Mineralization of Nickel in Saprolitic Ore of New Caledonia: Dynamics of Metal Transfer and Modeling of Coupled Geochemical and Hydrodynamic Processes Andrey Myagkiy

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Mineralization of Nickel in Saprolitic Ore of New Caledonia: Dynamics of Metal Transfer and Modeling of Coupled Geochemical and Hydrodynamic Processes Andrey Myagkiy Mineralization of Nickel in saprolitic ore of New Caledonia: Dynamics of metal transfer and modeling of coupled geochemical and hydrodynamic processes Andrey Myagkiy To cite this version: Andrey Myagkiy. Mineralization of Nickel in saprolitic ore of New Caledonia: Dynamics of metal transfer and modeling of coupled geochemical and hydrodynamic processes. Earth Sciences. Université de Lorraine, 2017. English. NNT : 2017LORR0277. tel-01909333 HAL Id: tel-01909333 https://hal.univ-lorraine.fr/tel-01909333 Submitted on 9 Dec 2019 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. AVERTISSEMENT Ce document est le fruit d'un long travail approuvé par le jury de soutenance et mis à disposition de l'ensemble de la communauté universitaire élargie. Il est soumis à la propriété intellectuelle de l'auteur. Ceci implique une obligation de citation et de référencement lors de l’utilisation de ce document. D'autre part, toute contrefaçon, plagiat, reproduction illicite encourt une poursuite pénale. Contact : [email protected] LIENS Code de la Propriété Intellectuelle. articles L 122. 4 Code de la Propriété Intellectuelle. articles L 335.2- L 335.10 http://www.cfcopies.com/V2/leg/leg_droi.php http://www.culture.gouv.fr/culture/infos-pratiques/droits/protection.htm UNIVERSITÉ DE LORRAINE GeoRessources - RP2E Thèse Présentée en vue d’obtenir le grade de DOCTEUR DE L’UNIVERSITÉ DE LORRAINE spécialité “Géosciences” par Andrey MYAGKIY Mineralization of Nickel in saprolitic ore of New Caledonia: Dynamics of metal transfer and modeling of coupled geochemical and hydrodynamic processes Thèse soutenue publiquement le 08/12/2017 devant le jury composé de : Mme. Cécile Quantin Professeur, Université Paris-Sud Rapporteur M. Vincent Lagneau Professeur, MINES ParisTech Rapporteur Mme. Martine Buatier Professeur, Université de Franche-Comté Examinatrice M. Jean-Paul Ambrosi Chargé de recherche, CEREGE Examinateur Mme. Marie-Odile Simonnot Professeur, LRGP Examinatrice vM. Fabrice Golfier Maître de conférences, Université de Lorraine Directeur M. Laurent Truche Professeur, Université Grenoble Alpes Co-directeur M. Michel Cathelineau Directeur de recherche, Université de Lorraine Co-directeur Laboratoire GeoRessources - ENSG, Rue du Doyen Marcel Roubault, 54518 VANDOEUVRE-LES-NANCY CEDEX. Acknowledgements irst and foremost, I would like to express my sincere gratitude to my three directors - F Fabrice GOLFIER, Laurent TRUCHE and Michel CATHELINEAU for motivation, for our friendship, and for all that work we made together. You were my mentors, my guides and provided me with everything for my scientific and personal growth. I couldn’t have done it without you. I would also like to thank my jury - Cécile Quantin, Vincent Lagneau, Martine Buatier, Jean-Paul Ambrosi and Marie-Odile Simonnot for accepting to evaluate my work, for your valuable comments and suggestions, and fruitful discussion. I am very grateful to you. I should also note that this work would not be possible without financial support of the French National Research Agency through the national program "Investissements d’avenir" with the reference ANR-10-LABX-21-01 / LABEX RESSOURCES21. Last but not least, I would like to thank my parents, my sister and all my good friends. Words can not express how grateful I am to my mom and my dad for all their sacrifices that they have made sending me first to Moscow from a little town in the south of Russia, and then to France. Thank you to you all! Yours sincerely, Andrey February 2, 2018. iii Résumé e nombreux travaux récents ont enrichi la connaissance des conditions de formations D d’enrichissement en Ni des latérites développées sur roches ultrabasique (Golightly, 2010; Butt and Cluzel, 2013; Freyssinet et al., 2005; Cluzel and Vigier, 2008; Cathelineau et al., 2016b,a; Villanova-de-Benavent et al., 2014; Quesnel et al., 2017). Dans le cas de la Nou- velle Calédonie, comme dans le cas de gisements équivalents à l’échelle mondiale (Cuba, République Dominicaine, Indonésie) (Fig. 1), le modèle principal de genèse des enrichisse- ments en Ni est basé sur le concept de développement de la latérite, où les éléments comme Si, Mg sont expulsés et lixiviés, tandis que le sol résiduel est enrichi dans tous les métaux insolubles (Fe, Al, Cr). L’enrichissement en Ni est beaucoup plus complexe à interpréter car il ne correspond pas à un enrichissement