Modelling Radionuclide Speciation and Solubility Limits in The Near-Field of a Deep Repository

1985 ◽  
Vol 50 ◽  
Author(s):  
Hans Wanner
Keyword(s):  
Near Field ◽  
Cast Steel ◽  
Significant Rise ◽  
High Level Waste ◽  
Glass Waste ◽  
Carbonate Concentration ◽  
Realistic Description ◽  
Carbonate Complexation ◽  
Main Components ◽  
High Level

AbstractIn the safety analysis recently reported for a potential Swiss high-level waste repository, radionuclide speciation and solubility limits are calculated for expected granitic groundwater conditions. With the objective of deriving a more realistic description of radionuclide release from the near-field, an investigation has been initiated to quantitatively specify the chemistry of the near-field. In the Swiss case, the main components of the near-field are the glass waste-matrix, a thick cast steel canister horizontally stored in a drift, and a backfill of highly compacted bentonite.Based on available experimental data, an ion-exchange model for sodium, potassium, magnesium, and calcium has been developed, in order to simulate the reaction of sodium bentonite backfill with groundwater. The model assumes equilibrium with calcite as long as sufficient carbonates remain in the bentonite, as well as quartz saturation. The application of this model to the reference groundwater used in ‘Project Gewaehr 85’ results in a significant rise in pH (by up to 3 units) as well as a marked increase in the carbonate concentration.Neptunium and plutonium speciation and solubility limits are calculated for the reference groundwater chemistry gradually altered to that of saturated bentonite water and back again by a water exchange cycle model. The solubility limits estimated in this way generally turn out to be higher for the bentonite water than for the reference groundwater, mainly due to carbonate complexation of the actinide components AnO2+ and AnO22+. Uncertainties are particularly large for neptunium solubility due to its strong Eh dependence in bentonite water.

scholarly journals High Level Waste (HLW) Vitrification Experience in the US: Application of Glass Product/Process Control to Other HLW and Hazardous Wastes

2008 ◽  
Vol 1107 ◽  
Author(s):  
Carol M. Jantzen ◽  
James C. Marra
Keyword(s):  
Process Control ◽  
High Level Waste ◽  
Glass Product ◽  
Mechanistic Models ◽  
Glass Waste ◽  
Statistical Process ◽  
Feed Composition ◽  
Feed Forward ◽  
Bonding Structure ◽  
High Level

AbstractVitrification is currently the most widely used technology for the treatment of high level radioactive wastes (HLW) throughout the world. At the Savannah River Site (SRS) actual HLW tank waste has successfully been processed to stringent product and process constraints without any rework into a stable borosilicate glass waste since 1996. A unique “feed forward” statistical process control (SPC) has been used rather than statistical quality control (SQC). In SPC, the feed composition to the melter is controlled prior to vitrification. In SQC, the glass product is sampled after it is vitrified. Individual glass property models form the basis for the “feed forward” SPC. The property models transform constraints on the melt and glass properties into constraints on the feed composition. The property models are mechanistic and depend on glass bonding/structure, thermodynamics, quasicrystalline melt species, and/or electron transfers. The mechanistic models have been validated over composition regions well outside of the regions for which they were developed because they are mechanistic. Mechanistic models allow accurate extension to radioactive and hazardous waste melts well outside the composition boundaries for which they were developed.

scholarly journals Reactive transport calculations to evaluate sulphide fluxes in the near-field of a SF/HLW repository

2019 ◽  
Vol 98 ◽  
pp. 10005
Author(s):  
Marek Pękala ◽  
Paul Wersin ◽  
Veerle Cloet ◽  
Nikitas Diomidis
Keyword(s):  
Reactive Transport ◽  
Spent Nuclear Fuel ◽  
Near Field ◽  
Opalinus Clay ◽  
High Level Waste ◽  
Waste Containment ◽  
Geological Repository ◽  
High Level ◽  
Reducing Bacteria ◽  
Hlw Repository

