Sorption of uranium and cesium by Hanford basalts and associated secondary smectite

Abstract

Three characterized basalts and an associated secondary smectite were used in comparative uranium and cesium sorption studies. Experiments utilizing two synthetic characteristic basalt groundwaters at 23° and 60°C allowed comparison of increased temperature and carbonate concentration effects on Cs and U sorption. The sorption data were fitted to the Dubinin-Radushkevich (D-R) isotherm, and loading maxima and energetics derived. An increase in temperature caused a decrease in Cs sorption maxima on all solids from all groundwaters studied and an increase in U sorption maxima, especially from the higher-carbonate-content groundwater. Sorption energies were characteristic of ion exchange for both Cs and U sorption processes. Basalt U sorption maxima were relatively insignificant, but smectite U sorption maxima surpassed Cs sorption maxima in both groundwaters at 60°C. The uranyl carbonate complexes thus may be relatively temperature-sensitive. Upon removal of excess Fe-oxides from the secondary smectite, U sorption decreased and the D-R isotherm reverted to a normal Freundlich sorption isotherm. Removal of excess Fe-oxides from the basalts and secondary smectite would probably result in Freundlich sorption isotherms for both Cs and U.