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Wellman, Dawn M.

Publications and source records attributed to Wellman, Dawn M..

At least 19 records

Addressing Technical and Policy Challenges for Remediation of Metals and Radionuclides within Complex Deep Vadose Zone Environments - 17028

Deep vadose zone contamination is a significant issue in many regions of the world. Although remediation of deep vadose zone contamination is important, direct contact with the contamination does not threaten human health or the environment due to its depth in the vadose zone. Yet, movement of contamination from the deep vadose zone to the groundwater creates the potential for exposure and risk to receptors. Therefore, the challenge of deep vadose zone remediation is to maintain a minimal rate of contaminant transport such that flux from the contaminated vadose zone is limited to protect groundwater resources and down-gradient receptors. We herein review major processes for viable remediation of deep vadose zone metal and radionuclides that form the practical constraints on remedial actions and provide an overview of how these principles are being practiced to address key contaminants at the U.S. Department of Energy Hanford Site. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

The Evaluation of Novel Tin Materials for the Removal of Technetium from Groundwater

Technetium-99 ( 99 Tc) is present at several U.S. Department of Energy (DOE) facilities, including the Hanford, Oak Ridge, Paducah, Portsmouth, and Savannah River sites. Due to its mobility, persistence, and toxicity in the environment, developing means to immobilize and/or remove technetium from the environment is currently a top priority for DOE. However, there are currently very few approaches that effectively manage the risks of technetium to human health and the environment. The objective of this study is to evaluate novel synthetic materials that could enable direct removal of technetium from groundwater. The following report •assesses the viability of existing methodologies for synthesis of tin (II) apatite for in situ formation and remediation of 99 Tc within the subsurface environment •discusses the development of alternative methodologies for production of tin (II) apatite •evaluates nanoporous tin phosphate materials for removal of technetium from groundwater.

37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CH↗

Elements of complexity in subsurface modeling, exemplified with three case studies

There are complexity elements to consider when applying subsurface flow and transport models to support environmental analyses. Modelers balance the benefits and costs of modeling along the spectrum of complexity, taking into account the attributes of more simple models (e.g., lower cost, faster execution, easier to explain, less mechanistic) and the attributes of more complex models (higher cost, slower execution, harder to explain, more mechanistic and technically defensible). In this paper, modeling complexity is examined with respect to considering this balance. The discussion of modeling complexity is organized into three primary elements: 1) modeling approach, 2) description of process, and 3) description of heterogeneity. Three examples are used to examine these complexity elements. Two of the examples use simulations generated from a complex model to develop simpler models for efficient use in model applications. The first example is designed to support performance evaluation of soil vapor extraction remediation in terms of groundwater protection. The second example investigates the importance of simulating different categories of geochemical reactions for carbon sequestration and selecting appropriate simplifications for use in evaluating sequestration scenarios. In the third example, the modeling history for a uranium-contaminated site demonstrates that conservative parameter estimates were inadequate surrogates for complex, critical processes and there is discussion on the selection of more appropriate model complexity for this application. All three examples highlight how complexity considerations are essential to create scientifically defensible models that achieve a balance between model simplification and complexity.

conceptual models↗

Integration of National Laboratory and Low-Activity Waste Pre-Treatment System Technology Service Providers - 16435

The National Laboratories are a critical partner and provide expertise in numerous aspects of the successful execution of the Direct-Feed Low Activity Waste Program. The National Laboratories are maturing the technologies of the Low-Activity Waste Pre-Treatment System (LAWPS) consistent with DOE Order 413.3B “Program and Project Management for the Acquisition of Capital Assets” expectations. The National Laboratories continue to mature waste forms, i.e. glass and secondary waste grout, for formulations and predictions of long-term performance as inputs to performance assessments. The working processes with the National Laboratories have been developed in procurements, communications, and reporting to support the necessary delivery-based technology support. The relationship continues to evolve from planning and technology development to support of ongoing operations and integration of multiple highly coordinated facilities.

