Shallow land burial in vadose zone sediment at the Hanford Site in Washington is being considered for the disposal of Category 3 low-level waste. A series of column experiments were conducted to evaluate and model the performance of the soil surrounding the trench encasement material for iodine-129 and technetium-99 by evaluating the mobility of these nuclides through the surrounding Trench 8 soil. These experiments were designed to determine effective diffusion coefficients for ¹²⁷I and ⁹⁹Tc through the following system: from contaminated soil into uncontaminated soil. The tests were performed at two different soil moisture contents to evaluate the effects of soil moisture content on diffusion. This thesis describes the experimental methods and presents the diffusion results for this media type. It was found that as the moisture content increased the diffusion increased by an order of magnitude (iodine 4% and 7% moisture content soil effective diffusion coefficients were 8.90E-08 and 1.84E-07 cm²/s respectively, and technetium 4% and 7% moisture content soil diffusion coefficients were 7.61E-08 and 1.45E-07 cm²/s respectively). These results, in combination with other diffusion systems results, will allow the development of release models and contaminant migration models that can be used to estimate the long-term fate of dose-controlling radionuclides that are or will be buried in solid waste burial trenches. / Graduation date: 2004

The Greater than Class C (GTCC) Environmental Impact Statement (EIS) evaluated the potential impacts from the construction and operation of a new facility or facilities, or use of an existing facility, employing various disposal methods (geologic repository, intermediate depth borehole, enhanced near surface trench, and above grade vault) at six federal sites and generic commercial locations. For three of the locations being considered as possible locations, consulting tribes were brought in to comment on their perceptions on how GTCC low level radioactive waste would affect Native American resources (land, water, air, plants, animals, archaeology, etc.) short and long term. The consulting tribes produced essays that were incorporated into the EIS and these essays are in turn included in this collection. This essay was produced by the Confederated Tribes of the Umatilla Indian Reservation.

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Thesis (M.S.)--Mississippi State University. Department of Chemical Engineering. / Title from title screen. Includes bibliographical references.

Thesis (M.S.)--Mississippi State University. Dave C. Swalm School of Chemical Engineering. / Title from title screen. Includes bibliographical references.

Uranium (U) is a crucial contaminant in the Hanford Site. Remediation techniques to prevent contaminant migration of U located in the soils to other important water resources such as the Columbia River are of paramount importance. Given the location of the contaminant in the deep vadose zone, sequestration of U caused by ammonia (NH3) gas injections appears to be a feasible method to decrease U mobility in the contaminated subsurface via pH manipulation, ultimately converting aqueous U mobile phases to lower solubility precipitates that are stable in the natural environment. This study evaluated the stability of those U-bearing precipitates via preparation of artificial precipitates mimicking those that would be created after NH3 gas injections and sequential extractions experiment. Results showed that most of the U was recovered with the extracting solutions targeted to remove uranyl silicates and hard-to-extract U phases, suggesting that U present in the solid particles has strong bonds to the vadose zone sediments, causing the precipitates to be stable and therefore the remediation technology to be effective under the simulated conditions.

The purpose of this work was to explore the use of fractional evaporative crystallization as a technology that can be used to separate medium-curie waste from the Hanford Site tank farms into a high-curie waste stream, which can be sent to a Waste Treatment and Immobilization Plant (WTP), and a low-curie waste stream, which can be sent to Bulk Vitrification. Experimental semi-batch crystallizations of sodium salts from simulant solutions of double-shell tank (DST) feed demonstrated that the recovered crystalline product met the purity requirement for exclusion of cesium and nearly met the requirement on sodium recovery. Batch fractional evaporative crystallization involves the removal of multiple solutes from a feed solution by the progressive achievement of supersaturation (through evaporation) and concomitant nucleation and growth of each species. The slurry collected from each of these crystallization stages was collected and introduced to filtration and washing steps. The product crystals obtained after washing were sampled for analysis by polarized light microscopy (PLM), dried, and sieved. The PLM results aided in identification of species crystallized in each stage. Carbonation was used as a supplemental method to evaporative crystallization in order to increase the sodium recovery in DST experiments. Carbonation was necessary due to the high aluminum ion concentration in the solution, which leads to formation of a viscous gel during evaporation. This gel was avoided by reacting carbon dioxide with hydroxyl ions, which modified the system behavior. Through two stages of carbonation, each followed by evaporation, the effect of carbonation on sodium recovery was demonstrated.

