IMPACTS OF REDUCING CONDITIONS IN THE SATURATED ZONE AT YUCCA MOUNTAIN

Variations in groundwater redox chemistry in the saturated zone near Yucca Mountain could have significant repository to the accessible environment. This study examines geochemical data relevant to the distribution of redox impacts on processes associated with the potential transport of redox-sensitive radionuclides from the proposed conditions in the saturated zone, the relationships between redox state and solubility and sorption coefficients for technetium and neptunium, and sensitivity in transport model simulations. Results indicate evidence for a zone of reducing conditions in the volcanic rocks of the saturated zone located to the east and south of the repository and along the inferred flow paths from the repository. A working hypothesis is that these reducing conditions are related to the presence of minor pyrite in the matrix of some volcanic units. Chemical equilibrium modeling of technetium solubility using EQ3/6 software codes is used to estimate the value of solubility limits as a function of Eh. Surface complexation modeling with the EQ3 code is used to estimate neptunium sorption coefficient values as a function of Eh. A general analytical approach, one-dimensional reactive transport modeling, and the three-dimensional saturated zone site-scale transport model using the FEHM software code are used to evaluate the impacts of solubility limits and enhanced sorption in reducing zones on the simulated transport of technetium and neptunium in the saturated zone. Results show that if precipitation occurs in response to flow through a reducing zone, then the peak concentration released to the accessible environment will be restricted to the solubility limit. Simulations also show that enhanced sorption within a reducing zone of modest width leads to significantly greater retardation of radionuclides in the saturated zone

Modeling acid-gas generation from boiling chloride brines

<p>Abstract</p> <p>Background</p> <p>This study investigates the generation of HCl and other acid gases from boiling calcium chloride dominated waters at atmospheric pressure, primarily using numerical modeling. The main focus of this investigation relates to the long-term geologic disposal of nuclear waste at Yucca Mountain, Nevada, where pore waters around waste-emplacement tunnels are expected to undergo boiling and evaporative concentration as a result of the heat released by spent nuclear fuel. Processes that are modeled include boiling of highly concentrated solutions, gas transport, and gas condensation accompanied by the dissociation of acid gases, causing low-pH condensate.</p> <p>Results</p> <p>Simple calculations are first carried out to evaluate condensate pH as a function of HCl gas fugacity and condensed water fraction for a vapor equilibrated with saturated calcium chloride brine at 50-150°C and 1 bar. The distillation of a calcium-chloride-dominated brine is then simulated with a reactive transport model using a brine composition representative of partially evaporated calcium-rich pore waters at Yucca Mountain. Results show a significant increase in boiling temperature from evaporative concentration, as well as low pH in condensates, particularly for dynamic systems where partial condensation takes place, which result in enrichment of HCl in condensates. These results are in qualitative agreement with experimental data from other studies.</p> <p>Conclusion</p> <p>The combination of reactive transport with multicomponent brine chemistry to study evaporation, boiling, and the potential for acid gas generation at the proposed Yucca Mountain repository is seen as an improvement relative to previously applied simpler batch evaporation models. This approach allows the evaluation of thermal, hydrological, and chemical (THC) processes in a coupled manner, and modeling of settings much more relevant to actual field conditions than the distillation experiment considered. The actual and modeled distillation experiments do not represent expected conditions in an emplacement drift, but nevertheless illustrate the potential for acid-gas generation at moderate temperatures (<150°C).</p

The Disposal Systems Evaluation Framework for DOE-NE

The Used Fuel Disposition (UFD) Campaign within DOE-NE is evaluating storage and disposal options for a range of waste forms and a range of geologic environments. For each waste form and geologic environment combination, there are multiple options for repository conceptual design. The Disposal Systems Evaluation Framework (DSEF) is being developed to formalize the development and documentation of options for each waste form and environment combination. The DSEF is being implemented in two parts. One part is an Excel workbook with multiple sheets. This workbook is designed to be user friendly, such that anyone within the UFD Campaign can use it as a guide to develop and document repository conceptual designs that respect thermal, geometric, and other constraints. The other part is an Access relational database file that will be centrally maintained to document the ensemble of conceptual designs developed with individual implementations of the Excel workbook. The DSEF Excel workbook includes sheets for waste form, environment, geometric constraints, engineered barrier system (EBS) design, thermal, performance assessment (PA), materials, cost, and fuel cycle system impacts. Each of these sheets guides the user through the process of developing internally consistent design options, and documenting the thought process. The sheets interact with each other to transfer information and identify inconsistencies to the user. In some cases, the sheets are stand-alone, and in other cases (such as PA), the sheets refer the user to another tool, with the user being responsible to transfer summary results into the DSEF sheet. Finally, the DSEF includes three top-level sheets: inputs & results, interface parameters, and knowledge management (references). These sheets enable users and reviewers to see the overall picture on only a few summary sheets, while developing the design option systematically using the detailed sheets. The DSEF Access relational database file collects the key inputs, results, and interface parameters from each Excel workbook implementation. The power of a relational database is available to sort and organize groups of designs, and to answer queries about what evaluations have been done in the UFD Campaign