Low-Activity Waste↗

Performance of a Surface Barrier for Waste Isolation and Flux Reduction at the Hanford Site - 16099

Based on the knowledge gained from a decade of laboratory, field, and numerical studies, the Prototype Hanford Barrier (PHB) was designed and constructed between late 1993 and late 1994 over the 216-B-57 Crib in the 200-BP-1 Operable Unit at the Hanford Site. The PHB has been monitored since 1994 to evaluate the physical, hydrologic, and ecological performance. Two stress tests were carried out in the past: 1) an enhanced (about 3 times the multi-year average of 160 mm/year) precipitation test from water year (WY) 1995 to WY1997, which included simulated 1000-year return, 24-hour rainstorms in March of each year, and 2) a controlled fire test in 2008. The purpose of this article is to present the main findings of the PHB demonstration since 1994. From 1994 to 2013-during which time the barrier experienced 3 years of enhanced precipitation, three 1000-year return, 24-hour simulated rainstorms, and a controlled fire-the PHB limited drainage to well below the 0.5 mm yr{sup -1} design criterion and had minimal erosion. Although the test period represents only 2% of the design life, the observations suggest the PHB is robust enough to control drainage and isolate subsurface contaminants. Future barrier performance will depend on barrier stability and hydrology. Given the 19-year record of successful performance and considering all processes and mechanisms that could degrade barrier stability and hydrology in the future, the results suggest that the PHB is very likely to perform for at least the remainder of its 1000-year design life. This conclusion is based on two assumptions: 1) the exposed sub-grade receives protection against erosion and 2) institutional controls prevent inadvertent human activity on the barrier. The findings at the PHB are useful for the design and monitoring of future surface barriers at Hanford and elsewhere. (authors)

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Performance of a Surface Barrier for Waste Isolation and Flux Reduction at the Hanford Site

Based on the knowledge gained from a decade of laboratory, field, and numerical studies, the Prototype Hanford Barrier (PHB) was designed and constructed between late 1993 and late 1994 over the 216-B-57 Crib in the 200-BP-1 Operable Unit at the Hanford Site. The PHB has been monitored since 1994 to evaluate the physical, hydrologic, and ecological performance. Two stress tests were carried out in the past: (1) an enhanced (about 3 times the multi-year average of 160 mm/year) precipitation test from water year (WY) 1995 to WY1997, which included a man-made 1000-year return 24-hour rainstorms in March each year, and (2) a controlled fire test in 2008. The purpose of this article is to present the main findings of the PHB demonstration since 1994. From 1994 to present, the PHB has limited drainage of less than 0.2 mm yr-1, which is below the 0.5 mm yr-1 design goal, and minimized erosion. The observations suggest the PHB is robust enough to endure the hydrological stress of three times average precipitation and 1000-year return 24-hour rainstorms. After the controlled fire, far less vegetation grows and grasses are the dominant vegetation (compared to shrubs on the unburned section). Even so, the grasses can remove nearly all the stored water in the burned section, although during a longer period of time than in the unburned section. The findings at the PHB are useful for the design and monitoring of future surface barriers at Hanford and elsewhere.

ET Cover↗

Accurate modeling and inversion of electrical resistivity data in the presence of metallic infrastructure with known location and dimension

Electrical resistivity tomography (ERT) has been widely used in environmental applications to study processes associated with subsurface contaminants and contaminant remediation. Anthropogenic alterations in subsurface electrical conductivity associated with contamination often originate from highly industrialized areas with significant amounts of buried metallic infrastructure. The deleterious influence of such infrastructure on imaging results generally limits the utility of ERT where it might otherwise prove useful for subsurface investigation and monitoring. In this manuscript we present a method of accurately modeling the effects of buried conductive infrastructure within the forward modeling algorithm, thereby removing them from the inversion results. The method is implemented in parallel using immersed interface boundary conditions, whereby the global solution is reconstructed from a series of well-conditioned partial solutions. Forward modeling accuracy is demonstrated by comparison with analytic solutions. Synthetic imaging examples are used to investigate imaging capabilities within a subsurface containing electrically conductive buried tanks, transfer piping, and well casing, using both well casings and vertical electrode arrays as current sources and potential measurement electrodes. Results show that, although accurate infrastructure modeling removes the dominating influence of buried metallic features, the presence of metallic infrastructure degrades imaging resolution compared to standard ERT imaging. However, accurate imaging results may be obtained if electrodes are appropriately located.

imaging↗

100-OL-1 Operable Unit Pilot Study: XRF Evaluation of Select Pre-Hanford Orchards

Prior to the acquisition of land by the U.S. Department of War in February 1943 and the creation of the Hanford Site, the land along the Columbia River was home to over 1000 people. Farming and orchard operations by both homesteaders and commercial organizations were prevalent. Orchard activities and the associated application of lead arsenate pesticide ceased in 1943, when residents were moved from the Hanford Site at the beginning of the Manhattan Project. Today, the residues from historical application of lead arsenate pesticide persist in some locations on the Hanford Site

