vol 824 ◽  
Author(s):  
Huifang X ◽  
Maozhong Min ◽  
Jia Zhen ◽  
Xinjian Peng ◽  
Jinping Wang ◽  
...  

AbstractFurniture contaminated with uranium will be disposed of, together with U-bearing waste, in ageological repository such as the WIPP site in New Mexico. It is important to understand the effect of the wooden furniture on the migration of uranium in order to predict long-term behavior of uranium in a geological repository environment. In this paper, we present natural uraninite-bearing carbonized wood pieces from a sandstone-hosted roll-type uranium ore deposit in NW China. Results from SEM and TEM observations show that there are nanometer sized, and micron-sized, uraninite crystals that have accumulated on cell walls of the carbonized wood. Some uranitite crystrals display oval and round shapes that may be the result of microbial-induced reduction of uranium from groundwater. The wood carbonized fragments are the most uranium-rich “phase.” In some areas, aggregates of pyrite crystals occur withthe uraninite. It is proposed that organic components from the decay of the wood cells provide nutrientsfor the anaerobic bacteria to grow. The wood pieces with the bacteria inside may serve as scavengers of uranium because of the local reducing chemical environment.


2017 ◽  
Vol 105 (11) ◽  
Author(s):  
Stephane Gin ◽  
Patrick Jollivet ◽  
Magaly Tribet ◽  
Sylvain Peuget ◽  
Sophie Schuller

AbstractRadioactive waste vitrification has been carried out industrially in several countries for nearly 40 years. Research into the formulation and long term behavior of high and intermediate level waste glasses, mainly borosilicate compositions, is still continuing in order to (i) safely condition new types of wastes and (ii) design and demonstrate the safety of the disposal of these long-lived waste forms in a deep geological repository. This article presents a summary of current knowledge on the formulation, irradiation resistance and the chemical durability of these conditioning materials, with a special focus on the fate of radionuclides during glass processing and aging. It is shown that, apart from the situation for certain elements with very low incorporation rate in glass matrices, vitrification in borosilicate glass can enable waste loadings of up to ~20 wt% while maintaining the glass homogeneity for geological time scales and guaranteeing a high stability level in spite of irradiation and water contact.


2021 ◽  
Vol 1756 ◽  
pp. 147334
Author(s):  
Charles Budaszewski Pinto ◽  
Natividade de Sá Couto-Pereira ◽  
Felipe Kawa Odorcyk ◽  
Kamila Cagliari Zenki ◽  
Carla Dalmaz ◽  
...  

Soil Systems ◽  
2020 ◽  
Vol 5 (1) ◽  
pp. 3
Author(s):  
David Singer ◽  
Elizabeth Herndon ◽  
Laura Zemanek ◽  
Kortney Cole ◽  
Tyler Sanda ◽  
...  

Coal mine spoil is widespread in US coal mining regions, and the potential long-term leaching of toxic metal(loid)s is a significant and underappreciated issue. This study aimed to determine the flux of contaminants from historic mine coal spoil at a field site located in Appalachian Ohio (USA) and link pore water composition and solid-phase composition to the weathering reaction stages within the soils. The overall mineralogical and microbial community composition indicates that despite very different soil formation pathways, soils developing on historic coal mine spoil and an undisturbed soil are currently dominated by similar mineral weathering reactions. Both soils contained pyrite coated with clays and secondary oxide minerals. However, mine spoil soil contained abundant residual coal, with abundant Fe- and Mn- (oxy)hydroxides. These secondary phases likely control and mitigate trace metal (Cu, Ni, and Zn) transport from the soils. While Mn was highly mobile in Mn-enriched soils, Fe and Al mobility may be more controlled by dissolved organic carbon dynamics than mineral abundance. There is also likely an underappreciated risk of Mn transport from coal mine spoil, and that mine spoil soils could become a major source of metals if local biogeochemical conditions change.


1997 ◽  
Vol 07 (11) ◽  
pp. 2487-2499 ◽  
Author(s):  
Rabbijah Guder ◽  
Edwin Kreuzer

In order to predict the long term behavior of nonlinear dynamical systems the generalized cell mapping is an efficient and powerful method for numerical analysis. For this reason it is of interest to know under what circumstances dynamical quantities of the generalized cell mapping (like persistent groups, stationary densities, …) reflect the dynamics of the system (attractors, invariant measures, …). In this article we develop such connections between the generalized cell mapping theory and the theory of nonlinear dynamical systems. We prove that the generalized cell mapping is a discretization of the Frobenius–Perron operator. By applying the results obtained for the Frobenius–Perron operator to the generalized cell mapping we outline for some classes of transformations that the stationary densities of the generalized cell mapping converges to an invariant measure of the system. Furthermore, we discuss what kind of measures and attractors can be approximated by this method.


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