Elemental and particle size fractionation during the transport of Eu(III)-silicate colloids in water-saturated porous media.

ABSTRACT

Actinides (An)-bearing colloids could facilitate An migration in the environment. However, little is known about the transport behavior of An(III)-silicate colloids, which are readily formed by the reaction of An3+ with silicic acid under environmental conditions. Column experiments were conducted to investigate the transport of Eu(III)-silicate colloids (chemical analog of An(III)-silicate colloids) in water-saturated porous media as a function of pH, ionic strength (IS) and the presence of fulvic acid (FA). The results showed that colloid transport was more favorable at relatively low IS (≤ 50 mM) and high pH levels (pH ≥ 7). The presence of FA (5-10 mg/L) significantly enhanced the colloid transport. Under high IS (≥ 100 mM), the transport feature of colloids was turned from blocking to ripening due to the on-going aggregation of colloids. Additionally, an interesting elemental fractionation, i.e., a discrepancy in the breakthrough curves (BTCs) with respect to the C/C0 values of Si and Eu, was observed in the IS of 100-500 mM. A detailed investigation indicated that the elemental fractionation could be attributed to the partial Si dissolution of the colloids, the heterogeneity of the colloid size and element composition, and particle size fractionation during colloid transport. Extended Derjaguin-Landau-Verwey-Overbeek interaction energy calculations and convective-dispersive equation modeling were performed to illustrate variations in the colloid transport profiles. These findings illustrate the importance of Si dissolution in the migration of metal-silicate colloids and highlight the significant influence of the heterogeneity of colloid size and composition on the transport/migration behavior of colloids in the environment.