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Source of Sulphur and the Alteration Footprint of the George Fisher Zn-Pb-Ag Massive Sulphide Deposit, Australia

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Source of Sulphur and the Alteration Footprint of the George Fisher Zn-Pb-Ag Massive Sulphide Deposit, Australia Source of sulphur and the alteration footprint of the George Fisher Zn-Pb-Ag massive sulphide deposit, Australia Dissertation zur Erlangung des Grades eines Doktors der Naturwissenschaften (doctor rerum naturalium) am Fachbereich Geowissenschaften der Freien Universität Berlin vorgelegt von: Philip Rieger Berlin, October 2020 First reviewer (Erstgutachterin): Prof. Dr. Sarah A. Gleeson Department of Earth Sciences, Freie Universität Berlin Inorganic and Isotope Geochemistry, GFZ German Research Centre of Geosciences Second reviewer (Zweitgutachter): Prof. Dr. Stephen Roberts School of Ocean and Earth Science, National Oceanography Centre, University of Southampton Doctoral Committee (Promotionsausschuss): Prof. Dr. Esther M. Schwarzenbach (Vorsitz) Department of Earth Sciences, Freie Universität Berlin Prof. Dr. Timm John Department of Earth Sciences, Freie Universität Berlin Prof. Dr. Sarah A. Gleeson Department of Earth Sciences, Freie Universität Berlin Inorganic and Isotope Geochemistry, GFZ German Research Centre of Geosciences Prof. Dr. Stephen Roberts School of Ocean and Earth Science, National Oceanography Centre, University of Southampton Dr. Joseph M. Magnall Inorganic and Isotope Geochemistry, GFZ German Research Centre of Geosciences Dr. J. Elis Hoffmann Department of Earth Sciences, Freie Universität Berlin Day of defense (Disputationsdatum): 26th of January 2021 Eidesstattliche Erklärung Ich versichere hiermit an Eides Statt, dass diese Arbeit von niemand anderem als meiner Person verfasst worden ist. Alle verwendeten Hilfsmittel wie Berichte, Bücher, Internetseiten oder ähnliches sind im Literaturverzeichnis angegeben, Zitate aus fremden Arbeiten sind als solche kenntlich gemacht. Die Arbeit wurde bisher in gleicher oder ähnlicher Form keiner anderen Prüfungskommission vorgelegt. Die Teile der Arbeit die schon veröffentlicht oder eingereicht wurden, sind im Vorwort (“Preface”) kenntlich gemacht. Weiterhin ist im Vorwort (“Preface”) dargelegt, zu welchem Teil der Arbeit andere Wissenschaftler beigetragen haben. I Acknowledgments To Joe and Sarah, there is so much that I want to thank you for, but most importantly, thanks for always being there to have my back: when I was melting away at >40 °C in the core yard at Mount Isa, when I had to get through the endless home office time this year, when deadlines for abstracts, paper submissions, or presentations came faster than expected, when I just needed to hear ‘it’s okay, you will get there’, and in countless other occasions. You gave me both the guidance and the freedom that I needed. I have learnt so much from you on this journey, both as a scientist and as a person, and I was extremely lucky to have such great supervision. Besides all the things I got to experience and learn throughout the last few years, by far the best was meeting, and becoming friends with, people from all parts of this world. You all left an impression on me, thank you. To the geology teams at Mount Isa Mines Resource Development and at George Fisher, it seems like ages ago when you took me up in your midst. You made me feel welcome, and you shared your experience, your rocks, and your barbecues with me, what more could I have asked for. Amongst everyone else, I would like to thank Alphonse, Dan, Natasha, Nick, Michael, Michelle, Orla, Peter, Ray, Vincent, and William for the great time back in Mount Isa and at George Fisher and for the support even when I was >14 000 km away. To Richard, thanks for getting things started and for giving us the opportunity to come to Mount Isa and to work on those brilliant rocks. One could really tell how much you love that place, thanks for sharing that enthusiasm with us. To all my colleagues at GFZ who helped me to get through this thesis with all the small and big things that you may not have realized at the time. Thanks for the time you shared with me, no matter if it were weeks, months, or years: Alan, Alejandro, Alex, Anja, Bob, Christof, Dang, Franzi, Gregor, Hans-Martin, Haoyang, Hartmut, Haruna, Jess, Johannes, Julia, Kevin, Marcus, Maria, Marta, Marta, Martin, Mengdi, Merilie, Mohammed, Nicole, Oona, Peter, Philipp, Spyros, Svenja, Tine, Uwe, Volker, Yang, and Yufu. II To Mathias, Max, and Malte, thanks for all the fresh air and rehydration breaks, thanks for all the laughs and discussions (both scientific and nonsensical), thanks for being at my side both in euphoric and in hard times, and thanks for turning going to work into meeting some of your best friends. Thanks for letting me be part of your life. To my friends and family, all of you have helped to get me here in one way or another. Thanks for all the laughs, the catch ups, the drinks, the food, the cultural holidays, the times kicking a ball, the chats, and, lately, the zoom or skype calls. All of you are more important to me than I could