Publications

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Radioactive iodine, 129I, a component of spent nuclear fuel, is of particular concern due to its extremely long half-life, its potential mobility in the environment and its effects on human health. In the spent fuel reprocessing scheme under consideration, the 129I is released in gaseous form and collected using Ag-loaded zeolites such as Ag-mordenite. The 129I can react with the Ag to form insoluble AgI. We have investigated the use of low temperature-sintering glass powders mixed with either AgI or AgI-zeolite to produce dense waste forms that can be processed at 500°C, where AgI volatility is low. These mixtures can contain up to 20 wt% crushed AgI-mordenite or up to 50 wt% AgI. Both types of waste forms were found to have the high iodine leach resistance in these initial studies.

Concerns over rising concentrations of greenhouse gases in the atmosphere have resulted in serious consideration of policies aimed at reduction of anthropogenic carbon dioxide (CO2) emissions. If large scale abatement efforts are undertaken, one critical tool will be geologic sequestration of CO2 captured from large point sources, specifically coal and natural gas fired power plants. Current CO2 capture technologies exact a substantial energy penalty on the source power plant, which must be offset with make-up power. Water demands increase at the source plant due to added cooling loads. In addition, new water demand is created by water requirements associated with generation of the make-up power. At the sequestration site however, saline water may be extracted to manage CO2 plum migration and pressure build up in the geologic formation. Thus, while CO2 capture creates new water demands, CO2 sequestration has the potential to create new supplies. Some or all of the added demand may be offset by treatment and use of the saline waters extracted from geologic formations during CO2 sequestration. Sandia National Laboratories, with guidance and support from the National Energy Technology Laboratory, is creating a model to evaluate the potential for a combined approach to saline formations, as a sink for CO2 and a source for saline waters that can be treated and beneficially reused to serve power plant water demands. This presentation will focus on the magnitude of added U.S. power plant water demand under different CO2 emissions reduction scenarios, and the portion of added demand that might be offset by saline waters extracted during the CO2 sequestration process.

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In an effort to address the potential to scale up of carbon dioxide (CO{sub 2}) capture and sequestration in the United States saline formations, an assessment model is being developed using a national database and modeling tool. This tool builds upon the existing NatCarb database as well as supplemental geological information to address scale up potential for carbon dioxide storage within these formations. The focus of the assessment model is to specifically address the question, 'Where are opportunities to couple CO{sub 2} storage and extracted water use for existing and expanding power plants, and what are the economic impacts of these systems relative to traditional power systems?' Initial findings indicate that approximately less than 20% of all the existing complete saline formation well data points meet the working criteria for combined CO{sub 2} storage and extracted water treatment systems. The initial results of the analysis indicate that less than 20% of all the existing complete saline formation well data may meet the working depth, salinity and formation intersecting criteria. These results were taken from examining updated NatCarb data. This finding, while just an initial result, suggests that the combined use of saline formations for CO{sub 2} storage and extracted water use may be limited by the selection criteria chosen. A second preliminary finding of the analysis suggests that some of the necessary data required for this analysis is not present in all of the NatCarb records. This type of analysis represents the beginning of the larger, in depth study for all existing coal and natural gas power plants and saline formations in the U.S. for the purpose of potential CO{sub 2} storage and water reuse for supplemental cooling. Additionally, this allows for potential policy insight when understanding the difficult nature of combined potential institutional (regulatory) and physical (engineered geological sequestration and extracted water system) constraints across the United States. Finally, a representative scenario for a 1,800 MW subcritical coal fired power plant (amongst other types including supercritical coal, integrated gasification combined cycle, natural gas turbine and natural gas combined cycle) can look to existing and new carbon capture, transportation, compression and sequestration technologies along with a suite of extracting and treating technologies for water to assess the system's overall physical and economic viability. Thus, this particular plant, with 90% capture, will reduce the net emissions of CO{sub 2} (original less the amount of energy and hence CO{sub 2} emissions required to power the carbon capture water treatment systems) less than 90%, and its water demands will increase by approximately 50%. These systems may increase the plant's LCOE by approximately 50% or more. This representative example suggests that scaling up these CO{sub 2} capture and sequestration technologies to many plants throughout the country could increase the water demands substantially at the regional, and possibly national level. These scenarios for all power plants and saline formations throughout U.S. can incorporate new information as it becomes available for potential new plant build out planning.

