Americium, Cesium, and Plutonium Colloid-Facilitated Transport in a Groundwater/Bentonite/Fracture Fill Material System: Column Experiments and Model Results

Abstract:

The objective of this study was to investigate and quantify the effects of desorption kinetics and colloid transport on radionuclides with different sorption affinities. We focused on quantifying transport mechanisms important for upscaling in time and distance. This will help determine the long-term fate and transport of radionuclides to aid in risk assessments. We selected a fractured/weathered granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model crystalline rock repository system because the system has been thoroughly studied and field experiments involving radionuclides have already been conducted. Working on this system provides a unique opportunity to compare lab experiments with field-scale observations.

Weathered fracture fill material (FFM) and bentonite used as backfill at the GTS were characterized (e.g., BET, SEM/EDS, QXRD), and batch and breakthrough column experiments were conducted. Solutions were prepared in synthetic groundwaters that matched the natural water chemistry. FFM samples were crushed, rinsed, sieved (150-355 µm), and equilibrated with synthetic groundwater. Bentonite was crushed, sodium-saturated, equilibrated with synthetic groundwater, and settled to yield a stable suspension. Suspensions were equilibrated with Am, Cs, or Pu. All experiments were conducted with Teflon^®materials to limit sorption to system components. After radionuclide/colloid injections reached stability, radionuclide-free solutions were injected to observe the desorption and release behavior.

Aliquots of effluent were measured for pH, colloid concentration, and total and dissolved radionuclides. Unanalyzed effluent from the first column was then injected through a second column of fresh material. The process was repeated for a third column and the results of all three breakthrough curves were modeled with a multi-site/multi-rate MATLAB code to elucidate the sorption rate coefficients and binding site densities of the bentonite colloids and fracture fill material. Nearly 50% of the sorbed Am was exchanged from the colloids to the fracture filling material in each of the three columns; whereas, less Cs and Pu was desorbed with each pass through a new column. Using a two-site kinetic model allowed for interrogation of desorption rates and dominant transport parameters.