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Formation of Hydrothermal Reephosphate Deposits View metadata, citation and similar papers at core.ac.uk brought to you by CORE provided by Helsingin yliopiston digitaalinen arkisto Formation of hydrothermal REE- phosphate deposits STEFAN S. ANDERSSON ACADEMIC DISSERTATION To be presented, with the permission of the Faculty of Science of the University of Helsinki, for public examination in auditorium D101, Physicum, Kumpula Campus, on May 29 2019, at 12 noon. DEPARTMENT OF GEOSCIENCES AND GEOGRAPHY A76 / HELSINKI 2019 © Stefan S. Andersson (synopsis and Paper III) © Reprinted with permission of Mineralogical Society of America (Paper I) © Reprinted with CC BY license, Elsevier (Paper II) Cover photo: Highly birefringent and fractured xenotime in Djupedal (© Stefan S. Andersson, field of view is 5 mm) Author´s address: Stefan S. Andersson Department of Geosciences and Geography P.O. Box 64 00014 University of Helsinki, Finland [email protected] ([email protected]) Supervised by: Professor Thomas Wagner Institute of Applied Mineralogy and Economic Geology RWTH Aachen University & Department of Geosciences and Geography University of Helsinki Dr. Erik Jonsson Department of Mineral Resources Geological Survey of Sweden & Department of Earth Sciences Uppsala University Reviewed by: Professor Martin Smith School of Environment and Technology University of Brighton Priv.-Doz. Dr. Michael Marks Department of Geosciences University of Tübingen Opponent: Professor emeritus Ulf Hålenius Swedish Museum of Natural History ISSN-L 1798-7911 ISSN 1798-7911 (print) ISBN 978-951-51-4915-2 (paperback) ISBN 978-951-51-4916-9 (PDF) http://ethesis.helsinki.fi Unigrafia Helsinki 2019 The Faculty of Science uses the Urkund system (plagiarism recognition) to examine all doctoral dissertations. DEPARTMENT OF GEOSCIENCES AND GEOGRAPHY A Andersson S.S., 2019. The formation of hydrothermal REE-phosphate deposits. Unigrafia. Helsinki. 53 pages, 4 tables and 7 figures. Abstract Rare earth elements (REE) are important CaCl2-HF-H2O fluids at high temperatures of metals used in green and low-carbon energy and ~600 °C at c. 1.8 Ga. Subsequently, the ore as- information technologies and are widely used semblages were variably modified during cool- for geological petrogenetic studies. It is becom- ing by CaCl2-NaCl to NaCl-CaCl2 brines, and ing increasingly evident that the REE can be partly, CO2-rich fluids down to temperatures of mobile in certain hydrothermal fluids and even ~300 °C and to at least 1.75 Ga. form hydrothermal REE deposits. This study fo- Hydrothermal REE deposits rich in REE- cuses on the formation of hydrothermal REE phosphates are commonly associated with deposits rich in the REE-phosphates (monazite alkaline magmatism, particularly in silicate- [(LREE,Y)PO4] and xenotime [(Y,HREE)PO4]). carbonatitic systems. This is because REE The main objective of the study was to char- and P both exhibit strong chemical affinities acterise the Olserum-Djupedal REE-phosphate with carbonatitic systems and the potential mineralisation in SE Sweden. Based on this, the for mobilisation of REE and P are high. This study evaluates different sources of REE and P study shows that REE deposits can also form in hydrothermal deposits and assesses how REE by hydrothermal activity related to subalkaline and P are transported in hydrothermal fluids. To magmatic rocks. Peraluminous granites exhibit characterise the Olserum-Djupedal REE miner- the greatest potential to exsolve fluids carrying alisation, this study combines fieldwork, petro- REE and P, which can lead to the formation graphical and textural analysis, major and trace of hydrothermal REE deposits rich in REE- element mineral chemistry of REE-bearing min- phosphates. erals and the main gangue phases, stable Cl iso- The general understanding on how hydro- topic and halogen analysis of fluorapatite, and thermal REE-phosphate deposits form is that fluid inclusion microthermometry and LA-ICP- REE and P are transported in separate fluids MS analysis. and that the REE-phosphates form when these The primary Olserum-Djupedal REE miner- two fluids mix, or the REE-phosphates form alisation comprises co-existing monazite-(Ce), when REE-bearing fluids interact with P-rich xenotime-(Y) and fluorapatite. These occur main- rocks. The lack of rocks pre-enriched in P in ly within veins dominated by biotite, magnetite, the Olserum-Djupedal district and the gedrite and quartz forming within metasedimen- co-crystallisation of fluorapatite, monazite-(Ce) tary rocks in or close to the contact aureole of a and xenotime-(Y), however, suggest that such peraluminous alkali feldspar granite. The veins scenarios not necessarily account for all occur- are also hosted by the granite within the outer- rences of hydrothermal REE-phosphate depos- most part