Development, Application and Validation Of Models for Waste Package Long-Term Performance; Current Trends

1986 ◽  
Vol 84 ◽  
Author(s):  
Lars O. Werme ◽  
Bernd Grambow

AbstractCurrent trends in modelling waste package performance are reviewed mainly from the perspective of the Swedish SKB studies. Examples are given, which illustrate the approaches for modelling different waste forms, i.e. HLW glass and spent nuclear fuel, and candidate canister materials, such as copper and steel. The relative importance of thermodynamics, reaction kinetics and near-field transport are discussed.

1988 ◽  
Vol 127 ◽  
Author(s):  
M. G. Piepho ◽  
P. J. Turner ◽  
P. W. Reimus

ABSTRACTRadiolysis may significantly affect the long-term performance of nuclear waste packages in a geologic repository. Radiolysis of available moisture and air in an unsaturated or saturated environment will create transient species that can significantly change the pH and/or Eh of the available moisture. These changes can influence rates of containment corrosion, waste form dissolution, and radionuclide solubilities and transport.Many of the pertinent radiochemical reactions are not completely understood, and most of the associated rate constants are poorly characterized. To help identify the important radiochemical reactions, rate constants, species, and environmental conditions, an importance theory code, SWATS (Sensitivity With Adjoint Theory-Sparse version)-LOOPCHEM, has been developed for the radiolytic chemical kinetics model in the radiolysis code LOOPCHEM. The LOOPCHEM code calculates the concentrations of various species in a radiolytic field over time. The SWATS-LOOPCHEM code efficiently calculates: 1) the importance (relative to a defined response of interest) of each species concentration over time, 2) the sensitivity of each parameter of interest, and 3) the importance of each equation in the radiolysis model. The calculated results will be used to guide future experimental and modeling work for determining the importance of radiolysis on waste package performance. A demonstration (the importance of selected concentrations and the sensitivities of selected parameters) of the SWATS-LOOPCHEM code is provided for illustrative purposes, and no attempt is made at this time to interpret the results for waste package performance assessment purposes.


1984 ◽  
Vol 44 ◽  
Author(s):  
John K. Bates ◽  
Thomas J. Gerding

AbstractA test method has been developed to measure the release of radionuclides from the waste package under simulated NNWSI repository conditions, and to provide information concerning materials interactions that may occur in the repository. Data from 13 weeks of unsaturated testing are discussed and compared to that from a 13 week analog test. The data indicate that the waste form test is capable of producing consistent, reproducible results that will be useful in evaluating the role of the waste package in the long-term performance of the repository.


1986 ◽  
Vol 84 ◽  
Author(s):  
A. Berusch ◽  
E. Gause

Summary:Each of the projects has made significant progress toward the eventual operation of a repository for the disposal of high-level radioactive wastes in the United States. Although much has been accomplished, much remains to be done. For example, the Site Characterization Plans for BWIP and NNWSI are nearing completion to be followed by initiation of site characterization activities. The Site Characterization Plan for the selected salt site is scheduled for completion later in 1987. Waste package advanced conceptual design studies are currently scheduled to begin at each project before the end of FY 1987. These efforts will lead to selections of concepts to be detailed in the license application design phase. Compliance with the NRC criteria that require long-term waste package performance will be demonstrated by DOE by performing all of the aforementioned activities. In doing so, the DOE will also be assured that its plan for the safe disposal of high-level waste will be satisfactorily implemented.


1992 ◽  
Vol 294 ◽  
Author(s):  
Rodney C. Ewing

ABSTRACTNatural materials may be used to advantage in the evaluation of the long-term performance of nuclear waste forms. Three case studies are presented: (I) radiation effects in ceramic waste forms; (II) corrosion products of U02 under oxic conditions; (III) corrosion rate of nuclear waste glasses. For each case, a natural phase which is structurally and chemically analogous to the waste form is identified and used to evaluate the long-term behavior of a nuclear waste form. Short-term experimental results are compared to the observations made of analogous natural phases. The three case studies illustrate that results may range between providing fundamental data needed for the long-term evaluation of a waste form to only providing qualitative data of limited use. Although in the most rigorous view the long-term behaviour of a phase cannot be predicted, the correspondence between short-term experimental results and observations made of natural phases provides confidence in the “predicted” behavior of the waste form. The strength of this approach rests with the degree to which a mechanistic understanding of the phenomenon is attained.


