Impact of Interactions between Natural Organic Matter and Metal Oxides on the Desorption Kinetics of Uranium from Heterogeneous Colloidal Suspensions

摘要

Colloids play an important role in governing the transport of radionuclides in geologic environments. As naturally occurring colloidal suspensions are compositionally heterogeneous, the subsurface fate of radionuclides may be sensitive to interactions among different kinds of colloids. Therefore, we investigated the adsorption equilibrium and desorption kinetics of uranium (U(Ⅵ)) in experiments conducted with compositionally homogeneous suspensions of colloidal SiO_2 ZnO, hydrous ferric oxide (HFO) or humic acids (HAs) as well as heterogeneous suspensions consisting of a colloidal metal oxide and HA. We found that interactions between HAs and ZnO or HFO greatly inhibited the sorption of U onto colloids in the heterogeneous suspensions. HA-ZnO interactions enhanced the desorption of U from the heterogeneous colloidal suspensions, while the association between HA and SiO_2 or HFO inhibited U desorption. Molecular-level characterizations reveal that HFO interacted with HAs by electrostatic interactions, association with aliphatic/aromatic carbon and inner-sphere complexation with carboxyl functional groups, while SiO_2 and ZnO mainly associated with HAs by weak interactions (e.g., van der Waals interactions). The present findings indicate that interactions between HA and metal-oxide colloids can substantially influence the desorption of U(Ⅵ) from these particles, thereby potentially affecting the mobility of this radionuclide in groundwater.