of this granite. Primary REE-miner- its. As an alternative, REE and P can have been als formed by granitic-derived NaCl-FeCl2-KCl- transported by the same fluid. This study dem- 4 onstrates that the most probable conditions for temperature hydrothermal systems, the interac- co-transport of REE and P are at temperatures tion of REE-bearing fluids with P-rich rocks or exceeding 400 °C and with increasing salinity fluids is probably the most efficient mechanism of the fluids, conditions that agree well with that for precipitating REE-phosphates. In high-tem- of the Olserum-Djupedal system. The most perature magmatic-hydrothermal systems, REE effective co-transport of REE and P would and P probably share a common origin and were occur at acidic conditions by REE-Cl, REE- transported by the same fluid. In such systems, F or REE-SO4 complexes. Yet, co-transport of pH changes, cooling and the destabilisation of the REE and P may also be feasible at neutral to alka- chief REE transporting complexes jointly con- line conditions by REE-OH complexes. In low- tribute to the precipitation of REE-phosphates. 5 DEPARTMENT OF GEOSCIENCES AND GEOGRAPHY A Svensk sammanfattning De sällsynta jordartsmetallerna (på engelska för- Hydrotermala mineraliseringar med REE- kortat REE; Rare Earth Elements) är en grupp fosfater förknippas vanligtvis med alkalina grundämnen som idag har en nyckelroll i mån- magmatiska bergarter och karbonatiter eftersom ga högteknologiska applikationer inklusive s.k. både REE och P i regel uppvisar en stark kemisk grön och fossilfri energiteknik. Över tid har flera affinitet till sådana magmor. Den här studien REE-mineraliseringar konstaterats ha bildats helt visar att REE-fosfatförekomster även kan bildas eller delvis av hydrotermala fluider (högtemper- av hydrotermal aktivitet relaterad till magmatiska erade vattenlösningar). Hur sådana förekomster bergarter av betydligt mindre alkalin karaktär. Av kan bildas är ett idag högaktuellt forskningsom- dessa system så har graniter med peraluminös råde. Den här studien är fokuserad på bildan- karaktär störst potential att avge fluider anrikade det av hydrotermala REE-förekomster inne- på både REE and P. hållande REE-fosfaterna monazit [(LREE,Y) Den generella uppfattningen om hur hydro- PO4] och xenotim [(Y,HREE)PO4], två viktiga termala REE-fosfatmineraliseringar har bildats värdmineral för REE i jordskorpan. Studien in- är att REE och P transporterats i separata flu- riktar sig främst på att karakterisera de nyup- ider och att REE-fosfater fällts ut som en kon- ptäckta REE-mineraliseringarna i området kring sekvens av att dessa fluider blandats, eller att Olserum-Djupedal utanför Västervik i sydöstra REE-fosfater bildats som ett resultat av att Sverige. Fortsättningsvis undersöks ursprunget REE-förande fluider reagerat med fosforrika av REE och P i dessa förekomster, hur REE och bergarter. Avsaknaden av fosforrika bergarter i P transporteras i de hydrotermala lösningarna och området kring Olserum-Djupedal och förekom- vilka processer som lett fram till bildandet av sten av samexisterande fluorapatit, monazit-(Ce) monazit och xenotim från dem. och xenotim-(Y) visar dock att sådana scenarier Den primära mineraliseringen i Olserum- inte nödvändigtvis förklarar alla förekomster av Djupedal domineras av samexisterande monazit- hydrotermala REE-fosfatmineraliseringar. Som (Ce), xenotim-(Y) och REE-förande fluorapatit i ett alternativ kan REE och P ha transporterats gångar huvudsakligen bestående av biotit, mag- i samma fluid. De mest troliga förhållanden för netit, gedrit och kvarts. Gångarna förekommer samtransport av REE och P är i fluider med tem- i metasedimentära bergarter kring och i kontak- peraturer som överstiger 400°C och som har höga tgården till en peraluminös alkalifältspatgranit. salthalter. Vidare så gynnar låga pH samtrans- Gångarna uppträder även i utkanten av samma port av REE och P då olika metallkomplex med granit. Sammantaget visar resultaten att den REE, exempelvis REE-Cl, REE-F eller REE- primära REE-mineraliseringen har ett hydroter- SO4, är väldigt stabila under dessa förhållanden. malt ursprung och bildades för omkring 1,8 mil- Samtransport av REE och P är också möjlig vid jarder år sedan av högtempererade (ca. 600°C) ett mer neutralt eller basiskt pH. I ett scenario fluider från den närliggande graniten. De primära som innefattar samtransport av REE och P så associationerna omvandlades därefter under kan pH-förändringar, sänkta temperaturer och avtagande temperatur till ca. 300°C för åtmin- destabilisering av viktiga REE-metallkomplex i stone 1,75 miljarder år sedan. kombination bidra till utfällning av REE-fosfater. 6 Sammanfattningsvis kan man säga att i låg- fosforrika bergarter. I många högtempererade tempererade hydrotermala system har REE- magmatisk-hydrotermala
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