100-OL-1↗

Radionuclide Migration through Sediment and Concrete: 16 Years of Investigations

The Waste Management Project provides safe, compliant, and cost-effective waste management services for the Hanford Site and the U.S. Department of Energy (DOE) complex. Part of these services includes safe disposal of low-level waste and mixed low-level waste at the Hanford Low-Level Waste Burial Grounds in accordance with the requirements of DOE Order 435.1, Radioactive Waste Management. To partially satisfy these requirements, performance assessment analyses were completed and approved. DOE Order 435.1 also requires continuing data collection to increase confidence in the critical assumptions used in these analyses to characterize the operational features of the disposal facility that are relied on to satisfy the performance objectives identified in the order. Cement-based solidification and stabilization is considered for hazardous waste disposal because it is easily done and cost-efficient. One critical assumption is that concrete will be used as a waste form or container material at the Hanford Site to control and minimize the release of radionuclide constituents in waste into the surrounding environment. Concrete encasement would contain and isolate the waste packages from the hydrologic environment and act as an intrusion barrier. Any failure of concrete encasement may result in water intrusion and consequent mobilization of radionuclides from the waste packages. The radionuclides iodine-129, selenium-75, technetium-99, and uranium-238 have been identified as long-term dose contributors (Mann et al. 2001; Wood et al. 1995). Because of their anionic nature in aqueous solutions, these constituents of potential concern may be released from the encased concrete by mass flow and/or diffusion and migrate into the surrounding subsurface environment (Serne et al. 1989; 1992; 1993a, b; 1995). Therefore, it is necessary to assess the performance of the concrete encasement structure and the ability of the surrounding soil to retard radionuclide migration. Each of the test methods performed throughout the lifetime of the project has focused on different aspects of the concrete waste form weathering process. Diffusion of different analytes [technetium-99 (Tc-99), iodine-125 (I-125), stable iodine (I), uranium (U), and rhenium (Re)] has been quantified from experiments under both saturated and unsaturated conditions. The water-saturated conditions provide a conservative estimate of the concrete’s performance in situ, and the unsaturated conditions provide a more accurate estimate of the diffusion of contaminants from the concrete.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Iodine adsorption on ion-exchange resins and activated carbons: batch testing

Iodine sorption onto seven resins and six carbon materials was evaluated using water from well 299-W19-36 on the Hanford Site. These materials were tested using a range of solution-to-solid ratios. The test results are as follows. The efficacy of the resin and granular activated carbon materials was less than predicted based on manufacturers’ performance data. It is hypothesized that this is due to the differences in speciation previously determined for Hanford groundwater. The sorption of iodine is affected by the iodine species in the source water. Iodine loading on resins using source water ranged from 1.47 to 1.70 µg/g with the corresponding K d values from 189.9 to 227.0 mL/g. The sorption values when the iodine is converted to iodide ranged from 2.75 to 5.90 µg/g with the corresponding K d values from 536.3 to 2979.6 mL/g. It is recommended that methods to convert iodine to iodide be investigated in fiscal year (FY) 2015. The chemicals used to convert iodine to iodate adversely affected the sorption of iodine onto the carbon materials. Using as-received source water, loading and K d values ranged from 1.47 to 1.70 µg/g and 189.8 to 226.3 mL/g respectively. After treatment, loading and K d values could not be calculated because there was little change between the initial and final iodine concentration. It is recommended the cause of the decrease in iodine sorption be investigated in FY15. In direct support of CH2M HILL Plateau Remediation Company, Pacific Northwest National Laboratory has evaluated samples from within the 200W pump and treat bioreactors. As part of this analysis, pictures taken within the bioreactor reveal a precipitate that, based on physical properties and known aqueous chemistry, is hypothesized to be iron pyrite or chalcopyrite, which could affect iodine adsorption. It is recommended these materials be tested at different solution-to-solid ratios in FY15 to determine their effect on iodine sorption.

