Chemical thermodynamics of ternary M-An(VI)-CO3 system (M = Mg, Ca, Sr, and Ba)

Abstract

This review provides an overview of the chemical thermodynamics on ternary earth-alkaline metal-actinyl-tricarbonate systems (i.e., M-AnO(2)-CO3, M = Mg, Ca, Sr, and Ba) and discusses the aqueous complexation and dissolution/precipitation equilibrium for these ternary aqueous systems. The aqueous ternary U(VI) carbonate species are remarkably predominant in the U(VI) speciation under natural environmental conditions at ambient temperature and moderate ionic strength condition, while the omnipresence, according to recent studies, would be hindered by an increase in temperature and ionic strength. With respect to the ternary solid U(VI) carbonate phases, most of the previously reported data have been focused on physical properties and thus a notable lack of available data on chemical thermodynamic properties, i.e., solubility product constant, has been identified. Nevertheless, substantial influences of these ternary M-AnO(2)-CO3 systems on the aqueous speciation and the solubility limiting phase under the natural environmental condition are taken into account according to the thermodynamic calculation. The authors point out that the completeness of the chemical thermodynamic model for predicting the chemical behavior of actinides in nature can be further improved on the basis of a sufficient understanding of ternary M-AnO(2)-CO3 systems.