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Concentration and Fractionation of Rare Earth Elements in Alkaline Complexes : the Role of Fluids Cyrielle Bernard

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Concentration and Fractionation of Rare Earth Elements in Alkaline Complexes : the Role of Fluids Cyrielle Bernard Concentration and fractionation of Rare Earth Elements in alkaline complexes : the role of fluids Cyrielle Bernard To cite this version: Cyrielle Bernard. Concentration and fractionation of Rare Earth Elements in alkaline complexes : the role of fluids. Hydrology. Université Paul Sabatier - Toulouse III, 2020. English. NNT: 2020TOU30187. tel-03179382 HAL Id: tel-03179382 https://tel.archives-ouvertes.fr/tel-03179382 Submitted on 24 Mar 2021 HAL is a multi-disciplinary open access L’archive ouverte pluridisciplinaire HAL, est archive for the deposit and dissemination of sci- destinée au dépôt et à la diffusion de documents entific research documents, whether they are pub- scientifiques de niveau recherche, publiés ou non, lished or not. The documents may come from émanant des établissements d’enseignement et de teaching and research institutions in France or recherche français ou étrangers, des laboratoires abroad, or from public or private research centers. publics ou privés. THÈSETHÈSE En vue de l’obtention du DOCTORAT DE L’UNIVERSITÉ DE TOULOUSE Délivré par : l’Université Toulouse 3 Paul Sabatier (UT3 Paul Sabatier) Présentée et soutenue le 23 octobre 2020 par : Cyrielle BERNARD Concentration et fractionnement des Terres Rares dans les complexes alcalins : le rôle des fluides JURY Kathryn GOODENOUGH British Geological Survey Rapportrice Alexandre TARANTOLA Université de Lorraine Rapporteur Michel GRÉGOIRE Université Toulouse 3 Examinateur Anne-Sylvie ANDRÉ-MAYER Université de Lorraine Examinatrice Didier BÉZIAT Université Toulouse 3 Directeur de thèse Guillaume ESTRADE Université Toulouse 3 Co-directeur de thèse Stefano SALVI Université Toulouse 3 Invité Julien BERGER Université Toulouse 3 Invité École doctorale et spécialité : SDU2E : Sciences de la Terre et des Planètes Solides Unité de Recherche : Géosciences Environnement Toulouse (UMR5563) Directeurs de Thèse : Didier BÉZIAT, Guillaume ESTRADE et Stefano SALVI iii Acknowledgements Although this manuscript is written in English, you will have to forgive me but I would like to thank everyone who accompanied me during these three years in French, my native language. J’adresse tout d’abord un immense merci à mes encadrants, MM. Guillaume Estrade, Stefano Salvi et Didier Béziat. Guillaume, pour ton guidage constant, depuis les couloirs labyrinthiques de l’OMP lors de notre première rencontre jusqu’à l’aboutissement de ce manuscrit, tu m’as permis de trouver la sortie sans me brûler les ailes. Stefano, pour avoir toujours trouvé du temps pour moi, même au beau milieu d’une pandémie, entre un HDR, un conseil de laboratoire et 3 articles à relire. Et Didier, pour tes conseils avisés, même après la retraite : vers l’infini et au-delà ! Je remercie beaucoup Kathryn Goodenough et Alexandre Tarantola pour avoir accepté d’être les rapporteurs de ce travail. Votre lecture attentive et vos commentaires ont permis d’améliorer la version finale de ce travail de longue haleine. Je remercie également les nombreuses personnes qui contribué à la bonne réalisation des analyses dans ce travail. Merci à Philippe de Parseval et Sophie Gouy pour leur implication et leur curiosité constante sur mon travail. Merci aussi à Thierry Aigouy pour son aide et sa réactivité lors des séances MEB, pour le meilleur et pour le pire (!). Merci également à Fabienne de Parseval pour la fabrication des lames minces sur lesquelles j’ai passé tant d’heures. Merci à David Chew et Foteini Drakou du Trinity College, Irlande, pour leur aide dans la réalisation de cartographies ICPMS. Merci à Chris Harris de l’Université de Cape Town, Afrique du Sud, ainsi que Etienne Deloule, Gaston Giuliani, Michel Champenois et Nordine Bouden du CRPG Nancy pour les analyses isotopiques. J’aimerais également remercier toutes les personnes qui m’ont aidée ponctuellement dans mes analyses : Sabine Choy pour l’accompagnement au broyage et à la séparation magnétique de mes roches, François Martin pour les analyses Mössbauer des pyroxènes, Claudie Josse et Teresa Hungria pour les observations MET dans ces mêmes pyroxènes, Yves Auda pour son accompagnement patient dans l’écriture iv du programme informatique pyroxènes, Corinne Routaboul pour les analyses de spectroscopie infrarouge sur les elpidites, Franck Poitrasson pour son aide à propose d’Evisa, et Aurélie Marquet pour les analyses LA-ICPMS. J’adresse ma gratitude à Marc de Rafélis pour son tutorat en tant qu’enseignant. Enfin, j’aimerais remercier Margot Munoz, Loïc Drigo, Carine Baritaud et Anne-Marie Cousin qui, même sans être directement connectés à mon doctorat, ont toujours été disponibles et souriants en toute situation. Un doctorat ne peut s’effectuer sans compagnons de route avec qui partager les bons et les moins bons moments. J’ai eu la chance de partager un bureau international et soudé avec Salomé, Aruã, Gina et Benjamin. Merci pour votre bonne humeur, le bureau H137 n’a pas fini d’entendre des discussions passionnées la bouche pleine de gâteaux ! J’adresse une