Publications

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Deep Borehole Disposal (DBD) of high-level radioactive wastes has been considered an option for geological isolation for many years (Hess et al. 1957). Recent advances in drilling technology have decreased costs and increased reliability for large-diameter (i.e., ≥50 cm [19.7”]) boreholes to depths of several kilometers (Beswick 2008; Beswick et al. 2014). These advances have therefore also increased the feasibility of the DBD concept (Brady et al. 2009; Cornwall 2015), and the current field test, introduced herein, is a demonstration of the DBD concept and these advances.

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Alkaline flocculation holds great potential as a low-cost harvesting method for marine microalgae biomass production. Alkaline flocculation is induced by an increase in pH and is related to precipitation of calcium and magnesium salts. In this study, we used the diatom Phaeodactylum tricornutum as model organism to study alkaline flocculation of marine microalgae cultured in seawater medium. Flocculation started when pH was increased to 10 and flocculation efficiency reached 90% when pH was 10.5, which was consistent with precipitation modeling for brucite or Mg(OH)₂. Compared to freshwater species, more magnesium is needed to achieve flocculation (>7.5 mM). Zeta potential measurements suggest that brucite precipitation caused flocculation by charge neutralization. When calcium concentration was 12.5 mM, flocculation was also observed at a pH of 10. Furthermore, zeta potential remained negative up to pH 11.5, suggesting that precipitated calcite caused flocculation by a sweeping coagulation mechanism.

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Deep Borehole Disposal (DBD) of high-level radioactive wastes has been considered an option for geological isolation for many years (Hess et al. 1957). Recent advances in drilling technology have decreased costs and increased reliability for large-diameter (i.e., ≥50 cm [19.7”]) boreholes to depths of several kilometers (Beswick 2008). These advances have therefore also increased the feasibility of the DBD concept (Brady et al. 2009), and the current field test, introduced herein, is a demonstration of the DBD concept and these advances. The US Department of Energy (DOE) Strategy for the Management and Disposal of Used Nuclear Fuel and High-Level Radioactive Waste (DOE 2013) specifically recommended developing a research and development plan for DBD as a key strategy objective. DOE’s Assessment of Disposal Options for DOE-Managed High-Level Radioactive Waste and Spent Nuclear Fuel (DOE 2014a) concludes “effective implementation of a strategy for management and disposal of all High-Level Waste and Spent Nuclear Fuel” would include focused research on deep boreholes, especially to retain flexible options for disposal of physically smaller DOEmanaged solid radioactive waste forms. More information regarding the characteristics, quantities, and sizes of these physically smaller waste forms is in the Evaluation of Options for Permanent Geologic Disposal of Spent Nuclear Fuel and High-Level Radioactive Waste (SNL 2014).

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Deep Borehole Disposal (DBD) of radioactive waste has some clear advantages over mined repositories, including incremental construction and loading, enhanced natural barriers provided by deep continental crystalline basement, and reduced site characterization. Unfavorable features for a DBD site include upward vertical fluid potential gradients, presence of economically exploitable natural resources, presence of high permeability connection from the waste disposal zone to the shallow subsurface, and significant probability of future volcanic activity. Site characterization activities would encompass geomechanical (i.e., rock stress state, fluid pressure, and faulting), geological (i.e., both overburden and bedrock lithology), hydrological (i.e., quantity of fluid, fluid convection properties, and solute transport mechanisms), chemical (i.e., rock and fluid interaction), and socioeconomic (i.e., likelihood for human intrusion) aspects. For a planned Deep Borehole Field Test (DBFT), site features and/or physical processes would be evaluated using both direct (i.e., sampling and in-hole testing) and indirect (i.e., surface and borehole geophysical) methods for efficient and effective characterization. Surface-based characterization would be used to guide the exploratory drilling program, once a candidate DBFT site has been selected. Borehole based characterization will be used to determine the variability of system state (i.e., stress, pressure, temperature, petrology, and water chemistry) with depth, and to develop material and system parameters relevant for numerical simulation. While the site design of DBD could involve an array of disposal boreholes, it may not be necessary to characterize each borehole in detail. Characterization strategies will be developed in the DBFT that establish disposal system safety sufficient for licensing a disposal array.

