A 300 d solubility study involving two carbonate-rich, uranium-contami
nated soils from the Department of Energy's Fernald Environmental Mana
gement Project site was conducted to predict the behavior of uranium d
uring on-site remediation of these soils. Geochemical modeling was per
formed on the aqueous species dissolved from these soils following the
solubility measurements to predict the on-site uranium leaching and t
ransport potential. Results showed that the soluble levels of the majo
r components (total uranium, calcium, magnesium, and carbonate) increa
sed continually for the first 4 weeks. After the first 4 weeks, these
components either reached a steady-state or continued to increase line
arly throughout the study. Soluble uranium levels of both soils and th
eir correlation with alkalinity was strongly mediated by the source te
rm of the contamination. Geochemical modeling predicted and anion exch
ange experiments confirmed that uranyl-carbonate complexes were the mo
st stable and abundant complexes. Further modeling showed that uranium
solubility in these soils and in onsite groundwater wells is controll
ed by UO2(H2PO4)(2), but is also mediated by complexation with carbona
te and the oxidation state of the uranium. For assessing the risk rela
ted to off-site transport of uranium, it should be recognized that the
solubility of uranium-bearing minerals is the critical factor in cont
rolling uranium solubility of these soils rather than sorption/desorpt
ion processes as measured by the uranium distribution coefficient (K-d
) in these soils.