Co-transport of U(Ⅵ) and gibbsite colloid in saturated granite particle column: Role of pH, U(Ⅵ) concentration and humic acid

摘要

Understanding the in-situ transport behavior of U(VI) in granitic formations is of considerable interest for geological disposal of high-level radioactive wastes (HLW). In this context, the co-transport of U(VI) and representative naturally-occurring colloids, i.e., humic add (HA) and gibbsite colloid (GC), was studied in granite column as a function of pH, U(VI) concentration and HA amount. It was found that, in addition to pH, co-transport of U(VI) and GC was also controlled by U(VI) concentration, the effect of which can be transport-facilitating and transport-impeding for U(VI) at relatively low concentration (2.0 x 10(-6) mol/L) and for U(VI) at high concentration (5.0 x 10(-6) mol/L), respectively. HA can present opposite effects on GC transport depending on HA amount. The transport-impeding effect by small amount of HA (5 mg/L) is due to strong aggregation between GC and HA from electrostatic attraction and complexation, whereas the transport-facilitating effect by big amount of HA (20 mg/L) is because of the complete HA coating which stabilizes associated colloids and alters surface charge from positive to negative. In ternary co-transport systems, a similar HA-dependent effect was also observed for both U(VI) and GC regardless of presence of high concentration U(VI). Besides the application of the Derjaguin-Landau-Verwey-Overbeek (DLVO) theory, the mechanisms behind binary and ternary co-transport of U(VI), GC and HA were also analyzed by assessing the evolutions of zeta potential and particle size in the column effluents. Finally, a two-site non-equilibrium model and a two-site kinetic attachment/detachment model were applied to describe the breakthrough curves of U(VI) and individual/combined colloids, respectively. The findings of this study indicated that combined effects of GC and HA on radionuclides transport is dominated by the amount of HA, and a facilitating transport of radionuclide can be expected in the underground environment rich in humic acid. (C) 2019 Elsevier B.V. All rights reserved.