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HEATON-THESIS.Pdf BIOGEOCHEMICAL INVESTIGATION OF CENTRIFUGED FINE TAILINGS DEPOSITS AT AN OIL SANDS MINE IN NORTHERN ALBERTA, CANADA A Thesis Submitted to the College of Graduate Studies and Research In Partial Fulfillment of the Requirements For the Degree of Master of Science In the Department of Geological Sciences University of Saskatchewan Saskatoon By KAITLYN KASSANDRA HEATON © Copyright Kaitlyn Kassandra Heaton, September 2015. All rights reserved. PERMISSION TO USE In presenting this thesis in partial fulfillment of the requirements for a Postgraduate degree from the University of Saskatchewan, I agree that the Libraries of this University may make it freely available for inspection. I further agree that permission for copying of this thesis in any manner, in whole or in part, for Scholarly purposes may be granted by the professors who supervised my thesis work or, in their absence, by the Head of the Department in which my thesis work was done. It is understood that any copying or publication or use of this thesis or parts thereof for financial gain shall not be allowed without my written permission. It is also understood that due recognition shall be given to me and to the University of Saskatchewan in any scholarly use which may be made of any material in my thesis. Requests for permission to copy or to make other use of material in this thesis in whole or in part should be addressed to: Head of the Department of Geological Sciences University of Saskatchewan 114 Science Place Saskatoon, Saskatchewan, Canada S7N 5E2 i ABSTRACT Centrifuged fine tailings (CFT) technology was developed to reduce volumes of fluid fine tailings (FFT) stored in tailings ponds at oil sands mines. Increasing FFT inventories in tailings ponds results from slow settlement of clay minerals suspended in oil sands process-affected water (OSPW). High sodium (Na) concentrations in OSPW increase the electrical double layer (EDL) thickness at clay-mineral surfaces, which hinders aggregation and, therefore, settlement. Production of CFT involves dredging FFT from tailings ponds, amending with polyacrylamide and gypsum, and decanter centrifuging. This process promotes aggregation and flocculation, and decreases gravimetric water content from approximately 70 to 55 % (w/w). The resulting CFT is deposited in thin lifts (< 2 m) into sub-aerial containment areas to facilitate further dewatering via freeze-thaw cycling. This research was focused on characterizing the biogeochemical conditions and processes within the CFT deposits. These deposits remain tension-saturated and, similar to tailings ponds, anaerobic redox processes including iron (Fe) reduction, sulfate (SO4) reduction, and methanogenesis likely dominate. The geochemistry, mineralogy, and microbiology of core samples from two field-scale test deposits and two full-scale production deposits were examined. Results were compared with previously published data from FFT deposits to assess impacts of chemical amendments on biogeochemical processes within CFT deposits. Pore-water chemistry within the CFT deposits is affected by evaporative concentration of dissolved ions, which leads to high concentrations of salts (Na, 3000 mg L-1; Cl, 1500 mg L-1; -1 -1 SO4, 5000 mg L ) and naphthenic acids (NAs 150 mg L ) near the surface (< 0.3 m) of these deposits. Increases in concentrations of conservative ions (i.e., Cl) indicated that 30 to 40 % of pore water was lost to evaporation at a depth of 0.1 m below surface. Results also suggest that microbially-mediated Fe reduction, SO4 reduction, and methanogenesis are dominant redox processes within the CFT deposits. Microbes related to genera known to use these terminal electron acceptors were identified by high-throughput DNA sequencing data. Increases in ii dissolved Fe and H2S with depth were also indicative of Fe and SO4 reduction, respectively. These results provide the first insight into biogeochemical conditions and processes within oil sands CFT deposits. iii ACKNOWLEDGEMENTS An immense thank you to my (co) supervisors, Drs. Matt Lindsay and Joyce McBeth, for all the guidance, encouragement, and mentorship provided throughout my degree - it was invaluable. Thank you so much for supporting my goal of finishing so quickly; I thoroughly appreciate the attention to detail you’ve shown in providing feedback and comments in the thesis writing process. You have helped to inspire me to consider a more holistic view of environmental problems than I would have done without this experience, which will be valuable in my future career. Thank you to Dr. Won Jae Chang for reminding me to consider statistics during experimental design and for the comments that helped to strengthen my thesis. Thank you also to my external examiner, Terry Fonstad, for reviewing this thesis and providing many helpful comments. Funding for this research was provided by Syncrude Canada Ltd and the National Sciences and Engineering Research Council of Canada (NSERC) through an Industrial Research Chair held by Matt Lindsay. A portion of the research described in this paper was performed at the Canadian Light Source, which is funded by the Canada Foundation for Innovation, the NSERC, the National Research Council Canada, the Canadian Institutes of Health Research, the Government of Saskatchewan, Western Economic Diversification Canada, and the University of Saskatchewan. My field sampling campaign could not have been completed without support. Thank you to Dallas Heisler for liaising information from others at Syncrude. Thank you to Lori Cyprian and Chris Beierling for the Syncrude on-site support, as well as Richard Maslanko and David Duford for Syncrude lab support. Thank you to Dyan Pratt and Spencer, Dave, Chris, Ben, Jake, Ashley, Tiereny, Farhan, and Dallas from Conetec for the assistance with collecting the cores. I also could not have possibly finished my lab work without the support of several people. Thank you to Danielle Penrod, Jake Nesbitt, Matt Lindsay, Jared Robertson, Yu Han, Amy Pitman, Colin Pitman, and Kathryn Dompierre - I couldn’t have completed my first and iv second stream sampling without you. Thank you to Darshil Koshti for preparing and measuring samples for PXRD. I also want to acknowledge Jonathan Vyskocil for processing the DNA sequencing data in mothur and related sequencing support, Matt Lindsay for processing the XANES data, and Jake Nesbitt for teaching me how to use PREEQCi and Match!. Thank you to Amy Pitman for the sanity check nearly every lunch-hour. Thank you to my family and friends for keeping me inspired that this research is interesting and valuable. And, finally, I am so grateful to Duncan for his unwavering support throughout my degree. v To Duncan. TABLE OF CONTENTS PERMISSION TO USE ................................................................................................................... i ABSTRACT .............................................................................................................................. ii ACKNOWLEDGEMENTS ........................................................................................................... iv LIST OF TABLES .......................................................................................................................... x LIST OF FIGURES ....................................................................................................................... xi LIST OF ABBREVIATIONS ...................................................................................................... xiii CHAPTER 1 INTRODUCTION ............................................................................................... 1 1.1 Research Hypotheses and Objectives .................................................................... 3 1.2 Thesis Organization............................................................................................... 4 CHAPTER 2 BIOGEOCHEMICAL CHARACTERISTICS OF CENTRIFUGED OIL SANDS FINE TAILINGS....................................................................................................... 5 2.1 Executive Summary .............................................................................................. 5 2.2 Introduction ........................................................................................................... 5 2.3 Site Description ..................................................................................................... 8 2.4 Materials and Methods .......................................................................................... 9 2.4.1 Sample collection ............................................................................................ 9 2.4.2 Pore-water extraction and analysis ................................................................ 10 2.4.3 Geochemical modelling................................................................................. 11 2.4.4 Microbiology ................................................................................................. 11 2.4.5 Mineralogy .................................................................................................... 13 2.4.6 Solid-phase geochemistry ............................................................................. 13 vii 2.5 Results ................................................................................................................. 14 2.5.1 Pore-water chemistry..................................................................................... 14 2.5.2 Microbiology ................................................................................................
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