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Determination of the Formation Constants of Ternary Complexes of Uranyl and Carbonate with Alkaline Earth Metals (Mg2+, Ca2+, Sr2+, and Ba2+) Using Anion Exchange Method

Journal Article · · Environmental Science & Technology
OSTI ID:978224
The formation constants of ternary complexes (MUO2(CO3)32- and M2UO2(CO3)30) of uranyl and carbonate with alkaline earth metals (M2+ denotes Mg2+, Ca2+, Sr2+, and Ba2+) were determined with an anion exchange method by varying the metal concentrations (0.1-5 mmol/L) at pH 8.1 and a constant ionic strength (0.1 mol/L NaNO3) under equilibrium with atmospheric CO2. The results indicate that the complexes of MUO2(CO3)32- and M2UO2(CO3)3 are simultaneously formed for Ca2+ and Ba2+, while Mg2+ and Sr2+ form only the MUO2(CO3)32- complex under our experimental conditions. The cumulative stability constants for the MUO2(CO3)32- complex obtained at I = 0 are: log 113 = 26.11 b 0.04, 27.18 b 0.06, 26.86 b 0.04, and 26.68 b 0.04 for Mg2+, Ca2+, Sr2+ and Ba2+, respectively. For M2UO2(CO3)30 the value of log 213 at I = 0 was measured to be 30.70 b 0.05 and 29.75 0.07 for Ca2+ and Ba2+, respectively. Based on the formation constants obtained in this study, speciation calculations indicate that at low Ca2+ concentration (e.g., < 2.2 mmol/L) CaUO2(CO3)32- is more important than Ca2UO2(CO3)3 and that the Ca2UO2(CO3)3 distribution increased with increasing Ca2+ concentration. Uranium sorption onto anion exchange resins is inhibited by the formation of the neutral Ca2UO2(CO3)30 species.
Research Organization:
Oak Ridge National Laboratory (ORNL)
Sponsoring Organization:
SC USDOE - Office of Science (SC)
DOE Contract Number:
AC05-00OR22725
OSTI ID:
978224
Journal Information:
Environmental Science & Technology, Journal Name: Environmental Science & Technology Journal Issue: 15 Vol. 40
Country of Publication:
United States
Language:
English

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