put in words here. To Vera and Andi, you turned one of the most stressful times of my life into one of the happiest times. Thanks for putting Jakob into my life, I will always be there for him. To Franzi, I do not even know where to start. Thanks for going through this with me. You had to do without many things, and I promise I will not do another PhD thesis. Thanks for being at my side with all your love. Most importantly, to my parents, I cannot imagine where I would be without you. You have always encouraged me to follow my dreams, even when I decided to study rocks and when that took me half a world away from you. You are constantly showing everyone what it means to care for others, to be respectful, to be confident, to be optimistic, and to be great parents. I will always be grateful. Finally, I had thought I will have a party with all of you to thank you for the part you played in my PhD journey and life over the course of the last few years. The virus has, however, made this impossible, or at least very irrational, for a while… So, if you find yourself mentioned above, either directly or indirectly, please feel hereby invited to claim a chat and a beverage of your choosing the next time you see me. III Summary The George Fisher deposit is located in the northern Australian Carpentaria province, which is host to several of the world’s largest Zn and Pb mineral deposits. The annual metal production from George Fisher is crucial in order to meet the global demand for Zn and Pb. The main ore minerals at George Fisher are sphalerite (ZnS) and galena (PbS), which occur in stratabound, and in discordant, massive sulphide ore bodies together with pyrite (FeS2) and pyrrhotite (FeS). These massive sulphide ore bodies are hosted within carbonaceous, pyritic, calcareous, dolomitic siltstones and mudstones of the Paleoproterozoic Urquhart Shale Formation (ca. 1654 Ma), which is also host to two other world class base metal deposits (Mount Isa and Hilton). All three deposits are highly deformed, the textural relationships are complex, and there is a lack of indicator minerals to constrain the metamorphic grade of the Urquhart Shale. As a result, there has been considerable debate over (1) the processes that led to the accumulation of such huge amounts of base metal sulphides in the deposits of the area, and (2) the alteration footprint these processes have produced beyond the massive sulphide zones. In this project, petrographic observations across several scales (drill core logging down to backscatter-electron microscopy) were combined with whole rock, and in situ, mineralogical, geochemical, and isotopic analyses of representative samples from (1) four drill holes that intersected the main ore bodies at George Fisher, and also from (2) a drill hole that intersected the barren Urquhart Shale Formation. These data were collected in order to constrain the background heterogeneity that is inherent to rocks of the Urquhart Shale Formation (e.g., from background diagenetic processes). Using this framework, the nature of some of the hydrothermal processes responsible for ore formation were constrained. Particular emphasis was put on constraining (1) the accumulation processes of reduced sulphur, (2) the ore forming processes, and (3) the mineralogical and geochemical alteration footprint of the George Fisher deposit. In brief, the data from this study suggest that the Urquhart Shale Formation in the location we studied has not undergone regional greenschist metamorphism. The mineralogy and the paleoredox proxies (S-isotope data, Mo concentrations, rare earth IV elements in carbonate minerals) from the barren Urquhart Shale sequence can, therefore, be interpreted in a sedimentary and diagenetic context; and those data concur with deposition of the Urquhart Shale Formation in a ferruginous, marine environment, which is consistent with the current understanding for the Paleoproterozoic oceans. Using this background composition as base line the petrographic, mineralogical, geochemical, and isotopic data from George Fisher suggest that (1) ore formation occurred in multiple events during diagenesis and later deformation, that (2) reduced sulphur in the deposit was likely derived via thermochemical sulphate reduction and the recycling of sulphur from pre-ore diagenetic pyrite, and that (3) fluid-rock interaction of hot (>200-250 °C), saline (Cl-rich), metal-bearing hydrothermal fluids with the Urquhart Shale Formation led to the dolomitization and replacement of pre-ore carbonate and the precipitation of base metal sulphides. Besides ore formation at George Fisher, these hydrothermal processes have resulted in mineralogical and bulk geochemical changes that include (1) albite, chlorite, and calcite depletion, (2) dolomite, phyllosilicate, and sulphide formation, (3) Na and Sr depletion, and (4) Tl and Mn enrichment relative to the barren host rocks. Furthermore, the fluid-rock interaction has led to light rare earth element (LREE) depletion in hydrothermal and hydrothermally altered carbonate minerals relative to whole rock and pre-ore carbonate LREE compositions.
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