This paper describes technical, logistical, and sociopolitical factors to be considered in the development of guidelines for siting a facility for deep borehole disposal of radioactive waste. Technical factors include geological, hydro-geochemical, and geophysical characteristics that are related to the suitability of the site for drilling and borehole construction, waste emplacement activities, waste isolation, and long-term safety of the deep borehole disposal system. Logistical factors to be considered during site selection include: The local or regional availability of drilling contractors (equipment, services, and materials) capable of drilling a large-diameter borehole to approximately 5 km depth; the legal and regulatory requirements associated with drilling, construction of surface facilities, waste handling and emplacement, and postclosure safety; and access to transportation systems. Social and political factors related to site selection include the distance from population centers and the support or opposition of local and state entities and other stakeholders to the facility and its operations. These considerations are examined in the context of the siting process and guidelines for a deep borehole field test, designed to evaluate the feasibility of siting and operating a deep borehole disposal facility.

While deep borehole disposal of nuclear waste should rely primarily on off-the-shelf technologies pioneered by the oil and gas and geothermal industries, the development of new science and technology will remain important. Key knowledge gaps have been outlined in the research roadmap for deep boreholes (B. Arnold et al, 2012, Research, Development, and Demonstration Roadmap for Deep Borehole Disposal, Sandia National Laboratories, SAND2012-8527P) and in a recent Deep Borehole Science Needs Workshop. Characterizing deep crystalline basement, understanding the nature and role of deep fractures, more precisely age-dating deep groundwaters, and demonstrating long-term performance of seals are all important topics of interest. Overlapping deep borehole and enhanced geothermal technology needs include: quantification of seal material performance/failure, stress measurement beyond the borehole, advanced drilling and completion tools, and better subsurface sensors. A deep borehole demonstration has the potential to trigger more focused study of deep hydrology, high temperature brine-rock interaction, and thermomechanical behavior.

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This report documents deep borehole disposal research during FY2014, as directed by U.S. Department of Energy (DOE) Used Fuel Disposition (UFD) Campaign. These research efforts are principally directed at advancing the deep borehole disposal project to the implementation of a full-scale Research, Development, and Demonstration (RD&D) project. Activities of particular relevance to this goal include evaluation of guidelines for selection of a deep borehole field test site, analyses of deep borehole disposal of alternative waste forms, and technical planning for borehole seals research.

Herein, we study the durability of the Sandia Bi-Si oxide Glass Composite Material (GCM) waste form when formulated with different weight percent levels of AgI-MOR. The post-iodine exposure AgI-MOR material was provided to SNL by ORNL. Durability results for the GCM fabricated with 22 and 25% AgI-MOR indicate releases of Ag and I at the same low rates as 15% AgI-MOR GCM, and by the same mechanism. Iodine and Ag release is controlled by the low solubility of an amorphous, hydrated silver iodide, not by the surface-controlled dissolution of I₂- loaded Ag-Mordenite. Based on this data, we postulate that much higher loading levels of AgIMOR are probable in this GCM waste form, and limits will govern by retention of mechanical integrity of the GCM versus the solubility of silver iodide.

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The study develops a novel stochastic frontier modeling approach to the gravity equation for rare earth element (REE) trade between China and its trading partners between 2001 and 2009. The novelty lies in differentiating betweenbehind the border' trade costs by China and theimplicit beyond the border costs' of China's trading partners. Results indicate that the significance level of the independent variables change dramatically over the time period. While geographical distance matters for trade flows in both periods, the effect of income on trade flows is significantly attenuated, possibly capturing the negative effects of financial crises in the developed world. Second, the total export losses due tobehind the border' trade costs almost tripled over the time period. Finally, looking atimplicit beyond the border' trade costs, results show China gaining in some markets, although it is likely that some countries are substituting away from Chinese REE exports.

