Evaluation of the long-term behavior of potential plutonium waste forms in a geological repository

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.

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.


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.


2013 ◽  
Vol 1518 ◽  
pp. 73-78 ◽  
Author(s):  
Shirley K. Fong ◽  
Brian L. Metcalfe ◽  
Randall D. Scheele ◽  
Denis M. Strachan

ABSTRACTA calcium phosphate ceramic waste-form has been developed at AWE for the immobilisation of chloride containing wastes arising from the pyrochemical reprocessing of plutonium. In order to determine the long term durability of the waste-form, aging trials have been carried out at PNNL. Ceramics were prepared using Pu-239 and -238, these were characterised by PXRD at regular intervals and Single Pass Flow Through (SPFT) tests after approximately 5 yrs.While XRD indicated some loss of crystallinity in the Pu-238 samples after exposure to 2.8 x 1018 α decays, SPFT tests indicated that accelerated aging had not had a detrimental effect on the durability of Pu-238 samples compared to Pu-239 waste-forms.


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