Sorption of Cs and Eu ions onto sedimentary rock in the presence of gamma-irradiated humic acid

Zhao, Q.*; Saito, Takeshi*; Miyakawa, Kazuya   ; Sasamoto, Hiroshi   ; Kobayashi, Taishi*; Sasaki, Takayuki*

The influence of humic acid and its radiological degradation on the sorption of Cs and Eu by sedimentary rock was investigated to understand the sorption process of metal ions and humic substances. Aldrich humic acid (HA) solution was irradiated with different doses of gamma irradiation using a Co-60 gamma-ray source prior to the contact between the metal ions and the solid sorbent. The HA molecule decomposed to smaller molecules with a lower complexation affinity. Batch sorption experiments were performed to evaluate the effect of gamma-irradiated HA on the sorption of Cs and Eu ions. The addition of non-irradiated HA weakened the sorption of Eu because of the lower sorption of the neutral or negatively charged Eu-HA complexes compared with free Eu ions. The sorption of monovalent Cs ions was barely affected by the presence of HA and its gamma irradiation. The concentration ratio of HA complexed species and non-complexed species in the solid and liquid phases was evaluated by sequential filtration and chemical equilibrium calculations. The ratios supported the minimal contribution of HA to Cs sorption. However, the concentration ratio for Eu in the liquid phase was high, indicating that the complexing ability of HA to Eu was higher than that of HA to Cs ions. Therefore, the sorption of free Eu would predominate with the gamma irradiation dose applied to the HA solution under a radiation field near the HLW package.