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Deep boreholes have been proposed for many decades as an option for permanent disposal of high-level radioactive waste and spent nuclear fuel. Disposal concepts are straightforward, and generally call for drilling boreholes to a depth of four to five kilometers (or more) into crystalline basement rocks. Waste is placed in the lower portion of the hole, and the upper several kilometers of the hole are sealed to provide effective isolation from the biosphere. The potential for excellent long-term performance has been recognized in many previous studies. This paper reports updated results of what is believed to be the first quantitative analysis of releases from a hypothetical disposal borehole repository using the same performance assessment methodology applied to mined geologic repositories for high-level radioactive waste. Analyses begin with a preliminary consideration of a comprehensive list of potentially relevant features, events, and processes (FEPs) and the identification of those FEPs that appear to be most likely to affect long-term performance in deep boreholes. The release pathway selected for preliminary performance assessment modeling is thermally-driven flow and radionuclide transport upwards from the emplacement zone through the borehole seals or the surrounding annulus of disturbed rock. Estimated radionuclide releases from deep borehole disposal of spent nuclear fuel, and the annual radiation doses to hypothetical future humans associated with those releases, are extremely small, indicating that deep boreholes may be a viable alternative to mined repositories for disposal of both high-level radioactive waste and spent nuclear fuel. © 2012 Materials Research Society.

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Deep boreholes could be a relatively inexpensive, safe, and rapidly deployable strategy for disposing Americaś nuclear waste. To study this approach, Sandia invested in a three year LDRD project entitled “Radionuclide Transport from Deep Boreholes.” In the first two years, the borehole reference design and backfill analysis were completed and the supporting modeling of borehole temperature and fluid transport profiles were done. In the third year, some of the logistics of implementing a deep borehole waste disposal system were considered. This report describes what was learned in the third year of the study and draws some conclusions about the potential bottlenecks of system implementation.

This document summarizes a three year Laboratory Directed Research and Development (LDRD) program effort to improve our understanding of algal flocculation with a key to overcoming harvesting as a techno-economic barrier to algal biofuels. Flocculation is limited by the concentrations of deprotonated functional groups on the algal cell surface. Favorable charged groups on the surfaces of precipitates that form in solution and the interaction of both with ions in the water can favor flocculation. Measurements of algae cell-surface functional groups are reported and related to the quantity of flocculant required. Deprotonation of surface groups and complexation of surface groups with ions from the growth media are predicted in the context of PHREEQC. The understanding of surface chemistry is linked to boundaries of effective flocculation. We show that the phase-space of effective flocculation can be expanded by more frequent alga-alga or floc-floc collisions. The collision frequency is dependent on the floc structure, described in the fractal sense. The fractal floc structure is shown to depend on the rate of shear mixing. We present both experimental measurements of the floc structure variation and simulations using LAMMPS (Large-scale Atomic/Molecular Massively Parallel Simulator). Both show a densification of the flocs with increasing shear. The LAMMPS results show a combined change in the fractal dimension and a change in the coordination number leading to stronger flocs.

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The effects of algae concentration, ferric chloride dose, and pH on the flocculation efficiency of the freshwater algae Chlorella zofingiensis can be understood by considering the nature of the electrostatic charges on the algae and precipitate surfaces. Two critical conditions are identified which, when met, result in flocculation efficiencies in excess of 90% for freshwater algae. First, a minimum concentration of ferric chloride is required to overcome the electrostatic stabilization of the algae and promote bridging of algae cells by hydroxide precipitates. At low algae concentrations, the minimum amount of ferric chloride required increases linearly with algae concentration, characteristic of flocculation primarily through electrostatic bridging by hydroxide precipitates. At higher algae concentrations, the minimum required concentration of ferric chloride for flocculation is independent of algae concentration, suggesting a change in the primary flocculation mechanism from bridging to sweep flocculation. Second, the algae must have a negative surface charge. Experiments and surface complexation modeling show that the surface charge of C. zofingiensis is negative above a pH of 4.0±0.3 which agrees well with the minimum pH required for effective flocculation. These critical flocculation criteria can be extended to other freshwater algae to design effective flocculation systems. © 2011 Wiley Periodicals, Inc.

