Date of Award

12-2017

Document Type

Thesis

Degree Name

Master of Science (MS)

Department

Environmental Engineering and Earth Sciences

Committee Member

Dr. Timothy A. DeVol, Committee Chair

Committee Member

Dr. Brian A. Powell

Committee Member

Dr. Daniel I. Kaplan

Abstract

The objective of this work is to quantify the one-dimensional spatial distribution of radionuclides in field lysimeters from the Radionuclide Field Lysimeter Experiment (RadFLEX) facility at the Savannah River Nationals Laboratory (SRNL). The lysimeters, containing 137Cs, 60Co, 133Ba and 152Eu incorporated either into solid wasteforms (Portland cement and reducing grout) or introduced into soil via a filter paper wasteform, were weathered for three to four years. The initial contaminant activities range from 4.0 to 9.0 MBq for the cementitious wasteforms and 0.25 to 0.47 MBq for the filter paper wasteform. An analytical method was developed to perform non-destructive measurements to quantify the spatial distributions measured in field lysimeters. This method provides an alternative to traditional destructive techniques to determine the spatial distribution of activity. This non-destructive method also allows for multiple scans to be performed periodically. Observing how these distributions change with time would improve modeling transport parameters. The detection system consists of a collimated high-purity germanium (HPGe) radiation detector coupled with a linear translational table. A lead collimator is used to achieve spatial resolution as high as 0.25 cm. The lysimeters are positioned relative to the detector using a linear translation stage that can move vertically via a computer-controlled stepping motor. A user control interface was developed with National Instruments LabVIEW® that synchronizes the data acquisition from the radiation detector with the lysimeter movement and positioning thus allowing the lysimeter scans to be automated. The detection efficiency of the system was investigated using two methods. Europium-152 is an ideal candidate for calibration source due to its multiple gamma-ray emissions across a wide range of energies. One method uses a 152Eu point source as the calibration standard while the other method uses the 152Eu within the lysimeter systems themselves as the calibration standard. These methods show that system geometry and source distribution are the key factors influencing the detection efficiency. This suggest that to reduce the impact from the source distribution and geometry variability within a volume, that lysimeters be rotated during measurements. These scans showed downward mobility of 60Co and 133Ba when the radionuclides were incorporated directly into the Savannah River Site (SRS) soil via the filter paper wasteform. When radionuclides were incorporated into the cementitious wasteforms positioned in the SRSS soil, 137Cs exhibited both upward and downward dispersion while the other radionuclides showed no movement. This dispersion was more significant for the Portland cement than the reducing grout wasteform. In the case of the filter paper wasteform, 137Cs mobility was greatly reduced. This suggests the presence of a cementitious wasteform enhances 137Cs mobility. The movement of 137Cs from the solid wasteform was modelled using a retarded diffusion model. Retardation factors for 137Cs are determined to range from approximately 700-2500 for Portland cement, 1500-4000 for reducing grout, and up to 2500-8000 the filter paper wasteform. Numerical simulations were run to investigate the hypothesis that ions released from the wasteforms compete for sorption sites in the SRS soil, enhancing the mobility of 137Cs. These simulations suggest ion-competition could be a factor, but more data is needed to explore this mechanism for Cs+ transport. Understanding radionuclide movement in the environment is important for informing strategies used for waste management and disposal.

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