Colloid-Facilitated Transport of Low-Solubility Radionuclides: A Field, Experimental, and Modeling Investigation

For the last several years, the Underground Test Area (UGTA) program has funded a series of studies carried out by scientists to investigate the role of colloids in facilitating the transport of low-solubility radionuclidesin groundwater, specifically plutonium (Pu). Although the studies were carried out independently, the overarching goals of these studies has been to determine if colloids in groundwater at the NTS can and will transport low-solubility radionuclidessuch as Pu, define the geochemical mechanisms under which this may or may not occur, determine the hydrologic parameters that may or may not enhance transport through fractures and provide recommendations for incorporating this information into future modeling efforts. The initial motivation for this work came from the observation in 1997 and 1998 by scientists from Lawrence Livermore National Laboratory (LLNL) and Los Alamos National Laboratory (LANL) that low levels of Pu originally from the Benham underground nuclear test were detected in groundwater from two different aquifers collected from wells 1.3 km downgradient (Kersting et al., 1999). Greater than 90% of the Pu and other radionuclideswere associated with the naturally occurring colloidal fraction (< 1 micron particles) in the groundwater. The colloids consisted mainly of zeolite ( mordenite, clinoptilolite/ heulandite), clays (illite,more » smectite) and cristobalite(SiO{sub 2}). These minerals were also identified as alteration mineral components in the host rock aquifer, a rhyolitic tuff. The observation that Pu can and has migrated in the subsurface at the NTS has forced a rethinking of our basic assumptions regarding the mechanical and geochemical transport pathways of low-solubility radionuclides. If colloid-facilitated transportis the primary mechanism for transporting low-solubility radionuclidesin the subsurface, then current transport models based solely on solubility arguments and retardation estimates may underestimate the flux and rate of Pu transport. Currently, the role of colloids in facilitating the transport of low-solubility radionuclidesis not understood well enough to effectively model contaminant transport. A fundamental understanding of the role that colloids may or may not play in the transport of low-solubility radionuclidesis needed in order to predict contaminant transport, design remediation strategies and provide risk assessments. Ryan and Elimelech (1996) have argued that in order to evaluate the potential for colloids to transport radionuclides, several criteria must be met: (1) colloids must exist and be stable, (2) radionuclidesmust have a high sorption affinity for the colloids, and (3) colloids must be transported. Only then can we understand the conditions where colloids can and will facilitate transport of radionuclides. In this report we compile the results from a series of field, laboratory and modeling studies funded by the UGTA program in order to evaluate the potential for colloids to transport low-solubility radionuclidesat the NTS. The studies presented in this report fall under three general areas of investigation: Characterization of natural colloids in groundwater at NTS, Pu sorption/desorption experiments on colloid minerals identified in NTS groundwater, and Transport of Pu-doped colloids through fractured rock core. Chapter 1 is a background review of our current understanding of colloids and their role in facilitating contaminant transport. Chapters 2, and 3 are field studies that focused on characterizing natural colloids at different hydrologic environments at the NTS and address Ryan and Elimelech's (1996) first criteria regarding the existence and stability of colloids. Chapters 4, 5 and 6 are laboratory experimental studies that investigate the sorption/desorption behavior of Pu and other low-solubility radionuclideson colloid minerals observed in NTS groundwater. These studies evaluate Ryan and Elimelech's (1996) second criteria that the affinity of Pu for colloids must be high. Chapters 7, 8, 9, and 10 are laboratory studies that focus on whether colloids can be transported through fractures. These transport studies address Ryan and Elimelech's (1996) third criteria that colloids must be transported. Chapter 11 discusses the implications of the fracture flow experimental results. Chapter 12 provides recommendations for future work that would help reduce uncertainties associated with the prediction of colloid-facilitated radionuclidetransport at the NTS.« less