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The effect of humic acid (HA) on the uranium(VI) sorption onto phyllite and onto its individual main mineralogical constituents, muscovite, albite, and quartz was studied in air-equilibrated batch experiments in the pH range of 3.5 to 9.5. The uranyl(VI) and HA concentration was 1×10-6 M and 5 mg/L, respectively. The ionic strength was held constant at 0.1 M (NaClO4 solution). A size fraction of 63 to 200 µm of the solids was used, the mass loading was 12.5 g/L, and the experimental volume was 40 mL.
The rock material phyllite shows both the highest HA sorption over the entire pH range and the highest uranyl sorption in the neutral pH range compared to the pure mineral phases muscovite, albite and quartz. In contrast to the minerals the maximum of the uranium sorption on phyllite is not shifted to lower pH values but remains largely unchanged in the pH range from 6 to 7.8 when HA is present at 5 mg/L. This is attributed to ferrihydrite a secondary mineral phase formed during the sorption experiments.
The humic acid and uranyl sorption on the mineral surfaces of the constituents of phyllite decreased in the sequence: muscovite > albite > quartz. Below pH 5, the uranium uptake is generally increased in the presence of HA. This is attributed to the fact that the HA is sorbed on the mineral surface thereby providing additional sorption sites due to their complexing ability and/or due to adsorption of uranyl humate complexes on the mineral surface. In the neutral pH range, the HA sorption decreases with increasing pH. The dissolved HA forms aqueous uranyl humate complexes thereby decreasing the uranyl uptake on the solids. At alkaline pH values, the HA has little or no effect on the amount of uranium sorbed by muscovite, albite and quartz. Inorganic carbonates with its high complexing ability towards uranyl ions predominate the influence of HA under the given experimental conditions. We conclude that the uranium sorption is determined by the kind of rock material or mineral and is strongly affected by both the pH and the presence of organic material.
In addition, the uranium adsorption on phyllite was studied as a function of the HA concentration (5 and 60 mg HA/L). Below pH 5.7, the uranium sorption is enhanced in the presence of 60 mg HA/L compared to experiments carried out with 5 mg HA/L. From pH 5.4 to 9.4, the uranium uptake, on a percentage basis, decreased as the humic acid concentration increased. Thus, a strong relationship between the initial humic acid concentration in solution and the amount of uranium adsorbed at a given pH was found.