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Application of a Mass Balance Partitioning Model of Ra-226, Pb-210 and Po-210 to Freshwater Lakes and Streams

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Application of a Mass Balance Partitioning Model of Ra-226, Pb-210 and Po-210 to Freshwater Lakes and Streams Application of a mass balance partitioning model of Ra-226, Pb-210 and Po-210 to freshwater lakes and streams Submitted by: Kevin John Britton Thesis submitted to the Faculty of Graduate and Postdoctoral Studies in partial fulfillment of the requirements for the Master of Science degree specialization in Chemical and Environmental Toxicology (Earth Sciences) Department of Earth Sciences Faculty of Science University of Ottawa Supervisors: Robert Jack Cornett† (Department of Earth Sciences) Ian D Clark (Department of Earth Sciences) Co-Supervisors: Trevor J Stocki (Department of Earth Sciences) Adrienne LM Ethier (Department of Earth Sciences) Thesis Committee: Clément Bataille Laurel Sinclair 2018 November 15 © Kevin John Britton, Ottawa, Canada, 2018 Abstract The objectives of this thesis were: (1) to develop a mass balance partitioning model of the natural uranium-238 series comprising radium-226, lead-210 and polonium-210 and (2) to apply the model to estimate the source and fate of these radionuclides in freshwater lakes and streams. Samples were collected from Ottawa River watershed tributaries and measured for lead-210 and polonium-210 content to determine the water concentrations that were input to the model. The radium-226 partitioning model was developed by reconstructing and analyzing Quantitative Water, Air, Sediment Interaction (QWASI) models of lead for Lake Ontario and Hamilton Harbour and selecting parameters for an updated QWASI model of lead for a Lake Ontario basin. This study gave insight about model basis definition, and partition coefficient and sediment particle constraint. The radium-226 series model was formulated by connecting separate QWASI modules for radium-226, lead-210 and polonium-210 with decay and ingrowth terms. The radium-226 model was applied to studies of Crystal Lake, Wisconsin; Bickford Pond, Massachusetts; and Clinton River, Michigan, using parameters reported in these and other studies. Model error was evident in the applications to Crystal Lake due to underlying lake heterogeneity, to Bickford Pond due to unidentified sources of lead-210 from sediment diffusion or watershed runoff, and to Clinton River from watershed runoff. The model was applied to seven Laurentian Shield lakes in the Ottawa River watershed using the sample measurements as the basis for water concentration inputs. The application showed that hydrologic flushing rate may be a factor in the proportion of watershed atmospheric deposition and overall Pb-210 input to the water. Laurentian Shield Lakes with the lowest hydrologic flushing rates (<3 a-1) had proportions of Pb-210 losses to sediment greater than 85%. In another application to Judge Sissons Lake, Nunavut, the model indicated that the watershed was the source of about 85% of Pb-210 and 98% of Po-210 input to the water, and that a significant geologic component of Pb-210 input to the lake was likely. The model indicated that most of the Pb-210 in Judge Sissons Lake was lost to outflow, and that most of the Po-210 was lost to sediment. The model showed that sedimentation is a better proxy measurement for atmospheric deposition of Pb-210 to the Laurentian lakes than originally estimated. The model also showed that watershed contributions to Judge Sissons Lake could explain the observed background concentrations of Pb-210 and Po-210. ii Acknowledgements I would like to acknowledge and thank Adrienne Ethier and Canadian Nuclear Laboratories (CNL) for initiating this research into adaptation of the HERMES model to uranium series radionuclides. Adrienne provided the original HERMES model, hosted me in the Environmental Protection Branch at CNL, and assisted with manuscript review. I would also like to thank Marilyne Stuart for assuming the role as CNL liaison. I would like to thank Diane Martens at AREVA (Orano) Resources Canada for providing the Kiggavik study data reports. I am most grateful to Jack Cornett at the University of Ottawa who enabled this thesis. I was fortunate for the time he shared with me. He is missed by many students. I would like to thank the staff and students of A. E. Lalonde Laboratory, particularly Barbara Francisco, Soroush Fard and Cole MacDonald. I would like to acknowledge and thank Trevor Stocki at Health Canada. Trevor assumed the role of supervisor after Jack. He gave many detailed reviews during manuscript writing. I would like to express special thanks to Ian Clark for bridging the gap at the University of Ottawa as official supervisor in these final months. Both made completion of this project possible. I would like to acknowledge and thank Jack Cornett and Canadian Nuclear Laboratories for funding this project. iii