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AbstractAbstract
[en] 226Ra, a radioactive decay product of 238U and the most prevalent naturally occurring isotope of radium leads to many environmental issues in various industries due to its half-life of 1600 years: hydrothermal energy, seawater desalination and zircon production among others. The most impacted industries are the extractive ones: shale oil and gas production, coal, phosphate and uranium extraction. 226Ra remains in tailings from U mines and its mobility is controlled by retention mechanisms: sorption on mineral surfaces (iron oxy-hydroxides, phyllosilicates, zeolites) and organic matter, or by the formation of solid solutions (sulfate minerals such as barite and carbonate minerals). The average concentration in lithospheric rocks being 32 Bq/kg, or 1 ppt, the identification of the retention mechanisms of this radionuclide at the scale of the material sampled in the field is made difficult because it is an ultra-trace element. Sequential extractions are commonly used to assess the retention of trace elements, but this technique is subject to experimental and analytical artefacts which are exacerbated in the case of an ultra-trace element. In this work, geochemical modeling of sequential extractions experiments has indeed shown that this technique leads to biased interpretations, particularly in the case of 226Ra which is remobilized during the different extraction steps. In order to have a better understanding of the retention of 226Ra and its distribution in heterogeneous and fine-grained materials, including mine tailings, a new approach has been developed. This approach combines alpha autoradiography, chemical elemental cartographies and mineralogical characterizations obtained on petrographic thin sections. A direct global analysis of the activity of the sample at the petrographic thin section scale is thus possible. This method was first qualified on model samples containing a single synthetic or natural mineral playing an important role in the retention of 226Ra in the natural environment. It was then tested on an assemblage of three of the main minerals responsible for the retention, namely: barite, clay minerals and iron oxy-hydroxides. Finally, it was applied to U-mine tailings. A first set of samples comes from the French post-mining storage sites of Bellezane, where the tailings are stored under a solid cover, and from Bois Noirs Limouzat, which uses a liquid cover. A second set of tailings sample comes from the on-going ore processing facility of McClean Lake, Canada, which uses a tailings neutralization process by barite precipitation. The results show that barite is the main trap of 226Ra via the formation of a solid solution (Ba, Ra)SO4 in all these tailings from different sites. Over a few years, with or without neutralization by barite precipitation, it appears that this solid solution tends towards a recrystallization equilibrium which controls the concentration of 226Ra in solution. These results will subsequently be integrated into reactive transport type modeling to predict the long-term behavior of these tailings. (author)
[fr]
Le 226Ra, descendant radioactif de l'238U et isotope majoritaire naturellement present sur Terre, suscite de nombreuses problematiques environnementales en raison de sa demi-vie de 1600 ans dans des industries variees: hydrothermalisme, desalinisation de l'eau de mer et production de zircon par exemple; mais surtout dans les industries extractives: petrole et gaz de schiste, charbon, phosphate et uranium. Le 226Ra est retenu au sein des residus de traitement des mines d'U et sa mobilite est controlee par les mecanismes de sorption a la surface de mineraux (oxy-hydroxydes de fer, phyllosilicates, zeolithes), ou de la matiere organique ou par la formation de solutions solides (mineraux sulfates comme la barytine et mineraux carbonates). La concentration moyenne dans les roches lithospheriques etant de 32 Bq/kg, soit 1 ppt, l'identification des mecanismes de retention de ce radionucleide a l'echelle du materiau echantillonne sur le terrain est rendue difficile par son caractere ultra-trace. Les extractions sequentielles, technique classique pour le suivi des elements traces, peuvent etre sujettes a de nombreux artefacts exacerbes pour les elements ultra-traces. Dans le cadre de ce travail, une modelisation geochimique d'experiences de lixiviations sequentielles a en effet montre que cette technique conduit a des interpretations biaisees en particulier dans le cas du 226Ra, soumis a de nombreux mecanismes de remobilisation aux differentes etapes de lixiviation. Afin de mieux comprendre les processus de retention du 226Ra et la distribution de celui-ci dans les materiaux heterogenes et finement divises, dont font partie les residus de traitement de l'extraction miniere, une nouvelle approche a ete developpee couplant autoradiographie alpha, cartographies chimiques elementaires et caracterisations mineralogiques obtenues entre autres par MEB/EDS sur lames minces petrographiques. Une analyse globale directe de l'ensemble de l'activite de l'echantillon a l'echelle de la lame mince petrographique est ainsi possible. Cette methode a ete qualifiee tout d'abord sur des echantillons de reference contenant un seul mineral synthetique ou naturel jouant un role important dans la retention du 226Ra en milieu naturel, puis a un assemblage de trois des principaux mineraux responsables de la retention, a savoir: barytine, mineraux argileux et oxy-hydroxydes de fer. Enfin, elle a ete directement appliquee a des residus de traitement. Un premier corpus est issu des sites francais de stockage post-miniers de Bellezane, ou les residus de traitement sont stockes sous couverture solide, et de Bois Noirs Limouzat, qui utilise une couverture liquide. Sont egalement consideres des residus du site en activite de traitement de minerai de McClean Lake, au Canada, qui utilise un processus de neutralisation des residus par precipitation de barytineOriginal Title
Etude de la mobilite du radium-226 en milieu naturel anthropise par approches experimentales et modelisation geochimique
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Source
15 Feb 2022; 344 p; 337 refs.; Available from the INIS Liaison Officer for France, see the INIS website for current contact and E-mail addresses; Geosciences, Ressources Naturelles et Environnement
Record Type
Report
Literature Type
Thesis/Dissertation
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Country of publication
ALKALINE EARTH ISOTOPES, ALPHA DECAY RADIOISOTOPES, CARBON 14 DECAY RADIOISOTOPES, CHARGED PARTICLES, DIMENSIONLESS NUMBERS, DISPERSIONS, EVEN-EVEN NUCLEI, GEOLOGIC DEPOSITS, HEAVY ION DECAY RADIOISOTOPES, HEAVY NUCLEI, HOMOGENEOUS MIXTURES, IONIZING RADIATIONS, ISOTOPES, MINERAL RESOURCES, MINERALS, MIXTURES, NUCLEI, RADIATIONS, RADIOISOTOPES, RADIUM ISOTOPES, RESOURCES, SEPARATION PROCESSES, SIMULATION, SOLID WASTES, SOLUTIONS, SULFATE MINERALS, WASTES, YEARS LIVING RADIOISOTOPES
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