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Reprocessing nuclear fuel releases gaseous radio-iodine containing compounds which must be captured and stored for prolonged periods. Ag-loaded mordenites are the leading candidate for scavenging both organic and inorganic radioiodine containing compounds directly from reprocessing off gases. Alternately, the principal off-gas contaminant, I2, and I-containing acids HI, HIO3, etc. may be scavenged using caustic soda solutions, which are then treated with bismuth to put the iodine into an insoluble form. Our program is focused on using state-of-the-art materials science technologies to develop materials with high loadings of iodine, plus high long-term mechanical and thermal stability. In particular, we present results from research into two materials areas: (1) zeolite-based separations and glass encapsulation, and (2) in-situ precipitation of Bi-I-O waste forms. Ag-loaded mordenite is either commercially available or can be prepared via a simple Ag+ ion exchange process. Research using an Ag+-loaded Mordenite zeolite (MOR, LZM-5 supplied by UOP Corp.) has revealed that I2 is scavenged in one of three forms, as micron-sized AgI particles, as molecular (AgI)x clusters in the zeolite pores and as elemental I2 vapor. It was found that only a portion of the sorbed iodine is retained after heating at 95o C for three months. Furthermore, we show that even when the Ag-MOR is saturated with I2 vapor only roughly half of the silver reacted to form stable AgI compounds. However, the Iodine can be further retained if the AgI-MOR is then encapsulated into a low temperature glass binder. Follow-on studies are now focused on the sorption and waste form development of Iodine from more complex streams including organo-iodine compounds (CH3I). Bismuth-Iodate layered phases have been prepared from caustic waste stream simulant solutions. They serve as a low cost alternative to ceramics waste forms. Novel compounds have been synthesized and solubility studies have been completed using competing groundwater anions (HCO3-, Cl- and SO42-). Distinct variations in solubility were found that related to the structures of the materials.

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Expansion of uranium mining in the United States is a concern to some environmental groups and sovereign Native American Nations. An approach which may alleviate some problems is to develop inherently safe in situ uranium recovery ('ISR') technologies. Current ISR technology relies on chemical extraction of trace levels of uranium from aquifers that, once mined, can still contain dissolved uranium and other trace metals that are a health concern. Existing ISR operations are few in number; however, high uranium prices are driving the industry to consider expanding operations nation-wide. Environmental concerns and enforcement of the new 30 ppb uranium drinking water standard may make opening new mining operations more difficult and costly. Here we propose a technological fix: the development of inherently safe in situ recovery (ISISR) methods. The four central features of an ISISR approach are: (1) New 'green' leachants that break down predictably in the subsurface, leaving uranium, and associated trace metals, in an immobile form; (2) Post-leachant uranium/metals-immobilizing washes that provide a backup decontamination process; (3) An optimized well-field design that increases uranium recovery efficiency and minimizes excursions of contaminated water; and (4) A combined hydrologic/geochemical protocol for designing low-cost post-extraction long-term monitoring. ISISR would bring larger amounts of uranium to the surface, leave fewer toxic metals in the aquifer, and cost less to monitor safely - thus providing a 'win-win-win' solution to all stakeholders.

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We investigated the synthesis of bismuth oxy-iodide and iodate compounds, in an effort to develop materials for iodine recovery from caustic waste streams and/or final waste disposal if repository conditions included ambient conditions similar to those under which the iodine was initially captured. The results presented involve the in-situ crystallization of layered bismuth oxide compounds with aqueous dissolved iodine (which resides as both iodide and iodate in solution). Although single-phase bismuth oxy-iodide materials have already been described in the context of capturing radioiodine, our unique contribution is the discovery that there is a mixture of Bi-O-I compositions, not described in the prior work, which optimize both the uptake and the degree of insolubility (and leachability) of iodine. The optimized combination produces a durable material that is suitable as a waste form for repository conditions such as are predicted at the Yucca Mountain repository (YMP) or in a similar type of repository that could be developed in coordination with iodine production via Global Nuclear Energy Program (GNEP) production cycles. © 2008 Materials Research Society.

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