The effect of calcium on aqueous uranium(VI) speciation and adsorption to ferrihydrite and quartz

摘要

Recent studies of uranium(VI) geochemistry have focused oil the potentially important role of the aqueous species, CaUO2(CO3)(3)(2-) and Ca2UO2(CO3)(3)(0)(aq), oil inhibition of microbial reduction and uranium(VI) aqueous speciation in contaminated groundwater. However, to our knowledge, there have been no direct studies of the effects of these species on U(VI) adsorption by mineral phases. The sorption of U(VI) oil quartz and ferrihydrite was investigated in NaNO3 solutions equilibrated with either ambient air (430 ppm CO2) or 2% CO2 in the presence of 0, 1.8, or 8.9 mM Ca2+. Under conditions where the Ca2UO2(CO3)(3)(0)(aq) species predominates U(VI) aqueous speciation, the presence of Ca in solution lowered U(VI) adsorption on quartz from 77% in the absence of Ca to 42% and 10% at Ca concentrations of 1.8 and 8.9 mM, respectively. U(VI) adsorption to ferrihydrite decreased from 83% in the absence of Ca to 57% in the presence of' 1.8 mM Ca. Surface complexation model predictions that included the formation constant for aqueous Ca2UO2(CO3)(3)(0)(aq) accurately simulated the effect of Ca2+ on U(VI) sorption onto quartz and ferrihydrite within the thermodynamic uncertainty of the stability constant value. This study confirms that Ca2+ call have a significant impact on the aqueous speciation of U(VI), and consequently, oil the sorption and mobility of U(VI) in aquifers. (c) 2006 Elsevier Inc. All rights reserved.