Colloid Facilitated Transport of Radioactive Cations in the Vadose Zone: Field Experiments Oak Ridge

The overarching goal of this study was to improve understanding of colloid-facilitated transport of radioactive cations through unsaturated soils and sediments. We conducted a suite of laboratory experiments and field experiments on the vadose-zone transport of colloids, organic matter, and associated contaminants of interest to the U.S. Department of Energy (DOE). The laboratory and field experiments, together with transport modeling, were designed to accomplish the following detailed objectives: 1. Evaluation of the relative importance of inorganic colloids and organic matter to the facilitation of radioactive cation transport in the vadose zone; 2. Assessment of the role of adsorption and desorption kinetics in the facilitated transport of radioactive cations in the vadose zone; 3. Examination of the effects of rainfall and infiltration dynamics and in the facilitated transport of radioactive cations through the vadose zone; 4. Exploration of the role of soil heterogeneity and preferential flow paths (e.g., macropores) on the facilitated transport of radioactive cations in the vadose zone; 5. Development of a mathematical model of facilitated transport of contaminants in the vadose zone that accurately incorporates pore-scale and column-scale processes with the practicality of predicting transport with readily available parameters

Understanding the Subsurface Reactive Transport of Transuranic Contaminants at DOE Sites

Our primary hypothesis is that actinides can interact with surfaces in fundamentally different ways than other metals, metalloids, and oxyanions and that this fundamental difference requires new approaches to studying and modeling transuranic sorption to minerals and geomedia. This project supports a key mission of the SBR program to develop sufficient scientific understanding such that DOE sites will be able to incorporate coupled physical, chemical, and biological processes into decision making for environmental management and long-term stewardship, while also supporting DOE’s commitment to education, training, and collaboration with DOE user facilities

Influences of Flow Transients and Porous Medium Heterogeneity on Colloid-Associated Contaminant Transport in the Vadose Zone

We are investigating the role of colloids in the movement of radionuclides and metals through water unsaturated porous media. This research is guided by a key objective of the Environmental Management Science Program (EMSP), which is to improve conceptual and predictive models for contaminant movement in complex vadose zone environments. In the report entitled National Roadmap for Vadose Zone Science and Technology [DOE, 2001], increases in the understanding of colloid-contaminant interactions, colloid mobilization, and colloid deposition within unsaturated soils are cited as requisite needs for predicting contaminant fate and distribution in the vadose zone. We seek to address these needs by pursuing three overarching goals: (1) identify the mechanisms that govern colloid mobilization, transport, and deposition within unsaturated porous media; (2) quantify the role of colloids in scavenging and facilitating the transport of contaminants; and (3) develop and test a mathematical model suitable for simulating the movement of colloid-associated radionuclides and metals through variably saturated porous media

Colloid Facilitated Transport of Radioactive Cations in the Vadose Zone: Field Experiments Oak Ridge

The overarching goal of this study was to improve understanding of colloid-facilitated transport of radioactive cations through unsaturated soils and sediments. We conducted a suite of laboratory experiments and field experiments on the vadose-zone transport of colloids, organic matter, and associated contaminants of interest to the U.S. Department of Energy (DOE). The laboratory and field experiments, together with transport modeling, were designed to accomplish the following detailed objectives: 1. Evaluation of the relative importance of inorganic colloids and organic matter to the facilitation of radioactive cation transport in the vadose zone; 2. Assessment of the role of adsorption and desorption kinetics in the facilitated transport of radioactive cations in the vadose zone; 3. Examination of the effects of rainfall and infiltration dynamics and in the facilitated transport of radioactive cations through the vadose zone; 4. Exploration of the role of soil heterogeneity and preferential flow paths (e.g., macropores) on the facilitated transport of radioactive cations in the vadose zone; 5. Development of a mathematical model of facilitated transport of contaminants in the vadose zone that accurately incorporates pore-scale and column-scale processes with the practicality of predicting transport with readily available parameters

Influences of Flow Transients and Porous Medium Heterogeneity on Colloid-Associated Contaminants Transport in the Vadose Zone

During the past year (June 2003 to June 2004), work at Yale has centered on investigating the influences of porewater pH, flow transients, and the presence of natural organic matter (NOM) on the deposition and mobilization of clay colloids (kaolinite and illite) within columns packed with unsaturated porous media. The experiments on pH and flow-transient effects were described in our First-Term Progress Report (which covered the initial 18 months of the study) and will not be repeated here. More recent experiments on the role of NOM in colloid transport proved equally as interesting. Even at porewater concentrations as low as 0.2 mg/L, soil-humic acid substantially lowered clay-colloid deposition rates compared to the case in which soil-humic acid was absent from the porewater. We attribute this to adsorption of the humic acid to the positively charged edge sites of the clay colloids, which effectively reduced the colloid affinity for negatively charged air- and solid-water interfaces. Comparison of the results of the column experiments to calculations of a new mathematical model has sharpened our inferences regarding mechanisms that govern the rate-limited deposition and mobilization of colloids. We are testing these inferences by carrying out flow-and-transport visualization experiments. We have constructed a semi-transparent representation of a porous medium, consisting of a rectangular parallel-plate chamber that encloses 3-5 layers of uniformly sized sand grains. Ceramic plates fused to the ends of the chamber maintain the capillary tension and syringe pumps (located at the inlet and outlet ends) regulate the flow of water and colloids through the partially saturated sand. By placing the chamber beneath a microscope, we can examine the distribution of colloids between air-water and solid-water interfaces, directly measure the kinetics of deposition onto these interfaces, and observe the mechanisms that contribute to the release of immobile colloids. To date, we have used fluorescent microspheres as the colloids, but, once we refine our methodology, we intend to use clay particles as the colloids