Solubility of schoepite: comparison and selection of complexation constants for U(VI)

Solubility of UO(3) x nH(2)O and sorption of U(VI) onto ferric (hydr)oxides were measured at pH 5.9, 6.8, and 7.8 at 10(-3.5)atm CO(2) using reaction times up to 48 days. Precipitation was fastest in the presence of hydrous ferric oxide and slower with hematite or without an initial solid phase. Solubility after 48 days was statistically similar for low to intermediate initial supersaturation conditions and increased for the highest initial supersaturation. Schoepite was identified for low-to-intermediate initial conditions of supersaturation and was not found for the highest initial supersaturation. Predicted concentrations of monomeric and polymeric species differed considerably with the different suites of complexation constants, resulting in significant differences in predicted oxidation-reduction potential and mobility of U(VI) in groundwater. Solubilities for low to intermediate initial supersaturation were best represented using complexation constants from Langmuir, D. [1978. Uranium solution-mineral equilibria at low temperatures with applications to sedimentary ore deposits. Geochim. Cosmochim. Acta 42, 547-569] and log*K(sp)=5.39 for schoepite, while solubilities for very high initial supersaturation were consistent with amorphous UO(3) x nH(2)O.