pensée particulière à Salomé : nous avons commencé notre thèse en même temps et, quelques guacamoles plus tard, nous la finissons ensemble. Je remercie également Steven et Gaétan qui m’ont, entre autres, suivie dans la folle aventure du Student Chapter. Nos péripéties espagnoles défilent dans ma tête... à une vitesse plus ou moins raisonnable ! Je remercie aussi Adrien, stagiaire devenu camarade par son sérieux et sa gentillesse. Merci également à tous ceux que j’ai côtoyés le temps d’une discussion ou d’un café : Anissa, Dahédrey, Sylvain, Rémi, Paty, Beatriz, Loïs, Vianney, et les autres. Enfin, merci à ceux qui étaient là avant : Samuel, mon jumeau semi-géologue; Aurélie, qui j’en ai bien peur ne comprendra jamais ma passion pour "les cailloux"; et Guilhem et Stellina, les meilleurs colocataires que l’on puisse souhaiter. Je ne peux évidement pas conclure ces remerciements sans envoyer une vague de gratitude à ma famille. Merci à mes parents, Nicole et Frédéric, qui ont cru en moi depuis le tout début. Vous avez été présents à chaque nouvelle étape de ma vie, encourageants et fiers quoi qu’il arrive. Vous m’avez donné les moyens de naviguer par moi-même dans ce monde et pour ça je ne vous remercierai jamais assez. Merci à mes sœurs, Candice et Lucile. Vous êtes le moteur qui me permet d’avancer, et je suis fière de vous. Enfin, merci à toi Nicolas, qui m’accompagne depuis déjà bien trop longtemps. Ton soutien indéfectible m’a permis d’aller plus loin que jamais. v Abstract The rare earth elements (REE) are critical resources used in many modern technologies, including high tech and renewable energy infrastructure. Their worldwide production is currently mostly restricted to China and Australia. The REE are divided in two groups, i.e. light REE (LREE, La-Eu) and heavy REE (HREE, Gd-Lu), the latter being rarer and with more industrial uses. REE deposits can be primary high temperature (igneous, carbonatites and alkaline systems) or secondary low temperature (placers and ion-adsorption). Type and grade of REE resources depends on many parameters including primary igneous source, magmatic processes, hydrothermal fluids circulation, and/or weathering. Among primary high temperature deposits, alkaline granites and associated pegmatites are the richest in HREE. Although it is accepted that magmatic processes are fundamental in concentrating the REE, the role of hydrothermal fluids in concentrating and fractionating these elements remains unclear. This manuscript investigates the importance and characteristics of hydrothermal fluids in concentrating and fractionating the REE relatively to magmatic and source processes. To do so, petrography and fluid inclusions are studied in six alkaline complexes worldwide, namely Amis (Namibia), Evisa (Corsica), Khan Bogd (Mongolia), Strange Lake (Canada), and Ambohimirahavavy and Manongarivo (Madagascar). The comparison of these complexes allows to draw general conclusions about REE enrichment and fractionation in alkaline complexes. This study shows that the main mineralogy is similar in all complexes and is made of quartz, alkali feldspar, Na-amphiboles, aegirine, and a complex zirconosilicate (elpidite or an eudialyte-group-mineral, EGM). Despite local variations, many accessory minerals are also common to most of these alkaline complexes, such as pyrochlore-group-minerals, zircon, and Fe and/or Ti-oxides. Amphibole, EGM, elpidite and feldspars grew exclusively during magmatic stage. Quartz and aegirine are zoned and grew from magmatic to hydrothermal stages; feldspars and primary zirconosilicates got hydrothermally altered. Primary vi zirconosilicates are commonly replaced by an assemblage of secondary minerals forming pseudomorphs. They present a wide variety of chemistries (silicates, oxides, halides, carbonates, phosphates). The detailed study of zoning and alteration of amphiboles and aegirine, which is the topic of a published paper, shows that hydrothermal fluids do mobilize and fractionate the REE. A quantitative estimation confirms their high importance compared with magmatic processes. A similar study of zircon highlights the local influence of these processes, as the REE composition of zircon in pseudomorphs depends on the REE composition of the replaced mineral. These observations point out the importance of studying rock-forming minerals such as pyroxenes and amphiboles to unravel geological events controlled by common processes. Composition and origin of hydrothermal fluids is explored through microthermometric and SEM studies of fluid inclusions in quartz of the six complexes. They reveal that although their salinity varies a lot, fluids circulate at a relatively low temperature (< 400 ◦C). All investigated complexes experienced the circulation of at least two fluids, one Na- and K-rich, and one Ca- and Na-rich. At the Malagasy complexes and Strange Lake, it has been established that the Na-K-bearing fluid is orthomagmatic and the Ca-Na-bearing one is secondary. In conclusion, this work shows that REE enrichment and fractionation in alkaline granites and associated pegmatites is linked to the circulation of a Na-K-rich and a Ca-Na-rich fluid, at temperatures below 400 ◦C. This fluid contains REE ligands such as F, OH, Cl that fractionate the REE.
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