Role of Radionuclide Sorption in High-Level Waste Performance Assessment: Approaches for the Abstraction of Detailed Models

Author(s):  
David R. Turner ◽  
F. Paul Bertetti ◽  
Roberto T. Pabalan
2001 ◽  
Vol 298 (1-2) ◽  
pp. 125-135 ◽  
Author(s):  
Dirk Mallants ◽  
Jan Marivoet ◽  
Xavier Sillen

1988 ◽  
Vol 127 ◽  
Author(s):  
Jan L. Marivoet ◽  
Geert Volckaert ◽  
Arnold A. Bonne

ABSTRACTPerformance assessment studies have been undertaken on the geological disposal of high-level waste in a clay layer in the framework of the CEC project PAGIS. The methodology applied consists of two consecutive steps : a scenario and a consequence analysis. The scenario analysis has indicated that scenarios of normal evolution, of human intrusion, of climatic change, of secondary glaciation effects and of faulting should be evaluated. For the consequence analysis as well deterministic “best estimate” as stochastic calculations, including uncertainty, risk and sensitivity analyses, have been elaborated.The calculations performed show that most radionuclides decay to negligible levels within the first fewjneters of the clay barrier. Just a few radionuclides, 99Tc, 135Cs and 237Np with its daughter nuclides 233U and 229Th can eventually reach the biosphere. The maximum dose rates arising from the geological disposal of HLW, as evaluated by the “best-estimate” approach are about 10−11 Sv/y for river pathways. If the sinking of a water well into the 150 m deep aquifer layer in the vicinity of the repository is considered together with a climatic change, the maximum calculated dose rate rises to a value of 3×10−7 Sv/y. The maximum dose rates evaluated by stochastic calculations are about one order of magnitude higher due to the considerable uncertainties in the model parameters. In the case of the Boom clay the estimated consequences of a fault scenario are of the same order of magnitude as the results obtained for the normal evolution scenario. The maximum risk is estimated from the results obtained through stochastic calculations to be about 5×10−8 per year. The sensitivity analysis has shown that the effective thickness of the clay layer, the retention factors of Tc, Cs and Np, and the Darcy velocity in the aquifer are parameters which strongly influence the calculated dose rates.


1986 ◽  
Vol 84 ◽  
Author(s):  
V. M. Oversby

AbstractPerformance assessment calculations are required for high level waste repositories for a period of 10,000 years under NRC and EPA regulations. In addition, the Siting Guidelines (IOCFR960) require a comparison of sites following site characterization and prior to final site selection to be made over a 100,000 year period. In order to perform the required calculations, a detailed knowledge of the physical and chemical processes that affect waste form performance will be needed for each site. While bounding calculations might be sufficient to show compliance with the requirements of IOCFR60 and 40CFRI91, the site comparison for 100,000 years will need to be based on expected performance under site specific conditions. The only case where detailed knowledge of waste form characteristics in the repository would not be needed would be where radionuclide travel times to the accessible environment can be shown to exceed 100,000 years. This paper will review the factors that affect the release of radionuclides from spemt fuel under repository conditions, summarize our present state of knowledge, and suggest areas where more work is needed in order to support the performance assessment calculations.


Author(s):  
Bernhard Kienzler ◽  
Peter Vejmelka ◽  
Volker Metz

Abstract The amount of mobile radionuclides is controlled by the geochemical isolation potential of the repository. Many investigations are available in order to determine the maximal radionuclide concentrations released from different waste forms of specific disposal strategies for disposal in rock salt formations. These investigations result in reaction (dissolution) rates, maximum concentrations, and sorption coefficients. The experimental data have to be applied to various disposal strategies. The case studies presented in this communication cover the selection, the volumes, and the composition of backfill materials used as sorbents for radionuclides. As an example, for brown coal fly ash (BFA) - Q-brine systems, sorption coefficients were measured as well as solublilities of several actinides and other long-lived radionuclides. Dissolved CO32− was buffered to negligible concentration by the presence of high amount of Mg in solution. In the sorption experiments Pu, Th, Np, and U concentrations close or below detection limit were obtained. Concentrations in the same ranges are computed by means of geochemical modeling, if precipitation of “simple” tetravalent hydroxides (An(OH)4(am) phases) is assumed. In the case of U in a Portland cement dominated geochemical environment, measured U(VI) concentration corresponds to the solubility of hexavalent solids, such as Na2U2O7. A similar behavior of U was observed in high-level waste glass experiments. Experiments investigating sorption behavior of corroded cement showed that in the case of application of a sufficient large inventory of actinides, measured concentrations were found to be independent of the inventory. In this case, measured concentrations were controlled by solid phases. If smaller actinide inventories were applied, resulting concentrations were found to be below concentrations constrained by well-known solids. Here, a more or less pronounced sorption of the radioactive elements was observed. The radionuclide concentrations determined in the BFA “sorption” experiments are found to be close to the detection limits. For this reason, it is not possible to extrapolate the radionuclide behavior to lower concentrations. We cannot distinguish, if sorption or precipitation controls measured radionuclide concentrations. However, in the presence of reducing materials such as BFA, solubilities of tetravalent actinides and of Tc(IV) represent a realistic estimation of the maximal element concentrations needed in performance assessment studies. The concentrations of these redox sensitive elements are controlled by precipitation of An(OH)4(am) phases for disposal concepts considered in German salt formations. Under this assumption, quantities such as solid-solution ratios used in (sorption) experiments do not affect the mobilization of the radionuclides. Additional conclusions can be drawn from comparison of the findings for the redox sensitive elements in the BFA / portland cement brine systems: We can assume that expected actinide and technetium concentrations in the near-field of radioactive wastes are affected by the total inventory of radionuclides in the disposal room. Sorption will be relevant, if the total dissolved radionuclide concentration remains below the maximal solubility defined by the solid radionuclide phase which is stable in the geochemical environment. In contrast to the portland cement system, the relevant radionuclide phase are most probably tetravalent hydroxides in the BFA systems. These conclusions are of high importance to performance assessment for the radioactive waste repository systems, because they restrict the applicability of sorption models in the near field of the waste.


1995 ◽  
Author(s):  
David Berwald ◽  
Anthony Favale ◽  
Timothy Myers ◽  
Jerry McDaniel

1984 ◽  
Vol 44 ◽  
Author(s):  
Bryan J. Travis ◽  
H. E. Nuttall

AbstractRecently, there is increased concern that radiocolloids may act as a rapid transport mechanism for the release of radionuclides from high-level waste repositories. The role of colloids is, however, controversial because the necessary data and assessment methodology have been limited. To quantitatively assess the role of colloids, the TRACR3D transport code has been enhanced by the addition of the population balance equations. The code was tested against the experimental laboratory column data of Avogadro et al. Next a low-level radioactive waste site was investigated to explore whether colloid migration could account for the unusually rapid transport of plutonium and americium observed. The nature and modeling of radiocolloids are discussed along with site simulation results from the TRACR3D code.


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