Statement of Originality Chapter 2 I studied the QWASI aquivalence model for lead in Lake Ontario and Hamilton Harbour developed by Dr. Donald Mackay et al to identify challenges to the planned extension to the Ra-226 series nuclides. I expected that the QWASI aquivalence model applications would be internally and mutually consistent. I studied the model partly by verifying and adapting the HERMES mercury model developed by Dr. Adrienne Ethier et al. to the QWASI lead formulation. I reproduced QWASI aquivalence model applications and confirmed the sources for the parameters cited. I found no unexpected inconsistencies among the QWASI aquivalence model applications, but two of the three did not constrain particle flux for molar conservation. Further, I found that input and output concentrations were not consistent, which I addressed with a modification of the basic QWASI aquivalence model to differentiate between diffusion from water to sediment and from sediment to water. I implemented the diffusion modification and particle conservation constraint to the existing applications. I applied the updated model of lead in Lake Ontario using some parameters from a rate constant study, and to a Lake Ontario basin using a combination of parameters representing a new application. Chapter 3 The updated QWASI aquivalence model was applicable to lead but needed to be further developed for the Ra-226 series, and a method was required to fit parameters for specific applications. I expected that the model would be applicable to Pb-210 using many of the existing parameters and could be extended to Ra-226 and Po-210 by selection of appropriate parameters from existing studies and the literature. I expected that the separate modules could be connected by terms for decay and ingrowth. I developed the Ra-226 model by linking the updated QWASI modules with terms for loss and ingrowth by decay for Ra-226, Pb-210 and Po-210. I assigned parameters to this model from previously published studies of Crystal Lake, Wisconsin; Bickford Pond, Massachusetts; and Clinton River, Michigan; and other sources, and adjusted the parameters in an optimization process developed from the Chapter 2 study. The results indicated that the model was extendable to each of the selected Ra-226 nuclides, and that modules could be linked to account for radioactive decay and ingrowth. The developed method was effective in adjusting parameters to the data in the original studies. Comparison of the Ra-226 model to the original dynamic study models revealed discrepancies, attributed either to the original models missing episodic events, and / or to the inability of the steady-state Ra-226 model to represent the effects of parameter variation by single expected values. Chapter 4 Two hypotheses were investigated in Chapter 4 with the Ra-226 series model developed in Chapter 3. The first question was whether the sedimentation iv proportion of Pb-210 losses from the water in a set of Laurentian lakes was as low as estimated in a previous study (CORNETT, 1984). The second question was whether water and sediment measurements of Judge Sissons Lake at the proposed Nunavut mine site (GUERIN, 2012) indicated a watershed contribution to Pb-210 and Po-210 concentrations. I augmented the Laurentian lakes study data with measurements of water from local streams. I selected sample locations, collected samples and with Soroush Fard I performed wet chemistry operations in the A. E. Lalonde actinide laboratory at the University of Ottawa under the direction of Dr. Robert Cornett. Dr. Cornett performed the alpha spectrometry measurements and Cole MacDonald and Dr. Barbara Francisco performed the Inductively-Coupled Plasma Source Mass Spectrometry (ICP-MS) measurements. I applied the Ra-226 model to the original studies using data from these and other sources. I used the Ra-226 model to estimate lake process rates in the original studies. The sedimentation rates in the Laurentian lakes were concluded to be higher than originally estimated: above 85% in five of the seven lakes. I concluded that the watershed was the source of most of the Pb-210 and Po-210 in Judge Sissons Lake water and sediment, and further that a significant proportion from the watershed may originate in the ground. v Contents Abstract ........................................................................................................ ii Acknowledgements ....................................................................................... iii Statement of Originality ................................................................................. iv Contents ...................................................................................................... vi Abbreviations .............................................................................................. xiv 1 Introduction ............................................................................................
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