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A coordination chemistry analysis of oil-calcite adhesion allows waterflood chemistry controls over enhanced oil recovery from limestones to be understood. The model relies on temperature-dependent surface complexation models of calcite and oil. The primary electrostatic bridges holding oil to calcite are calculated to be [-COO^-][>CaOH₂⁺], [-COO^-][>COOCa⁺], [>CaSO₄^-][-COOCa⁺] and [-COOCa⁺][>COO^-] (“>” denotes calcite surface groups; “-” denotes polar oil surface groups; Mg²⁺ can substitute for Ca⁺²). The [-COO^-][>CaOH₂⁺] bridge between oil carboxylate and protonated calcite calcium sites is most sensitive to changes in waterflood chemistry. Model calculations predict that increased levels of Ca⁺², Mg⁺², and SO₄^-2, alone or in combination, will increase oil recovery from limestones by decreasing the number of [-COO^-][>CaOH₂⁺] bridges. Divalent cations decrease the local interfacial potential by decreasing the net negative charge on oil carboxylate groups; SO₄^-2 coordinates to protonated calcite calcium sites to decrease charge and electrostatic attraction. Increases in ionic strength should increase adhesion by increasing the net charge on each surface, though the effect will be less on calcite. The model presented here requires no fitting parameters yet accurately reproduces observed oil mobilization trends suggesting the model to be a potentially valuable tool for designing chemistries of waterfloods employed in limestones.

A reference design and operational procedures for the disposal of high-level radioactive waste in deep boreholes have been developed and documented. The design and operations are feasible with currently available technology and meet existing safety and anticipated regulatory requirements. Objectives of the reference design include providing a baseline for more detailed technical analyses of system performance and serving as a basis for comparing design alternatives. Numerous factors suggest that deep borehole disposal of high-level radioactive waste is inherently safe. Several lines of evidence indicate that groundwater at depths of several kilometers in continental crystalline basement rocks has long residence times and low velocity. High salinity fluids have limited potential for vertical flow because of density stratification and prevent colloidal transport of radionuclides. Geochemically reducing conditions in the deep subsurface limit the solubility and enhance the retardation of key radionuclides. A non-technical advantage that the deep borehole concept may offer over a repository concept is that of facilitating incremental construction and loading at multiple perhaps regional locations. The disposal borehole would be drilled to a depth of 5,000 m using a telescoping design and would be logged and tested prior to waste emplacement. Waste canisters would be constructed of carbon steel, sealed by welds, and connected into canister strings with high-strength connections. Waste canister strings of about 200 m length would be emplaced in the lower 2,000 m of the fully cased borehole and be separated by bridge and cement plugs. Sealing of the upper part of the borehole would be done with a series of compacted bentonite seals, cement plugs, cement seals, cement plus crushed rock backfill, and bridge plugs. Elements of the reference design meet technical requirements defined in the study. Testing and operational safety assurance requirements are also defined. Overall, the results of the reference design development and the cost analysis support the technical feasibility of the deep borehole disposal concept for high-level radioactive waste.

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Deep boreholes have been proposed for many decades as an option for permanent disposal of high-level radioactive waste and spent nuclear fuel. Disposal concepts are straightforward, and generally call for drilling boreholes to a depth of three to five kilometers into crystalline basement rocks. Waste is placed in the lower portion of the hole, and the upper several kilometers of the hole are sealed to provide effective isolation from the biosphere. The potential for excellent long-term performance has been recognized in many previous studies. This paper reports updated results of what is believed to be the first quantitative analysis of releases from a hypothetical disposal borehole repository using the same performance assessment methodology applied to mined geologic repositories for high-level radioactive waste. Analyses begin with a preliminary consideration of a comprehensive list of potentially relevant features, events, and processes (FEPs) and the identification of those FEPs that appear to be most likely to affect long-term performance in deep boreholes. Performance assessment model estimates of releases from deep boreholes, and the annual radiation doses to hypothetical future humans associated with those releases, are extremely small, indicating that deep boreholes may be a viable alternative to mined repositories for disposal of both high-level radioactive waste and spent nuclear fuel.