Radioactive waste is planned to be disposed in a deep geological repository in the Opalinus Clay (OPA) rock formation in Switzerland. Cu coating of the steel disposal canister is considered as potential a measure to ensure complete waste containment of spent nuclear fuel (SF) and vitrified high-level waste (HLW) or a period of 100,000 years. Sulphide is a potential corroding agent to Cu under reducing redox conditions. Background dissolved sulphide concentrations in pristine OPA are low, likely controlled by equilibrium with pyrite. At such concentrations, sulphide-assisted corrosion of Cu would be negligible. However, the possibility exists that sulphate reducing bacteria (SRB) might thrive at discrete locations of the repository’s near-field. The activity of SRB might then lead to significantly higher dissolved sulphide concentrations. The objective of this work is to employ reactive transport calculations to evaluate sulphide fluxes in the near-field of the SF/HLW repository in the OPA. Cu canister corrosion due to sulphide fluxes is also simplistically evaluated.

Assessment of Redox Conditions in the Near Field of Nuclear Waste Repositories: Application to the Swiss high-level and intermediate level waste disposal concept

2003 ◽  
Vol 807 ◽  
Author(s):  
Paul Wersin ◽  
Lawrence H. Johnson ◽  
Bernhard Schwyn
Keyword(s):  
Solid Phase ◽  
Near Field ◽  
Intermediate Level ◽  
Redox Conditions ◽  
High Level Waste ◽  
Redox Potentials ◽  
Spent Fuel ◽  
Reducing Conditions ◽  
High Level ◽  
Waste Repositories

ABSTRACTRedox conditions were assessed for a spent fuel and high-level waste (SF/HLW) and an intermediate-level waste (ILW) repository. For both cases our analysis indicates permanently reducing conditions after a relatively short oxic period. The canister-bentonite near field in the HLW case displays a high redox buffering capacity because of expected high activity of dissolved and surface-bound Fe(II). This is contrary to the cementitious near field in the ILW case where concentrations of dissolved reduced species are low and redox reactions occur primarily via solid phase transformation processes.For the bentonite-canister near field, redox potentials of about -100 to -300 mV (SHE) are estimated, which is supported by recent kinetic data on U, Tc and Se interaction with reduced iron systems. For the cementitious near field, redox potentials of about -200 to -800 mV are estimated, which reflects the large uncertainties related to this alkaline environment.

Near Field Radionuclide Concentrations: Sorption or Solubility Constrained?

2001 ◽  
Author(s):  
Bernhard Kienzler ◽  
Peter Vejmelka ◽  
Volker Metz
Keyword(s):  
Portland Cement ◽  
Performance Assessment ◽  
Geochemical Modeling ◽  
Coal Fly Ash ◽  
Near Field ◽  
High Level Waste ◽  
Sorption Behavior ◽  
Geochemical Environment ◽  
Backfill Materials ◽  
High Level

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.

Wipp Waste Package Testing on Simulated DHLW: Emplacement

1984 ◽  
Vol 44 ◽  
Author(s):  
Martin A. Molecke
Keyword(s):  
Thermal Loading ◽  
Accelerated Aging ◽  
Waste Form ◽  
Future Application ◽  
High Level Waste ◽  
Glass Waste ◽  
Waste Package ◽  
High Level ◽  
Artificial Introduction ◽  
Materials Behavior

AbstractSeveral series of simulated (nonradioactive) defense high-level waste (DHLW) package tests have recently been emplaced in the WIPP, a research and development facility authorized to demonstrate the safe disposal of defense-related wastes. The primary purpose of these 3-to-7 year duration tests is to evaluate the in situ materials performance of waste package barriers (canisters, overpacks, backfills, and nonradioactive DHLW glass waste form) for possible future application to a licensed waste repository in salt. This paper describes all test materials, instrumentation, and emplacement and testing techniques, and discusses progress of the various tests.These tests are intended to provide information on materials behavior (i.e., corrosion, metallurgical and geochemical alterations, waste form durability, surface interactions, etc.), as well as comparison between several waste package designs, fabrications details, and actual costs.These experiments involve 18 full-size simulated DHLW packages (approximately 3.0 m x 0.6 m diameter) emplaced in vertical boreholes in the salt drift floor. Six of the test packages contain internal electrical heaters (470 W/canister), and were emplaced under approximately reference DHLW repository conditions. Twelve other simulated DHLW packages were emplaced tinder accelerated-aging or overtest conditions, including the artificial introduction of brine, and a thermal loading approximately three to four times higher than reference. Eight of these 12 test packages contain 1500 W/canister electrical heaters; the other four are filled with DHLW glass.

