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Experimental Evidence For Colloid-Facilitated Transport Of Plutonium, Hilary Emerson Dec 2014

Experimental Evidence For Colloid-Facilitated Transport Of Plutonium, Hilary Emerson

All Dissertations

Colloid-facilitated transport of the actinides has been observed previously in the field on the kilometer scale. The objective of this work is to investigate the mechanisms of colloid-facilitated transport with controlled settings and conditions. The experimental work in this dissertation investigates transport of a ternary complex with iron oxide colloids, organic ligands and actinides in the presence of quartz or a natural sandy soil as well as simplified systems building up to the ternary complexes. The first three papers investigate the following: (1) unsaturated transport of iron oxide colloids in a natural sandy soil lysimeter with and without natural organic …


Describing Plutonium Contamination Issues In Hanford Soils: Development Of A Thermodynamic Surface Complexation Model, Sarah Herr Aug 2013

Describing Plutonium Contamination Issues In Hanford Soils: Development Of A Thermodynamic Surface Complexation Model, Sarah Herr

All Theses

The development of remediation strategies for long-term site management requires knowledge of an actinide's geochemical behavior. Understanding this behavior can lead to the formation of a subsurface transport model. For example, plutonium mobility in the subsurface environment is significantly influenced by oxidation-reduction and complexation reactions. This work considered the surface-mediated reduction of plutonium, as well as the hydrolysis and carbonate complexation of the actinide.
Evaluating the significance of these reactions required several variable pH batch sorption studies. Experiments incorporated plutonium and neptunium sorption to sediments from the Hanford Nuclear Reservation in Washington State. Two different sediments were examined: coarse-grained and …


Influence Of Natural Organic Matter On Plutonium Sorption To Gibbsite, Laura Simpkins Aug 2011

Influence Of Natural Organic Matter On Plutonium Sorption To Gibbsite, Laura Simpkins

All Theses

Understanding plutonium geochemical behavior is imperative to the development of schemes for remediation of plutonium environmental contamination and accurate assessment of risks posed by the disposal of plutonium bearing wastes. The primary mechanism of plutonium mobility in the environment is subsurface transport. The mobility of plutonium is significantly influenced by redox and complexation reactions. Although the effects of surface mediated redox reactions on plutonium's subsurface mobility have been previously documented, little has been done to determine the impact of organic materials on sorption behavior and oxidation states. To adequately predict the behavior of plutonium in the environment, the influence of …


Determination Of Sorption Coefficients For Neptunium, Plutonium, Iodine, And Technetium In Engineered And Natural Systems Under Oxidizing And Reducing Conditions, Michael Lilley Dec 2010

Determination Of Sorption Coefficients For Neptunium, Plutonium, Iodine, And Technetium In Engineered And Natural Systems Under Oxidizing And Reducing Conditions, Michael Lilley

All Theses

Plutonium, neptunium, technetium, and iodine present appreciable risks at nuclear waste disposal sites around the world due to their potential mobility. Sorption of each of these radionuclides is profoundly influenced by oxidation/ reduction reactions. Therefore, the mobility of each radionuclide may be greatly influenced by redox conditions of the natural or engineered system. The primary focus of this study was to determine distribution coefficients (Kd) for each radionuclide for engineered concrete and saltstone systems with varying amounts of reducing slag (a cement additive to create a reducing environment), and for iodide/iodate in natural sediments. Saltstones are a mixture …


Plutonium - Humic Acid Stability Constant Determination And Subsequent Studies Examining Sorption In The Ternary Pu(Iv) - Humic Acid - Gibbsite System, Trevor Zimmerman May 2010

Plutonium - Humic Acid Stability Constant Determination And Subsequent Studies Examining Sorption In The Ternary Pu(Iv) - Humic Acid - Gibbsite System, Trevor Zimmerman

All Theses

Plutonium has been released to the environment through a variety of intentional and unintentional mechanisms, including atmospheric testing, disposition from weapons manufacturing processes, and subsurface disposal. Therefore, a thorough understanding of the chemical, physical, and biological processes affecting plutonium transport is imperative. It has been shown that humic acid (HA) (a refractory component of natural organic matter (NOM)) can effectively solubilize plutonium (Santschi et al., 2002). Increased solubility may result in enhanced subsurface transport, due to the higher concentration of Pu in the aqueous phase. In contrast, the formation of ternary surface complexes may hinder actinide transport. Solution pH is …


Modeling Long-Term Plutonium Transport In The Savannah River Site Vadose Zone, Deniz Demirkanli Dec 2006

Modeling Long-Term Plutonium Transport In The Savannah River Site Vadose Zone, Deniz Demirkanli

All Dissertations

Improved understanding of flow and radionuclide transport in vadose zone sediments is fundamental to future planning involving radioactive materials. Long-term experiments were conducted at the Savannah River Site (SRS), where a series of lysimeters containing sources of different Pu oxidation states were placed in the shallow subsurface and exposed to the environment for 2 to 11 years. After the experiments, Pu activity concentrations were measured along vertical cores. The distributions were anomalous in nature, with irregular downward migration and unexpected upward migration. Previous studies suggested that surface-mediated, oxidation/reduction (redox) reactions may be responsible for the anomalies. This hypothesis is tested …