résiduel s.s., le niveau enrichi n’étant pas situé dans les latérites jaunes et rouges (soit les principaux horizons résiduels), mais dans la saprolite surmontant le bedrock. Figure 1 – Global distribution of Ni resources (Butt, 2007). Laterite-Nickel Ore deposits are presented in Cuba, New Caledonia, Indonesia, Philippines, Burma, Vietnam, Brazil and Nickel Sulphide Ore deposits - in Canada, Russia, Australia, China, South Africa, etc. L’objectif principal de ce travail est de proposer et tester un modèle conceptuel qui tient v compte des observations les plus récentes des différents types de minerais. La thèse cherche à détailler le rôle relatif des paramètres physico-chimiques qui régissent les principaux processus de dissolution-reprécipitation et d’adsorption qui contrôlent les enrichissements en Ni. Il a été réalisé dans le cadre des actions de modélisation du transport - réactif mené dans le cadre du labex Ressources 21. Contexte et approche Les travaux menés partent sur la modélisation du transport réactif dans le contexte de la formation d’un profil latéritique se développant sur roche ultra-basique. Un des premiers travaux publiés dans ce domaine est celui de Domenech et al (2017), mais il est restreint au rôle de l’adsorption, et de la formation des oxy-hydroxydes. Le concept des modélisa- tions réalisées dans le cadre de la thèse est basé sur le développement: i) d’un modèle 1D puissant dont l’objectif est de traiter le comportement géochimique du Nickel au cours de l’altération progressive de la péridotite, en comparant les évolutions modélisées avec celles observées sur le terrain, et s’intéressant en particulier à la mobilité spécifique et relative des éléments en traces comme les métaux, et ii) d’un modèle 2D thermo-hydro-chimique qui donne un nouvel éclairage sur le rôle des discontinuités et les différents paramètres contrôlant l’hydrodynamique des aquifères situés au dessus du bedrock (rôle du relief, topographie de l’interface saprolite-bedrock, impact des fractures et des réseaux de discontinuités). Les minerais en Nouvelle Calédonie peuvent se classer en deux grands types distincts : les minerais oxydés constitués essentiellement d’oxy-hydroxydes de fer, de chromites résiduelles et de faibles quantités d’argiles , et les minéraux silicates constitués principalement de sili- cates résiduels non encore totalement dissous (olivine , pyroxène, serpentine) et de silicates néoformés (talc-like ou kérolite, rarement de la sépiolite, des smectites de type nontronite dans certains profiles particuliers). Le nickel peut être présent sous différentes formes : i) adsorbé sur des sites faibles ou forts sur la goethite, ii) incorporé dans le réseau cristallin de la goethite (Fe, Ni) O-OH, ou encore précipité dans des silicates néoformés. Les simu- lations ont été réalisées en utilisant le code géochimique PHREEQC et la base de données thermodynamique de LLNL (llnl.dat) , avec des calculs spécifiques réalisés afin de disposer de données sur la "garniérite", soit les silicates composés potentiellement de talc-like (série kérolite-pimélite), et localement de sépiolite. Le modèle 2D a été réalisé en utilisant une in- terface, nommée iCP, qui permet de couper les processus physiques dans COMSOL avec des calculs géochimiques dans PHREEQC, ceci permettant de fusionner les capacités des deux codes dans un seul. vi Résultats Modèle 1D de transport-réactif. Le premier modèle développé consiste en une étude détaillée de la formation des minéraux néoformés le long du profil d’altération, en particulier en fonction de la migration vers le bas du front de dissolution et d’altération des minéraux de la péridotite. Le travail a consisté a calculer et représenter : i) la formation d’une latérite sur une longue période de temps (10 Ma), ii) la mobilité des éléments et évaluer les facteurs qui contrôlent cette mobilité, iii) comparer les profils modélisés avec ceux rencontrés sur les sites naturels, iv) les processus de rétention. Le mécanisme principal de transfert puis de rétention du Nickel s’avère contrôlé par la compétition entre les processus d’adsorption et d’incorporation dans le réseau de la goethite, puis la formation des silicates nickélifères (kérolite/ sépiolite). Cette modélisation tient compte de l’ensemble des principaux processus de rétention du Nickel et démontre que la formation et l’épaississement de la zone enrichie en Ni est gouvernée par la progres- sion du front pH. Le mécanisme principal de rétention du nickel dans la zone limonitique (latérite jaune des mineurs) est son incorporation dans le réseau de la goethite, les mécan- ismes d’adsorption n’étant que transitoires. Il est à noter que les travaux de lixiviation
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