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Injection of CO{sub 2}-laden flue gas can decrease the potential for silica and calcite scale formation in cooling tower blowdown by lowering solution pH to decrease equilibrium calcite solubility and kinetic rates of silica polymerization. Flue gas injection might best inhibit scale formation in power plant cooling towers that use impaired makeup waters - for example, groundwaters that contain relatively high levels of calcium, alkalinity, and silica. Groundwaters brought to the surface for cooling will degas CO{sub 2} and increase their pH by 1-2 units, possibly precipitating calcite in the process. Recarbonation with flue gas can lower the pHs of these fluids back to roughly their initial pH. Flue gas carbonation probably cannot lower pHs to much below pH 6 because the pHs of impaired waters, once outgassed at the surface, are likely to be relatively alkaline. Silica polymerization to form scale occurs most rapidly at pH {approx} 8.3 at 25 C; polymerization is slower at higher and lower pH. pH 7 fluids containing {approx}220 ppm SiO{sub 2} require > 180 hours equilibration to begin forming scale whereas at pH 8.3 scale formation is complete within 36 hours. Flue gas injection that lowers pHs to {approx} 7 should allow substantially higher concentration factors. Periodic cycling to lower recoveries - hence lower silica concentrations - might be required though. Higher concentration factors enabled by flue gas injection should decrease concentrate volumes and disposal costs by roughly half.

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Effective capture of atmospheric carbon is a key bottleneck preventing non bio-based, carbon-neutral production of synthetic liquid hydrocarbon fuels using CO{sub 2} as the carbon feedstock. Here we outline the boundary conditions of atmospheric carbon capture for recycle to liquid hydrocarbon fuels production and re-use options and we also identify the technical advances that must be made for such a process to become technically and commercially viable at scale. While conversion of atmospheric CO{sub 2} into a pure feedstock for hydrocarbon fuels synthesis is presently feasible at the bench-scale - albeit at high cost energetically and economically - the methods and materials needed to concentrate large amounts of CO{sub 2} at low cost and high efficiency remain technically immature. Industrial-scale capture must entail: (1) Processing of large volumes of air through an effective CO{sub 2} capture media and (2) Efficient separation of CO{sub 2} from the processed air flow into a pure stream of CO{sub 2}.

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This report evaluates the feasibility of high-level radioactive waste disposal in shale within the United States. The U.S. has many possible clay/shale/argillite basins with positive attributes for permanent disposal. Similar geologic formations have been extensively studied by international programs with largely positive results, over significant ranges of the most important material characteristics including permeability, rheology, and sorptive potential. This report is enabled by the advanced work of the international community to establish functional and operational requirements for disposal of a range of waste forms in shale media. We develop scoping performance analyses, based on the applicable features, events, and processes identified by international investigators, to support a generic conclusion regarding post-closure safety. Requisite assumptions for these analyses include waste characteristics, disposal concepts, and important properties of the geologic formation. We then apply lessons learned from Sandia experience on the Waste Isolation Pilot Project and the Yucca Mountain Project to develop a disposal strategy should a shale repository be considered as an alternative disposal pathway in the U.S. Disposal of high-level radioactive waste in suitable shale formations is attractive because the material is essentially impermeable and self-sealing, conditions are chemically reducing, and sorption tends to prevent radionuclide transport. Vertically and laterally extensive shale and clay formations exist in multiple locations in the contiguous 48 states. Thermal-hydrologic-mechanical calculations indicate that temperatures near emplaced waste packages can be maintained below boiling and will decay to within a few degrees of the ambient temperature within a few decades (or longer depending on the waste form). Construction effects, ventilation, and the thermal pulse will lead to clay dehydration and deformation, confined to an excavation disturbed zone within a few meters of the repository, that can be reasonably characterized. Within a few centuries after waste emplacement, overburden pressures will seal fractures, resaturate the dehydrated zones, and provide a repository setting that strongly limits radionuclide movement to diffusive transport. Coupled hydrogeochemical transport calculations indicate maximum extents of radionuclide transport on the order of tens to hundreds of meters, or less, in a million years. Under the conditions modeled, a shale repository could achieve total containment, with no releases to the environment in undisturbed scenarios. The performance analyses described here are based on the assumption that long-term standards for disposal in clay/shale would be identical in the key aspects, to those prescribed for existing repository programs such as Yucca Mountain. This generic repository evaluation for shale is the first developed in the United States. Previous repository considerations have emphasized salt formations and volcanic rock formations. Much of the experience gained from U.S. repository development, such as seal system design, coupled process simulation, and application of performance assessment methodology, is applied here to scoping analyses for a shale repository. A contemporary understanding of clay mineralogy and attendant chemical environments has allowed identification of the appropriate features, events, and processes to be incorporated into the analysis. Advanced multi-physics modeling provides key support for understanding the effects from coupled processes. The results of the assessment show that shale formations provide a technically advanced, scientifically sound disposal option for the U.S.

