Assessment of 226Ra and U colloidal transport in a mining environment

Marine Reymond; Michaël Descostes; Clémence Besançon; Martine Leermakers; Sophie Billon; Gaël Cherfallot; Marie Muguet; Catherine Beaucaire; Vendula Smolíková; Patricia Patrier

doi:10.1016/j.chemosphere.2023.139497

Assessment of 226Ra and U colloidal transport in a mining environment

Marine Reymond, Michaël Descostes, Clémence Besançon, Martine Leermakers, Sophie Billon, Gaël Cherfallot, Marie Muguet, Catherine Beaucaire, Vendula Smolíková, Patricia Patrier

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The colloidal transport of trace (Fe, Al, Ba, Pb, Sr, U) and ultra-trace (226Ra) elements was studied in a mining environment. An original approach combining 0.45 μm filtered water sampling, the Diffusive Gradient in Thin films (DGT) technique, mineralogical characterization, and geochemical modelling was developed and tested at 17 sampling points. DGT was used for the truly dissolved fraction of the elements of interest, while the 0.45 μm filtration includes both colloidal and truly dissolved fractions (together referred to as total dissolved fraction). Results indicated a colloidal fraction for Al (up to 50%), Ba (up to 86%), and Fe (up to 99%) explained by the presence of submicrometric grains of kaolinite, barite, and ferrihydrite, respectively. Furthermore, the total dissolved 226Ra concentration in the water samples reached up to 10–25 Bq/L (1.2–3.0 10−12 mol/L) at 3 sampling points, while the truly dissolved aqueous 226Ra concentrations were in the mBq/L range. Such high total dissolved concentrations are explained by retention on colloidal barite, accounting for 95% of the total dissolved 226Ra concentration. The distribution of 226Ra between the truly dissolved and colloidal fractions was accurately reproduced using a (Rax,Ba1-x)SO4 solid solution, with values of the Guggenheim parameter a0 close to ideality. 226Ra sorption on ferrihydrite and kaolinite, other minerals well known for their retention properties, could not explain the measured colloidal fractions despite their predominance. This illustrates the key role of barite in such environments. The measured concentrations of total dissolved U were very low at all the sampling points (<4.5 10−10 mol/L) and the colloidal fraction of U accounted for less than 65%. U sorption on ferrihydrite could account for the colloidal fraction. This original approach can be applied to other trace and ultra-trace elements to complement when necessary classical environmental surveys usually performed by filtration on 0.45 μm.

Originele taal-2	English
Artikelnummer	139497
Aantal pagina's	11
Tijdschrift	Chemosphere
Volume	338
DOI's	https://doi.org/10.1016/j.chemosphere.2023.139497
Status	Published - okt. 2023

Bibliografische nota

Funding Information:
The authors would like to thank the staff of COMUF's ORANO Mining subsidiary who made it possible to collect the samples used in this article. This work was funded by the R&D Environment division of ORANO Mining (funding contract 20.124-MN-UNIV POITIERS). The authors acknowledge financial support from the European Union (ERDF) and Région Nouvelle Aquitaine.

Publisher Copyright:
© 2023 Elsevier Ltd

Copyright:
Copyright 2023 Elsevier B.V., All rights reserved.

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10.1016/j.chemosphere.2023.139497

Reymond et al_CHEM113608_Accepted author manuscript
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Accepted author manuscript, 1,29 MBLicentie: CC BY-NC-ND

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title = "Assessment of 226Ra and U colloidal transport in a mining environment",

abstract = "The colloidal transport of trace (Fe, Al, Ba, Pb, Sr, U) and ultra-trace (226Ra) elements was studied in a mining environment. An original approach combining 0.45 μm filtered water sampling, the Diffusive Gradient in Thin films (DGT) technique, mineralogical characterization, and geochemical modelling was developed and tested at 17 sampling points. DGT was used for the truly dissolved fraction of the elements of interest, while the 0.45 μm filtration includes both colloidal and truly dissolved fractions (together referred to as total dissolved fraction). Results indicated a colloidal fraction for Al (up to 50%), Ba (up to 86%), and Fe (up to 99%) explained by the presence of submicrometric grains of kaolinite, barite, and ferrihydrite, respectively. Furthermore, the total dissolved 226Ra concentration in the water samples reached up to 10–25 Bq/L (1.2–3.0 10−12 mol/L) at 3 sampling points, while the truly dissolved aqueous 226Ra concentrations were in the mBq/L range. Such high total dissolved concentrations are explained by retention on colloidal barite, accounting for 95% of the total dissolved 226Ra concentration. The distribution of 226Ra between the truly dissolved and colloidal fractions was accurately reproduced using a (Rax,Ba1-x)SO4 solid solution, with values of the Guggenheim parameter a0 close to ideality. 226Ra sorption on ferrihydrite and kaolinite, other minerals well known for their retention properties, could not explain the measured colloidal fractions despite their predominance. This illustrates the key role of barite in such environments. The measured concentrations of total dissolved U were very low at all the sampling points (<4.5 10−10 mol/L) and the colloidal fraction of U accounted for less than 65%. U sorption on ferrihydrite could account for the colloidal fraction. This original approach can be applied to other trace and ultra-trace elements to complement when necessary classical environmental surveys usually performed by filtration on 0.45 μm.",