1983 ◽  
Vol 26 ◽  
Author(s):  
Thomas H. Pigford

ABSTRACTThis study was conducted for the U. S. Department of Energy by the Waste Isolation Systems Panel appointed by the National Academies of Science and Engineering. The panel was charged to review the alternative technologies available for Isolating of radioactive waste in mined geologic repositories, evaluate the performance benefits from these technologles as potential elements of a waste Isolation system, and identify appropriate technical criteria for satisfactory long-term performance of a geologic repository. Conceptual repositories in basalt, granite, salt, and tuff were considered. Site-specific data on geology, hydrology, and geochemical properties were evaluated and used to define parameters for estimating long-term environmental releases, supplemented when necessary by generic properties.The technology for solid waste forms and waste packages was reviewed and evaluated. Borosilicate glass and unreprocessed spent fuel are the waste forms appropriate for further testing and for repository designs. Testing in a simulated repository environment is necessary to develop an adeauate prediction of the long term performance of waste packages in a geologic repository. Back-up research and development on alternative waste forms should be continued. The expected functions of backfill placed between the rock and waste package need clearer definition and validation.The overall criterion to be used by federal agencies in designing a geologic waste-isolation system and in evaluating its nerformance has not yet been specified. As a guideline, the panel selected an average annual dose of 10-4 sieverts to a maximally exposed individual at any future time, if the exposure is from expected events such as the slow dissolution of waste solids in wet-rock repositories and the groundwater transport of dissolved radionuclides to the biosphere. Risks from unexpected events such as human intrusion were not evaluated.Calculations were made of the long-term isolation and environmental releases for conceptual repositories in basalt, granite, salt, and tuff. The major contributors to geologic isolation are the slow dissolution of key radioelements as limited by solubility and by diffusion and convection in groundwater surrounding the waste solids, long water travel times from the waste to the environment, and sorption retardation in the media surrounding the repository. Dilution by surface water can reduce the individual radiation exposures that can result from the small fraction of the waste radioactivity that may ultimately reach the environment. Estimates of environmental releases and individual doses were made both for unreprocessed spent fuel and for reprocessing wastes.Accelerated dissolution of waste exposed to groundwater during the period of repository heating was also considered. Long-term environmental releases of radioactivity from some repositories were calculated to cause doses to maximally exposed individuals that are several orders of magnitude below the Individual dose criterion of 10-4 Sieverts per year. Other conceptual repositories were found to not meet the individual dose criterion, although these repositories could still meet the radioactivity release limits in the standard proposed by the Environmental Protection Agency.The technology for geologic waste disposal has advanced to the state of a preliminary technical plan, suitable for testing, verification, and for pllot-facility confirmation. The waste Isolation program needs a reliable prediction of long-term performance that will serve as a basis for final design, construction, licensing, and waste emplacement.


1988 ◽  
Vol 127 ◽  
Author(s):  
G. R. Lumpkin ◽  
R. C. Ewing

ABSTRACTCubic pyrochlore structure types, A2-mB2O6(O, OH, F) i-n*pH2O, and their derivatives (e.g., monoclinic zirconolite) are important actinide-bearing phases in polyphase, ceramic waste forms (e.g., SYNROC). These waste form phases may typically accumulate alpha-decay doses of 1025 alpha-events/m3 in 1, 000 years or 1026alpha-events/m3 in one million years (i.e., for SYNROC with 20 wt. % HLW). Natural pyrochlores have calculated doses ranging from 1024 to 1027 alpha-events/m3 (= 0.02 to 50 dpa) which have accumulated over ten to a thousand million years. Actinide doping experiments typically reach doses of 1025 alpha-events/m3over periods of several years. Detailed x-ray diffraction analysis of natural samples reveals that the alpha-decay dose at which there is an initial loss of crystallinity (i.e., transition from crystalline to the aperiodic, metamict state as a result of alpha-decay damage) increases as a function of the geologic age of the sample. The increase in the calculated alpha-decay dose which is associated with a specific degree of damage (e.g., loss of x-ray diffraction intensity) is attributed to annealing of isolated alpha-recoil tracks back to the original, crystalline structure. Based on a model of gradual track fading, the alpha-recoil tracks in natural pyrochlores have mean lives on the order of 108 years. In contrast, minerals which remain crystalline (e.g., uraninite, UO2) despite doses of over 1027 alpha-events/m3 have mean alpha-recoil track lives of approximately 104 years. This demonstrates that the microstructure of alpha-decay damaged materials depends not only on the total alpha-event dose, but also on the annealing kinetics of alpha-recoil track fading. Therefore, the prediction of the long-term performance and final state of crystalline phases in ceramic nuclear waste forms requires the determination of alpha-recoil damage annealing as a function of time and temperature.


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