An Approach to Analysis of High Level waste Container Performance in an Unsaturated Repository Environment

1993 ◽  
Vol 333 ◽  
Author(s):  
John C. Walton ◽  
Narasi Sridhar ◽  
Gustavo Cragnolino ◽  
Tony Torng ◽  
Prasad Nair
Keyword(s):  
Dominant Role ◽  
Near Field ◽  
Temperature Fields ◽  
Localized Corrosion ◽  
High Level Waste ◽  
Quantitative Methodology ◽  
Waste Container ◽  
Wide Range ◽  
Engineered Barrier ◽  
High Level

ABSTRACTOne of the requirements for the performance of waste packages prescribed in 10CFR 60.113 is that the high level waste must be “substantially completely” contained for a minimum period of 300 to 1000 years. During this period, the radiation and thermal conditions in the engineered barrier system and the near-field environment are dominated by fission product decay. In the present U.S design of the engineered barrier system, the outer container plays a dominant role in maintaining radionuclide containment. A quantitative methodology for analyzing the performance of the container is described in this paper. This methodology enables prediction of the evolution of the waste package environment in terms of temperature fields, stability of liquid water on the container surface, and concentration of aggressive ions such as chloride. The initiation and propagation of localized corrosion is determined by the corrosion potential of the container material and critical potentials for localized corrosion. The coiTOsion potential is estimated from the kinetics of the anodic and cathodic reactions including oxygen diffusion through scale layers formed on the container surface. The methodology described is applicable to a wide range of metals, alloys and environmental conditions.

Packaging of High Burnup UO2 and MOX Spent Fuel Considering Temperature Restrictions in the Near Field of a Repository

1997 ◽  
Vol 506 ◽  
Author(s):  
D.F. McGinnes ◽  
J. W. Schneider
Keyword(s):  
Near Field ◽  
Management Program ◽  
High Level Waste ◽  
Heat Output ◽  
Spent Fuel ◽  
Ambient Temperatures ◽  
Heat Loading ◽  
High Burnup ◽  
Maximum Temperatures ◽  
High Level

ABSTRACTThe direct disposal of spent fuel is one of the options considered in the Swiss high level waste management program. One of the important questions, within this program, is the heat generation from high-burnup UO2and MOX spent fuels. Depending on the repository boundary conditions (e.g. ambient temperatures at depth, thermal properties of the host rock etc.), on the maximum temperatures allowed in the near field and on the heat output of the fuel, it may not always be possible to completely fill the conceptual waste canister. The aim of this paper is to address the potential loading of spent fuel into canisters for different possible repository heat loading restrictions

Evolution of Chemistry and Its Effects on the Corrosion of Engineered Barrier Materials

2006 ◽  
Vol 985 ◽  
Author(s):  
Darrell Dunn ◽  
Yi-Ming Pan ◽  
Xihua He ◽  
Lietai Yang ◽  
Roberto Pabalan
Keyword(s):  
Environmental Conditions ◽  
Environmental Influence ◽  
Near Field ◽  
Yucca Mountain ◽  
High Level Waste ◽  
Seepage Water ◽  
Waste Package ◽  
Barrier Materials ◽  
Engineered Barrier ◽  
High Level

ABSTRACTThe evolution of environmental conditions within the emplacement drifts of a potential high-level waste repository at Yucca Mountain, Nevada, may be influenced by several factors, including the temperature and relative humidity within the emplacement drifts and the composition of seepage water. The performance of the waste package and the drip shield may be affected by the evolution of the environmental conditions within the emplacement drifts. In this study, tests evaluated the evolution of environmental conditions on the waste package surfaces and in the surrounding host rock. The tests were designed to (i) simulate the conditions expected within the emplacement drifts; (ii) measure the changes in near-field chemistry; and (iii) determine environmental influence on the performance of the engineered barrier materials. Results of tests conducted in this study indicate the composition of salt deposits was consistent with the initial dilute water chemistry. Salts and possibly concentrated calcium chloride brines may be more aggressive than either neutral or alkaline brines.

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