A Methodology for Characterizing Potential Uranium Transport in Deep Geological Disposal Sites
Abstract
In order to make safe and reasonable decisions about radioactive waste disposal in deep geologic sites, it is important to understand the fate and potential transport of long half-life transuranic radionuclides over a wide range of time and distance scales. The objective of this study was to evaluate and demonstrate new experimental methods for quantifying the potential for actinide transport in deep fractured crystalline rock formations. We selected a fractured/weathered granodiorite at the Grimsel Test Site (GTS) in Switzerland as a model system because field experiments involving uranium, as well as other actinides, have already been conducted. Working on this system provides a unique opportunity to compare lab experimental results with field-scale observations. Drilled rock cores and weathered fracture fill material (FFM) from the GTS were shipped to Los Alamos National Laboratory, characterized by x-ray diffraction and microscopy, and used in batch sorption/desorption and column breakthrough experiments. Uranium solutions were made by adding uranium to a synthetic Grimsel groundwater that matched the natural water chemistry found in the GTS groundwater. Batch and breakthrough experiments were conducted using solutions between pH 6.9 and 9.0. All column experiments were conducted using syringe pumps at low flow rate (<0.3 ml h-1) in small columns containing 5 g of material with pore volumes of 2-3 ml. These small columns allow rapid and economical evaluation of sorption/desorption behavior under flowing conditions (and in duplicate or triplicate). Solutions were switched to uranium-free synthetic Grimsel groundwater after equilibration in batch experiments or after near-steady uranium breakthrough occurred in column experiments. The measurement of uranium concentrations as a function of time under these conditions allowed interrogation of desorption rates which we believe control uranium fate and transport over long time and distance scales. Uranium transport was conservative and matched tritium breakthrough for pH 9.0; however, retardation increased when pH was reduced to 7.9 and 6.9. We are currently evaluating uranium adsorption/desorption rates as a function of water chemistry (initial focus on pH), with future testing planned to evaluate the influence of carbonate concentrations, flow rates, mineralogy, bentonite colloids and other actinides (e.g., Am). Figure 1. Uranium breakthrough results for (a) 6.5 μM U, (b) U-free solution, (c) flow rate increased from 0.3 to 0.6 mL h-1, (d) pH increased from 6.8 to 7.2, and (e) pH increased from 7.2 to 8.8.
- Publication:
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AGU Fall Meeting Abstracts
- Pub Date:
- December 2013
- Bibcode:
- 2013AGUFM.H21D1092D
- Keywords:
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- 1012 GEOCHEMISTRY Reactions and phase equilibria;
- 1009 GEOCHEMISTRY Geochemical modeling;
- 0412 BIOGEOSCIENCES Biogeochemical kinetics and reaction modeling;
- 1847 HYDROLOGY Modeling