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In Tropical Iron Ore Systems Alan Levett B.Sc. H. Majoring in Geological

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In Tropical Iron Ore Systems Alan Levett B.Sc. H. Majoring in Geological Development of ferruginous duricrusts (canga) in tropical iron ore systems Alan Levett B.Sc. H. Majoring in Geological Sciences (UQ) 2014 B.Sc. Extended Major in Biomedical Sciences (UQ) 2011 A thesis submitted for the degree of Doctor of Philosophy at The University of Queensland – 2020 School of Earth and Environmental Sciences Abstract Iron-rich duricrusts (canga) that cap iron ore deposits in Brazil evolve by the redox-based cycling of iron oxide minerals, continually forming new iron-rich cements that effectively prevent the physical erosion of these landforms. This thesis aimed to understand the biological influences on the geochemical cycling of iron within canga, to determine if these processes could be used to accelerate iron cement formation, for example, in a post-mining context. Re- cementing waste material (canga) from iron ore mining may provide an environmentally- friendly solution for iron ore mine remediation in Brazil and the restoration of a rare ecosystem associated with canga outcrops. Field emission scanning electron microscopy revealed an array of microorganisms fossilised within canga, highlighting the innate role of microorganisms in the evolution of canga horizons. Nanoscale elemental mapping of these microfossils revealed a role for aluminium in the long-term preservation of organic and inorganic biosignatures. A suite of high-resolution analytical techniques were correlated to understand the fossilisation processes that contribute to biosignature preservation in near-neutral iron-rich environments. Further investigation of the microfossils in canga, revealed the complex weathering patterns induced by microorganisms. Grains within canga could be completely weathered and texturally replaced by microfossils; only remnants of the grain’s shape and traces of most immobile elements (for example, thorium) were left behind. The minor and trace element proportions of the canga cements revealed the microscale redistribution of titanium, likely to be driven by microorganisms, and the long-range redistribution of phosphorus, both preserved within these iron-rich duricrusts. Aeolian phosphorus from Africa appears to provide an external phosphorus source for the canga-associated ecosystems. As part of fieldwork in the montane regions of Northern Brazil, a lake-edge microbial ecosystem where canga cements appeared to form relatively rapidly was characterised. Examining these rocks, fossilised biofilms were found to play an intricate role in the formation of the meniscus-type cements within canga. Without the organic framework provided by microbial biofilms, and connecting grains together, the iron oxide minerals would simply have enlarged the existing grains without making cements. Armed with new information revealing the microbiome in canga plays an important role in the dissolution and the re-precipitation of iron oxides, these processes were applied to accelerate the reformation of iron-rich crusts in the laboratory. Microbially-mediated iron reduction was promoted within an open-air bioreactor and the iron-rich solutions were allowed to flow over crushed canga on a slope of approximately 10. Astonishingly, within 6 months the top 3 – 5 cm of the experiment had i been stabilised by fossilisation of the microbial biofilms that naturally aggregate materials. This experiment is a platform for field-scale trial aiming to progressively stabilise the slope of an expended mine site. Understanding and harnessing microbial processes that contribute to iron cement formation in canga offers an alternative remediation strategy for iron ore mines in Brazil. ii Declaration by author This thesis is composed of my original work, and contains no material previously published or written by another person except where due reference has been made in the text. I have clearly stated the contribution by others to jointly-authored works that I have included in my thesis. I have clearly stated the contribution of others to my thesis as a whole, including statistical assistance, survey design, data analysis, significant technical procedures, professional editorial advice, and any other original research work used or reported in my thesis. The content of my thesis is the result of work I have carried out since the commencement of my research higher degree candidature and does not include a substantial part of work that has been submitted to qualify for the award of any other degree or diploma in any university or other tertiary institution. I have clearly stated which parts of my thesis, if any, have been submitted to qualify for another award. I acknowledge that an electronic copy of my thesis must be lodged with the University