The purpose of the work described in this thesis was to explore the use of fractional crystallization as a technology that can be used to separate medium-curie waste from the Hanford Site tank farms into a high-curie waste stream, which can be sent to a Waste Treatment and Immobilization Plant (WTP), and a low-curie waste stream, which can be sent to Bulk Vitrification. The successful semi-batch crystallization of sodium salts from two single shell tank simulant solutions (SST Early Feed, SST Late Feed) demonstrated that the recovered crystalline product met the purity requirement for exclusion of cesium, sodium recovery in the crystalline product and the requirement on the sulfate-to-sodium molar ratio in the stream to be diverted to the WTP. The experimental apparatus, procedures and results obtained in this thesis on scaled-down experiments of SST Early and Late Feed simulated solutions were adapted and reproduced under hot-cell with actual wastes by our partners at Hanford. To prepare the application of the pretreatment process to pilot scale process, several varation to the feed solutions were investigated including the presence of carboxylates and amines organics compounds and solids particles. Results of the study showed that 4 organics species presented complications to the process (NTA, HEDTA, EDTA and sodium citrate) while the other species (Formate, acetate, glycolate and IDA) and solids particles did not in the conditions of the stored wastes. In this thesis, the kinetics of the crystalline species formed at the condition of the early feed certification run (66 °C and 25 g/h evaporation) were determined along with the effect of the operating temperature and evaporation rate on these kinetics. On one hand, the study of evaporation rate values ranging from 25g/h to 75g/h showed that an increase in evaporation rate increased the specific nucleation while decreasing the specific growth rate. On the other hand, experiments on operating temperature ranging from 35 °C to 75 °C displayed that the nucleation rate of all species increased with temperature at the exception of sodium carbonate monohydrate and burkeite crystals, and that the growth rate of all species increased with temperature at the exception of sodium nitrate. Furthermore, sulfate based crystals such as trisodium fluoride sulfate were only roduced at 45 °C and 75 °C. A simple steady state MSMPR population balance model was developed expressing the total population density function as the sum of the specific population density functions. The specific semi-batch crystallization kinetics were implemented in this model.

This presentation is a project overview and discussion of Native American participation in preparing documents for the Greater Than Class C Environmental Impact Statement. Tribal representatives were involved in the assessments at the Hanford Site, Nevada Test Site, and Los Alamos National Lab.

The purpose of the work described in this thesis was to explore the use of fractional crystallization as a technology that can be used to separate medium-curie waste from the Hanford Site tank farms into a high-curie waste stream, which can be sent to a Waste Treatment and Immobilization Plant (WTP), and a low-curie waste stream, which can be sent to Bulk Vitrification. The successful semi-batch crystallization of sodium salts from two single shell tank simulant solutions (SST Early Feed, SST Late Feed) demonstrated that the recovered crystalline product met the purity requirement for exclusion of cesium, sodium recovery in the crystalline product and the requirement on the sulfate-to-sodium molar ratio in the stream to be diverted to the WTP. In this thesis, experimental apparatus, procedures and results are given on scaled-down experiments of SST Early Feed for hot-cell adaptation along with operating parameters and crystallization mechanism studies on early feed multi-solute crystallization. Moreover, guidance is given regarding future steps towards adapting the technology to multi-salt crystallization kinetic parameter estimates and modeling. Crystallization, Evaporative Fractional Crystallization, Nuclear Waste Pretreatment, Cesium Removal, Hanford, SST Early and Late feed, Multi-solute, Multi-salts, Simulant Testing