Predominance of the alkaline earth (II) triscarbonatoactinyl (VI) complexes in different geochemical contexts: Review of existing data and estimation of potentially unidentified species - Archive ouverte HAL Accéder directement au contenu
Article Dans Une Revue Chemosphere Année : 2024

Predominance of the alkaline earth (II) triscarbonatoactinyl (VI) complexes in different geochemical contexts: Review of existing data and estimation of potentially unidentified species

Résumé

From the available thermodynamic data in the literature, a review of the impact of the formation of complexes between triscarbonatoactinyl(VI) and alkaline earth(II) (Ae) is estimated under varying conditions. First, using the ascertained thermodynamic data available from the commissioned reviews from the Nuclear Energy Agency (Organization for the Economic Cooperation and Development) Thermochemical DataBank Project on actinides (An) U, Np, and Pu, and from recently determined Ae$_n$UO$_2$(CO$_3$)$_3$$^{(4-2n)-}$ thermodynamic functions, the formation of Ae$_n$UO$_2$(CO$_3$)$_3$$^{(4-2n)-}$ complexes for Pu(VI) and Np(VI) are estimated using linear free energy relationships (LFERs). The data are in good agreement with the sole determination of AePuO$_2$(CO$_3$)$_3$$^{2-}$ from Jo et al. (Dalton Trans. 49, 11605), which gives a relative confidence in the LFERs, and allows the application to actual situations. From existing uranium data, first, the impact of the origin of the data on the calculated predominance is addressed under 0.1 M NaCl and atmospheric CO$_2$(g); second, the influence of ionic strength and salinity on predominance is estimated; and finally, the influence of temperature up to 50 °C on the solubility of uraninite in a deep geological radioactive waste storage or disposal site is calculated. For neptunium and plutonium, the impact of the potential log$_{10}$$\beta$°(Ae$_n$UO$_2$(CO$_3$)$_3$$^{(4-2n)-}$) on Pourbaix diagrams of Pu and Np in Mg-Ca-CO$_3$ media are estimated from Jo et al. (Dalton Trans. 49, 11605) and LFERs. Finally, the application to the speciation of Pu and Np in seawater is proposed.

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Chimie
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Dates et versions

hal-04394102 , version 1 (18-01-2024)

Licence

Paternité - Pas d'utilisation commerciale - Partage selon les Conditions Initiales

Identifiants

Citer

Pascal E. Reiller. Predominance of the alkaline earth (II) triscarbonatoactinyl (VI) complexes in different geochemical contexts: Review of existing data and estimation of potentially unidentified species. Chemosphere, 2024, 350, pp.141049. ⟨10.1016/j.chemosphere.2023.141049⟩. ⟨hal-04394102⟩
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