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Geochemical Evolution of Fracture Filling Minerals from the Chalk River Laboratory Site

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Geochemical Evolution of Fracture Filling Minerals from the Chalk River Laboratory Site Geochemical Evolution of Fracture Filling Minerals from the Chalk River Laboratory Site, Ontario, Canada by Long Tian A thesis presented to the University of Waterloo in fulfillment of the thesis requirement for the degree of Master of Science in Earth Sciences Waterloo, Ontario, Canada, 2016 © Long Tian 2016 Author’s Declaration I hereby declare that I am the sole author of this thesis. This is a true copy of the thesis, including any required revisions, as accepted by any examiners. I understand that my thesis may be made electronically available to the public. ii Abstract The isotope geochemistry combined with fluid inclusion studies of several generations of fracture minerals from the Chalk River Laboratory site (CRL) has been applied to investigate the past fluid evolution including hydrothermal processes and hydrogeochemical evolution of the rock mass. Typical fracture minerals found at the CRL site include chlorite, quartz, dolomite, and calcite. Fracture mineral investigations use oxygen and carbon isotopes from calcites combined with fluid inclusion information such as homogenization temperatures (Th), and melting temperatures (Tm) to calculate temperature and salinity of calcite forming fluids. By combining Th with oxygen isotopic data, we were able to use δ18O geothermometry calculations to estimate past isotopic characteristics and composition of the fluids responsible for calcite precipitation. From petrologic evidence, calcite from the CRL site mainly includes four varieties: fibrous calcite, metasomatic calcite, crystal calcite, and vuggy calcite. Fibrous calcite precipitated at a temperature of 78 to 128 oC with a δ13C signature of -4.91 to -7.88 ‰ (VPDB) and a δ18O signature of -9.36 to -17.34 ‰ (VPDB). These calcites were formed at an elevated temperature, in a low salinity, Na-Cl fluid that could have been a mixture of hydrothermal water derived from meteoric fluids or seawater. Metasomatic calcite precipitated at 62.1 to 90.0 oC with a δ13C signature of -4.64 to -8.59 ‰ (VPDB) and a δ18O signature of -11.98 to -15.08 ‰ (VPDB). These fluids were elevated in temperature, had higher salinity and a Ca-Na-Cl composition similar to a sedimentary basinal brine. iii Crystal calcite separated into three groups according to fluid inclusion analyses and results, which are (a) elevated-temperature (67 to 113 oC) low-salinity calcite (lower than 15.14 wt. %), (b) elevated-temperature (73.7 to 91.7 oC) high-salinity (30 to 40 wt. %) calcite, and (c) higher-temperature (179.6 to 199 oC) low-salinity (lower than 7.33 wt. %) calcite. Group (a) has a δ13C isotopic signature of -5.61 to -10.42 ‰ (VPDB) and a δ18O signature of -8.35 to -16.04 ‰ (VPDB), Group (b) has a δ13C isotopic signature of -4.64 to -8.60 ‰ (VPDB) and a δ18O signature of -12.34 to -15.04 ‰ (VPDB), and Group (c) has δ13C signature of -5.59 to -8.06 ‰ (VPDB) and a δ18O signature of -10.03 to -16.17 ‰ (VPDB). Group (a) most likely formed from a hydrothermal fluid with a meteoric water origin, Group (b) could have formed during hydrothermal fluid mixing with an evaporated seawater or basinal brine, and group (c) seems to have formed as a result of a mixture of meteoric and lower salinity metamorphic or crystalline rock fluids. Vuggy calcite precipitated at 85 to 89 oC with a δ13C signature of -7.47 to -9.04 ‰ (VPDB) and a δ18O signature of -9.32 to -10.59 ‰ (VPDB). This case is from a high temperature, high Ca-Na-Cl salinity fluid which is hydrothermal fluids mixed with basinal brines. Strontium isotopic ratios, thorium-uranium ratios and REE data associated with the fracture calcites show that they have a limited water/rock interaction with the host bedrock. Some elevated thorium or uranium concentration were sourced from specific rock types such as pegmatite intrusions in the site. iv Acknowledgments I would like to thank my advisor Dr. Shaun K. Frape for his guidance and patience in the lab and all the thesis edits. Thanks for giving me a chance to participate in this project and helping me with all my confusion. I would like to thank Rhys Gwynne for helping me in the Environmental Isotope Laboratory and fluid inclusion experiments. I would like to thank Lori Labelle, and Yinze Wang for the assistance of my thesis. I would like to thank my parents for all the support of my master study. I appreciate my mom Nai Zhang to help me in fluid inclusion experiments and analyses in China. I would like to thank Karen Sharp for answers of my questions and assistance of my thesis. I would like to thank my committee, Brian Kendall and Lingling Wu for your help, feedback and constructive comments. v Table of Contents Author’s Declaration ......................................................................................................................... ii Abstract ............................................................................................................................................ iii Acknowledgments ............................................................................................................................. v List of Figures ................................................................................................................................. vii List of Tables .................................................................................................................................... xi Introduction ....................................................................................................................................... 1 Bedrock Geology at CRL .............................................................................................................. 7 Fracture minerals ........................................................................................................................ 13 Quaternary geology ..................................................................................................................... 16 Methodology ................................................................................................................................... 18 Results and Discussion.................................................................................................................... 22 Petrography and fracture minerals .............................................................................................. 22 Results of fluid inclusion analyses .............................................................................................. 37 Isotopic results for 13C-18O ......................................................................................................... 44 δ18O geothermometry results and analyses ................................................................................. 46 Strontium results and analyses .................................................................................................... 50 Elemental geochemistry results and analyses ............................................................................. 53 Summary ......................................................................................................................................... 61 Reference ........................................................................................................................................ 65 Appendix 1 ...................................................................................................................................... 71 Appendix 2 ...................................................................................................................................... 79 Appendix 3 ...................................................................................................................................... 85 Appendix 4 ...................................................................................................................................... 89 Appendix 5 ...................................................................................................................................... 92 Appendix 6 ...................................................................................................................................... 93 vi List of Figures Figure 1. Map of the Chalk River Nuclear Laboratory site ...................................................................... 2 Figure 2. The range of isotopic measurements on fracture calcites from other Canadian sites compared to Chalk River calcites measured in preious studies at the site. Also shown are the potential end members; hydrothermal or modern/meteoric source water (after Blyth et al., 2009) ....................... 6 Figure 3. A) Lithotectonic subdivision of the southwestern Grenville Province and the Ottawa- Bonnechere graben including the location of the Chalk River Laboratories site (CRL) (Davidson, 1998; Neymark et al., 2013). B) Site geology of the CRL site showing three different gneiss assemblages from A to C (Thivierge et al., 2011). ........................................................................... 8 Figure 4. Stratigraphic column for the CRL site showing geologic ages and information and tectonic events that occured in the area (from Thivierge et al., 2011). .......................................................... 9 Figure 5. Lithostructural configuration of the CRL site including the three bedrock assemblages recognized by CRL personal and a cross section showing the geologic divisions (from Thivierge et al., 2011) ....................................................................................................................................
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