keywords = "Colloidal transport, 226Ra, U, Barite, Ferrihydrite, DGT",

author = "Marine Reymond and Micha{\"e}l Descostes and Cl{\'e}mence Besan{\c c}on and Martine Leermakers and Sophie Billon and Ga{\"e}l Cherfallot and Marie Muguet and Catherine Beaucaire and Vendula Smol{\'i}kov{\'a} and Patricia Patrier",

note = "Funding Information: The authors would like to thank the staff of COMUF's ORANO Mining subsidiary who made it possible to collect the samples used in this article. This work was funded by the R&D Environment division of ORANO Mining (funding contract 20.124-MN-UNIV POITIERS). The authors acknowledge financial support from the European Union (ERDF) and R{\'e}gion Nouvelle Aquitaine. Publisher Copyright: {\textcopyright} 2023 Elsevier Ltd Copyright: Copyright 2023 Elsevier B.V., All rights reserved.",

year = "2023",

month = oct,

doi = "10.1016/j.chemosphere.2023.139497",

language = "English",

volume = "338",

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AU - Reymond, Marine

AU - Descostes, Michaël

AU - Besançon, Clémence

AU - Leermakers, Martine

AU - Billon, Sophie

AU - Cherfallot, Gaël

AU - Muguet, Marie

AU - Beaucaire, Catherine

AU - Smolíková, Vendula

AU - Patrier, Patricia

N1 - Funding Information: The authors would like to thank the staff of COMUF's ORANO Mining subsidiary who made it possible to collect the samples used in this article. This work was funded by the R&D Environment division of ORANO Mining (funding contract 20.124-MN-UNIV POITIERS). The authors acknowledge financial support from the European Union (ERDF) and Région Nouvelle Aquitaine. Publisher Copyright: © 2023 Elsevier Ltd Copyright: Copyright 2023 Elsevier B.V., All rights reserved.

PY - 2023/10

Y1 - 2023/10

N2 - The colloidal transport of trace (Fe, Al, Ba, Pb, Sr, U) and ultra-trace (226Ra) elements was studied in a mining environment. An original approach combining 0.45 μm filtered water sampling, the Diffusive Gradient in Thin films (DGT) technique, mineralogical characterization, and geochemical modelling was developed and tested at 17 sampling points. DGT was used for the truly dissolved fraction of the elements of interest, while the 0.45 μm filtration includes both colloidal and truly dissolved fractions (together referred to as total dissolved fraction). Results indicated a colloidal fraction for Al (up to 50%), Ba (up to 86%), and Fe (up to 99%) explained by the presence of submicrometric grains of kaolinite, barite, and ferrihydrite, respectively. Furthermore, the total dissolved 226Ra concentration in the water samples reached up to 10–25 Bq/L (1.2–3.0 10−12 mol/L) at 3 sampling points, while the truly dissolved aqueous 226Ra concentrations were in the mBq/L range. Such high total dissolved concentrations are explained by retention on colloidal barite, accounting for 95% of the total dissolved 226Ra concentration. The distribution of 226Ra between the truly dissolved and colloidal fractions was accurately reproduced using a (Rax,Ba1-x)SO4 solid solution, with values of the Guggenheim parameter a0 close to ideality. 226Ra sorption on ferrihydrite and kaolinite, other minerals well known for their retention properties, could not explain the measured colloidal fractions despite their predominance. This illustrates the key role of barite in such environments. The measured concentrations of total dissolved U were very low at all the sampling points (<4.5 10−10 mol/L) and the colloidal fraction of U accounted for less than 65%. U sorption on ferrihydrite could account for the colloidal fraction. This original approach can be applied to other trace and ultra-trace elements to complement when necessary classical environmental surveys usually performed by filtration on 0.45 μm.

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Assessment of 226Ra and U colloidal transport in a mining environment

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