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This report summarizes the work completed under the Laboratory Directed Research and Development (LDRD) project 09-1351, 'Computational Investigation of Thermal Gas Separation for CO{sub 2} Capture'. Thermal gas separation for a binary mixture of carbon dioxide and nitrogen is investigated using the Direct Simulation Monte Carlo (DSMC) method of molecular gas dynamics. Molecular models for nitrogen and carbon dioxide are developed, implemented, compared to theoretical results, and compared to several experimental thermophysical properties. The molecular models include three translational modes, two fully excited rotational modes, and vibrational modes, whose degree of excitation depends on the temperature. Nitrogen has one vibrational mode, and carbon dioxide has four vibrational modes (two of which are degenerate). These models are used to perform a parameter study for mixtures of carbon dioxide and nitrogen confined between parallel walls over realistic ranges of gas temperatures and nominal concentrations of carbon dioxide. The degree of thermal separation predicted by DSMC is slightly higher than experimental values and is sensitive to the details of the molecular models.

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Preliminary evaluation of deep borehole disposal of high-level radioactive waste and spent nuclear fuel indicates the potential for excellent long-term safety performance at costs competitive with mined repositories. Significant fluid flow through basement rock is prevented, in part, by low permeabilities, poorly connected transport pathways, and overburden self-sealing. Deep fluids also resist vertical movement because they are density stratified. Thermal hydrologic calculations estimate the thermal pulse from emplaced waste to be small (less than 20 C at 10 meters from the borehole, for less than a few hundred years), and to result in maximum total vertical fluid movement of {approx}100 m. Reducing conditions will sharply limit solubilities of most dose-critical radionuclides at depth, and high ionic strengths of deep fluids will prevent colloidal transport. For the bounding analysis of this report, waste is envisioned to be emplaced as fuel assemblies stacked inside drill casing that are lowered, and emplaced using off-the-shelf oilfield and geothermal drilling techniques, into the lower 1-2 km portion of a vertical borehole {approx}45 cm in diameter and 3-5 km deep, followed by borehole sealing. Deep borehole disposal of radioactive waste in the United States would require modifications to the Nuclear Waste Policy Act and to applicable regulatory standards for long-term performance set by the US Environmental Protection Agency (40 CFR part 191) and US Nuclear Regulatory Commission (10 CFR part 60). The performance analysis described here is based on the assumption that long-term standards for deep borehole disposal would be identical in the key regards to those prescribed for existing repositories (40 CFR part 197 and 10 CFR part 63).

Understanding the corrosion of spent nuclear fuel (SNF) and the subsequent mobilization of released radionuclides, particularly under oxidizing conditions, is one of the key issues in evaluating the long-term performance of a nuclear waste repository. However, the large amounts of iron in the metal waste package may create locally reducing conditions that would lower corrosion rates for the SNF, as well as reduce the solubility of some key radionuclides, e.g., Tc and Np. In order to investigate the interactions among SNF-waste package-fluids, four smallscale (∼1:40 by length) waste package mockups were constructed using metals similar to those proposed for use in waste packages at the proposed repository at Yucca Mountain. Each mockup experiment differed with respect to water input, exposure to the atmosphere, and temperature. Simulated Yucca Mountain process water (YMPW) was injected into three of the mockups at a rate of 200 μL per day for five days a week using a calibrated needle syringe. The YMPW was prepared by equilibrating 50 mg/L silica as sodium metasilicate with air, and adding enough HC1 to lower the pH to 7.6 in contact with an excess of powdered calcite. X-ray powder diffraction and scanning electron microscopy confirm that, where corrosion occurred, the dominant corrosion product in all cases was magnetite. In the high temperature (60°C) experiment, hematite and a fibrous, Fe-O-Cl phase were also identified. The Fe(II)/Fe(III) ratios measured in the corrosion products using a wet chemistry technique indicate extremely low oxygen fugacities (10-36 bar). Experiments are in progress in which 0.1g powdered UO2 was included in the mock-up in order to investigate the relative kinetics of Fe and U oxidation and to identify the U corrosion products formed under these conditions. © 2008 Materials Research Society.

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