12 MANAGEMENT OF RADIOACTIVE AND NON-RADIOACTIVE W↗

Radioiodine Biogeochemistry and Prevalence in Groundwater

129I is commonly either the top or among the top risk drivers, along with 99Tc, at radiological waste disposal sites and contaminated groundwater sites where nuclear material fabrication or reprocessing has occurred. The risk stems largely from 129I having a high toxicity, a high bioaccumulation factor (90% of all the body’s iodine concentrates in the thyroid), a high inventory at source terms (due to its high fission yield), an extremely long half-life (16M yr), and rapid mobility in the subsurface environment. Another important reason that 129I is a key risk driver is that there is the uncertainty regarding its biogeochemical fate and transport in the environment. We typically can define 129I mass balance and flux at sites, but cannot predict accurately its response to changes in the environment. As a consequence of some of these characteristics, 129I has a very low Drinking Water Standard, DWS, which is set at 1 pCi/L, the lowest of all radionuclides in the Federal Register. Recently, significant advancements have been made in detecting iodine species at ambient groundwater concentrations, defining the nature of the organic matter and iodine bond, and quantifying the role of naturally occurring sediment microbes to promote iodine oxidation and reduction. These recent studies have led to a more mechanistic understanding of radioiodine biogeochemistry. The objective of this review is to describe these advances and to provide a state of the science of radioiodine biogeochemistry relevant to its fate and transport in the terrestrial environment and provide information useful for making decisions regarding the stewardship and remediation of 129I contaminated sites. As part of this review, knowledge gaps were identified that would significantly advance the goals of basic and applied research programs for accelerating 129I environmental remediation and reducing uncertainty associated with disposal of 129I waste. Together the information gained from addressing these knowledge gaps will not alter the observation that 129I is primarily mobile, but it will likely permit demonstration that the entire 129I pool in the source term is not moving at the same rate and some may be tightly bound to the sediment, thereby “smearing” the modeled 129I peak and reducing maximum calculated risk.

Kaplan, Daniel I.↗

100-OL-1 Operable Unit Field Portable X-Ray Fluorescence (XRF) Analyzer Pilot Study Plans

A pilot study is being conducted to support the approval of the Remedial Investigation/Feasibility Study (RI/FS) Work Plan to evaluate the 100-OL-1 Operable Unit (OU) pre-Hanford orchard lands. Based on comments received by the U.S. Environmental Protection Agency (EPA) and Washington State Department of Ecology, the pilot study will evaluate the use of field portable X-ray fluorescence (XRF) spectrometry measurements for evaluating lead and arsenic concentrations on the soil surface as an indicator of past use of lead arsenate pesticide residue in the OU. The work will be performed in the field during the summer of 2014, and assist in the planning for the characterization activities in the RI/FS.

46 INSTRUMENTATION RELATED TO NUCLEAR SCIENCE AND ↗

Radionuclide Retention in Concrete Wasteforms – FY13

Assessing long-term performance of Category 3 waste cement grouts for radionuclide encasement requires knowledge of the radionuclide-cement interactions and mechanisms of retention (i.e., sorption or precipitation); the mechanism of contaminant release; the significance of contaminant release pathways; how wasteform performance is affected by the full range of environmental conditions within the disposal facility; the process of wasteform aging under conditions that are representative of processes occurring in response to changing environmental conditions within the disposal facility; the effect of wasteform aging on chemical, physical, and radiological properties; and the associated impact on contaminant release. This knowledge will enable accurate prediction of radionuclide fate when the wasteforms come in contact with groundwater. Data collected throughout the course of this work will be used to quantify the efficacy of concrete wasteforms, similar to those used in the disposal of low-level waste and mixed low-level waste, for the immobilization of key radionuclides (i.e., uranium, technetium, and iodine). Data collected will also be used to quantify the physical and chemical properties of the concrete affecting radionuclide retention.

concrete↗

Quantification of Kinetic Rate Law Parameters of Uranium Release from Sodium Autunite as a Function of Aqueous Bicarbonate Concentrations

ABSTRACT: Hydrogen carbonate is one of the most significant components within the uranium geochemical cycle. In aqueous solutions, hydrogen carbonate forms strong complexes with uranium. As such, aqueous bicarbonate may significantly increase the rate of uranium release from uranium minerals. Quantifying the relationship of aqueous hydrogen carbonate solutions to the rate of uranium release during dissolution is critical to understanding the long-term fate of uranium within the environment. Single-pass flow-through (SPTF) experiments were conducted to estimate the rate of uranium release from Na meta-autunite as a function of bicarbonate solutions (0.0005-0.003 M) under the pH range of 6-11 and temperatures of 5-60oC. Consistent with the results of previous investigation, the rate of uranium release from sodium autunite exhibited minimal dependency on temperature; but were strongly dependent on pH and increasing concentrations of bicarbonate solutions. Most notably at pH 7, the rate of uranium release exhibited 370 fold increases relative to the rate of uranium release in the absence of bicarbonate. However, the effect of increasing concentrations of bicarbonate solutions on the release of uranium was significantly less under higher pH conditions. It is postulated that at high pH values, surface sites are saturated with carbonate, thus the addition of more bicarbonate would have less effect on uranium release. Results indicate the activation energies were unaffected by temperature and bicarbonate concentration variations, but were strongly dependent on pH conditions. As pH increased from 6 to 11, activation energy values were observed to decrease from 29.94 kJ mol-1 to 13.07 kJ mol-1. The calculated activation energies suggest a surface controlled dissolution mechanism.

Aqueous Bicarbonate↗