Library and, subject to the policy and procedures of The University of Queensland, the thesis be made available for research and study in accordance with the Copyright Act 1968 unless a period of embargo has been approved by the Dean of the Graduate School. I acknowledge that copyright of all material contained in my thesis resides with the copyright holder(s) of that material. Where appropriate I have obtained copyright permission from the copyright holder to reproduce material in this thesis. iii Publications during candidature Peer-reviewed Journal Articles: Levett, A., Gagen, E.J., Shuster, J., Rintoul, L., Tobin, M., Vongsvivut, J., Bambery, K., Vasconcelos, P., Southam, G. (2016) Evidence of biogeochemical processes in iron duricrust formation. Journal of South American Earth Sciences, 71, 131-142. Gagen, E.J., Levett, A., Shuster, J., Fortin, D., Vasconcelos, P., Southam, G. (2018) Microbial diversity in actively forming iron oxides from weathered banded iron formation systems. Microbes and Environments, 33, 385-393. Spier, C.A., Levett, A., Rosière, C.A. (2018) Geochemistry of canga (ferricrete) and evolution of the weathering profile developed within itabirite and iron ore in the Quadrilátero Ferrífero region, Minas Gerais, Brazil. Mineralium Deposita, 54, 983-1080. Levett, A., Gagen, E.J., Diao, H., Guagliardo, P., Rintoul, L., Paz, A., Vasconcelos, P.M., Southam, G. (2019) The role of aluminium in the preservation of microbial biosignatures. Geoscience Frontiers, 10, 1125-1138. Gagen, E.J., Levett, A., Paz, A., Cecilio, C.F., Southam, G., Oliveira, G., Siqueira, J., Bittencourt, J., Gastauer, M., Vasconcelos, P., Valadares, R., Alves, R. (2019) Biogeochemical processes in canga ecosystems: protection of iron ore and importance in iron duricrust restoration in Brazil. Ore Geology Reviews, 107, 573-586. Levett, A., Gagen, E.J., Southam, G. (2019). Small but mighty: microorganisms offer inspiration for iron ore remediation and mine waste stabilisation. Microbiology Australia, 40, 190-194. Paz, A., Gagen, E.J., Levett, A., Zhao, Y., Kopittke, P.M., Southam, G. (2020) Biogeochemical cycling of iron oxides in the rhizosphere of plants grown on ferruginous duricrust (canga). Science of the Total Environment, 713, 136637. Levett, A., Gagen, E.J., Vasconcelos, P.M., Zhao, Y., Paz, A., Southam, G. (2020) Biogeochemical cycling of iron: implications for biocementation and slope stabilisation. Science of the Total Environment, 707, 136128. Levett, A., Vasconcelos, P.M., Gagen, E.J., Rintoul, L., Spier, C.A., Guagliardo, P., Southam, G. (2020) Microbial weathering signatures in lateritic ferruginous duricrusts. Earth and Planetary Science Letters 538, 116209. iv Conference Abstracts: Levett, A., Gagen, E.J., Southam, G. (2019) Microorganims promote hillslope stabilisation and mine waste stabilisation. Australian Microbial Ecology Conference (AusME), Western Australia, February 11-13. Paz, A., Gagen, E.J., Levett, A., Southam, G. (2019) Evidence of primary surface colonizers on iron duricrust (canga) in Carajás, Brazil. Australian Microbial Ecology Conference (AusME), Western Australia, February 11-13. Paz, A., Gagen, E.J., Levett, A., Southam, G. (2019) Biogeochemical cycling of iron oxide in the rhizosphere of plants grown on ferruginous duricrust (canga) in Carajás, Brazil. Goldschmidt, Barcelona, 18-23 August. Levett, A., Paz, A., Gagen. E.J., Diao, H., Guagliardo, P., Rintoul, L., Vasconcelos, P., Southam, G. (2018) The role of aluminium in microbial fossilisation and preservation of organic biosignatures. Gordon Research Conference: Geobiology, Galveston, Texas, USA. January 21-26. Levett, A., Paz, A., Gagen. E.J., Diao, H., Guagliardo, P., Rintoul, L., Vasconcelos, P., Southam, G. (2017) Preservation of organic and inorganic biosignatures in iron oxide mineralised microfossils. The 23rd International Symposium for Environmental Biogeochemistry, Cairns, Australia. September 25-29. Levett, A., Gagen, E.J., Shuster, J., Paz, A., Southam, G. (2016) Iron oxide diagenesis: the role of iron-oxidising bacteria. The 26th Annual V.M. Goldschmidt Conference, Yokohama, Japan, June 26-July 1. Southam, G., Gagen, E.J., Levett, A., Monteiro, H., Paz, A., Vaconcelos, P. (2016) The importance of iron duricrust formation to Brazil iron ore production. The 26th Annual V.M. Goldschmidt Conference, Yokohama, Japan, June 26-July 1. Gagen, E.J., Levett, A., Shuster, J., Monteiro, H., Rintoul, L., Tyson, G., Vasconcelos, P., Southam, G. (2015) Biogeochemical cycling of iron in canga ecosystems. Gordon Research Conference: Applied and Environmental Microbiology. South Hadley, USA. July 12–17. v Accepted publications included in thesis Levett, A. Gagen, E.J., Diao, H., Guagliardo, P., Rintoul, L., Paz, A., Vasconcelos, P.M., Southam, G. (2019) The role of aluminium in the preservation of microbial biosignatures. Geoscience Frontiers,
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