Solubility and species distributions of radionuclides in domestic groundwater conditions are required for the safety assessment of deep underground disposal system of spent nuclear fuel (SNF). Minor actinides including Am contribute significant extents to the long-term radiotoxicity of SNF. In this study, the solubility of Am was evaluated in synthetic groundwater (Syn-DB3), which were simulated for the groundwater of the DB3 site in the KAERI Underground Research Tunnel (KURT). Geochemical modeling was performed based on the ThermoChimie_11a (2022) thermochemical database from Andra to estimate the solubility and species distributions of Am in the Syn-DB3 condition. Dissolved Am concentrations in the Syn-DB3 were experimentally measured under oversaturation conditions. Am(III) stock solution in perchlorate media was sequentially diluted in Syn-DB3 to prepare 8 μM Am(III) in Syn-DB3. The pH of the solutions was adjusted to be in the range of 6.4–10.5. A portion of the samples was transferred to quartz cells for UV-Vis absorption and time-resolved laser fluorescence spectroscopy studies and the rest were stored in centrifuge tubes. The absorption spectra of the samples were monitored over 70 days and the results suggest that Am colloidal particles were formed initially in all the samples and precipitated rapidly within two days. Over the experimental period of 236 days, small volume (10 μL) of the samples in the centrifuge tubes were periodically withdrawn after centrifugation (18000 rpm, 1 hr) for the liquid scintillation counting to measure the concentrations of Am dissolved in Syn-DB3. In the end of the experiments, pH of the samples was checked again and the final dissolved Am concentrations were determined after ultrafiltration (10 kDa) to exclude the contribution of colloidal particles. In the pH range of 8-9, which is relevant to the KURT-DB3 groundwater condition, the measured dissolved Am(III) concentrations were converged to around 10-8 M. These values are higher than the solubility of AmCO3OH:0.5H2O(s), but lower than that of AmCO3OH(am). There was no indication of transformation of the amorphous phase to the crystalline phase in our observation time window.

The solubility and species distribution of radionuclides in groundwater are essential data for the safety assessment of deep underground spent nuclear fuel (SNF) disposal systems. Americium is a major radionuclide responsible for the long-term radiotoxicity of SNF. In this study, the solubility of americium compounds was evaluated in synthetic groundwater (Syn- DB3), simulating groundwater from the DB3 site of the KAERI Underground Research Tunnel. Geochemical modeling was performed using the ThermoChimie_11a thermochemical database. Concentration of dissolved Am(III) in Syn-DB3 in the pH range of 6.4–10.5 was experimentally measured under over-saturation conditions by liquid scintillation counting over 70 d. The absorption spectra recorded for the same period suggest that Am(III) colloidal particles formed initially followed by rapid precipitation within 2 d. In the pH range of 7.5–10.5, the concentration of dissolved Am(III) converged to approximately 2×10−7 M over 70 d, which is comparable to that of the amorphous AmCO3OH(am) according to the modeling results. As the samples were aged for 70 d, a slow equilibrium process occurred between the solid and solution phases. There was no indication of transformation of the amorphous phase into the crystalline phase during the observation period.

본 연구에서는 핵폐기물 매립장의 인공 방벽으로 사용되는 시멘트 물질들과 주변 지하수 반응 결과로 형성되는 강알칼리성 지하수와 주변 암과의 반응을 통해 변화되는 지하수 특성을 지구화학 모델링을 통해 예측하고자 하였다. 연구 결과 시멘트 수화반응을 통해서 pH는 13.3를 나타내었으며 이때 생성되는 광물들은 Brucite, Katoite, Calcium Silicate Hydrate(CSH 1.1), Ettringite, Hematitie, Portlandite였다. 이들 광물들과 경주 지역에서 채취된 지하수의 반응 모델링에서는 지하수의 pH가 12.4로 예측되었다. 이러한 강알칼리성 지하수와 주변 화강암과의 반응은 년 동안 반응속도 모델링을 통해 모사하였다. 그 결과 지하수의 최종 pH는 11.2였으며 pH는 규산염 광물과 CSH 광물들의 용해 침전에 의해 조절되고 있었다. 또한 지하수 수질도 이들 광물들과 점토광물 및 산화광물들의 용해 침전에 의해 결정되고 있었다. 본 연구 결과는 장기간 동안의 강알칼리성 지하수와 주변 암과의 반응 모델링을 통해 지구화학 및 수질 변화를 예측함으로서 인공 방벽의 안정성 평가에 기여할 수 있을 것으로 판단된다.