Thermodynamics of the Eu(iii)–Mg–SO4–H2O and Eu(iii)–Na–SO4–H2O systems. Part I: solubility experiments and the full dissociation Pitzer model - BRGM - Bureau de recherches géologiques et minières Accéder directement au contenu
Article Dans Une Revue Dalton Transactions Année : 2024

Thermodynamics of the Eu(iii)–Mg–SO4–H2O and Eu(iii)–Na–SO4–H2O systems. Part I: solubility experiments and the full dissociation Pitzer model

Résumé

The solubility of Eu(III) was investigated under undersaturated conditions in acidic, dilute to concentrated MgSO4 and Na2SO4 solutions at T = (22 ± 2) °C. After attaining equilibrium conditions, solid phases were characterized by a multi-method approach, including X-ray diffraction (XRD), Raman and infrared (IR) spectroscopy, quantitative chemical analysis (ICP-OES) and thermogravimetric analysis (TG-DTA). A total of 45 solubility samples were investigated for the systems Eu2(SO4)3–MgSO4–H2O (19 samples) and Eu2(SO4)3–Na2SO4–H2O (26 samples). Eu2(SO4)3·8H2O(cr) was found to control the solubility of Eu(III) in all investigated MgSO4 solutions, as well as in dilute Na2SO4 systems. The transformation of Eu2(SO4)3·8H2O(cr) into the double salt Na2Eu2(SO4)4·2H2O(cr) was observed at mNa2SO4 > 0.01 mol kg−1. The latter phase is characterized by significantly lower solubility. Based on these experimental solubility measurements, thermodynamic and activity models were proposed based on the Pitzer equations considering the full dissociation of the Eu(III) species in MgSO4 and Na2SO4 aqueous solutions, i.e. deliberately excluding Eu(III)-sulfate complex formation. A combination of the geochemical calculation code PhreeSCALE and the parameter estimation code PEST was used to determine the values of solubility products Image ID:d3dt04322c-t1.gif and binary and ternary specific interaction parameters (β(0)ij, β(1)ij, Cϕij, θik, Ψijk).
Fichier principal
Vignette du fichier
d3dt04322c.pdf (1.48 Mo) Télécharger le fichier
Origine : Publication financée par une institution

Dates et versions

hal-04510034 , version 1 (18-03-2024)

Identifiants

Citer

P F dos Santos, Arnault Lassin, X Gaona, K Garbev, M Altmaier, et al.. Thermodynamics of the Eu(iii)–Mg–SO4–H2O and Eu(iii)–Na–SO4–H2O systems. Part I: solubility experiments and the full dissociation Pitzer model. Dalton Transactions, 2024, ⟨10.1039/d3dt04322c⟩. ⟨hal-04510034⟩

Collections

BRGM
11 Consultations
3 Téléchargements

Altmetric

Partager

Gmail Facebook X LinkedIn More