Cotransport of uranyl carbonate loaded on amorphous colloidal silica and strip-shaped humic acid in saturated porous media: Behavior and mechanism

Abstract

Uranyl carbonate (UC(VI)) is a stable form of uranyl (U(VI)) that widely coexists with amorphous colloidal silica (ACSi) and humic acid (HA) in carbonate-rich U-contaminated areas. In this context, the cotransport behavior and mechanism of UC(VI) with ACSi (100 mg L−1) and HA colloids in saturated porous media were systematically investigated. It was found that the ACSi and strip-shaped HA have a strong adsorption capacity for UC(VI), and their adsorption distribution coefficient (Kd) is 4–5 orders of magnitude higher than that of quartz sand (QS). In the ternary system, UC(VI) was mainly existing in the colloid-associated form at low UC(VI) concentration (4.2 × 10−6 M). Compared with the individual transport of UC(VI), the presence of ACSi and strip-shaped HA in the binary system promotes the transport of low-concentration UC(VI) (4.2 × 10−6 M) but shows a hindering effect when UC(VI) = 2.1 × 10−5 M. When ionic strength (IS) increased from 0 to 100 mM, the individual transport of UC(VI) and ACSi was weakened owing to the masking effect and the compression of the electrical double layer, respectively; this weakening effect is more pronounced in the binary (UC(VI)–ACSi) system. Notably, the transport of UC(VI) and ACSi in the ternary system is independent of the changes in IS due to the surface charge homogeneity strengthening the electrostatic repulsion between HA and QS. The Derjaguin–Landau–Verwey–Overbeek theory and retention profiles reveal the co-deposition mechanism of ACSi and UC(VI) in the column under different hydrochemical conditions. The nonequilibrium two-site model and the mathematical colloidal model successfully described the breakthrough data of UC(VI) and ACSi, respectively. These results are helpful for evaluating the pollution caused by UC(VI) migration in an environment rich in HA and formulating corresponding effective control strategies.