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Uptake of Eu, Th, U, and Pu by granite and biotite gneiss in Korean fresh groundwater under oxidizing and reducing conditions

  • Hyeonjin Eun ORCID logo , Peter Gyula Szabo ORCID logo , Darlyn Rehhorn , Seungwoo Lee ORCID logo , Yongheum Jo ORCID logo , Marcus Altmaier , Jinyoung Lee ORCID logo , Xavier Gaona ORCID logo EMAIL logo and Jong-Il Yun ORCID logo EMAIL logo
Published/Copyright: December 19, 2024
Radiochimica Acta
From the journal Radiochimica Acta Volume 113 Issue 3

Abstract

The uptake of Eu, Th, U, and Pu by Korean granite and biotite gneiss was investigated in a series of batch experiments. Experiments were conducted under well-defined redox conditions, i.e., oxidizing (air), mildly reducing (Ar-atmosphere and buffered with hydroquinone, pe + pH ≈ 8–9), and strongly reducing (Ar-atmosphere and buffered with Na2S2O4, pe + pH ≈ 0.5–3). Radionuclide concentration, pH and Eh were systematically monitored up to t ≤ 113 days after the addition of the radionuclide. The natural content of Eu, Th and U in pristine granite and biotite gneiss materials was quantified by means of alkaline fusion. Eu exhibited moderate sorption on biotite gneiss displaying higher distribution ratios (Rd) compared to granite. This observation was possibly explained by the affinity of Ln(III)/An(III) towards biotite mineral absent in the investigated granite material. Strong sorption was observed for Th, U, and Pu in reducing systems where the predominance of the +IV oxidation state is expected. For these three systems, the strength of the uptake follows the order Rd(Pu(IV)) > Rd(U(IV)) > Rd(Th(IV)), consistent with the hydrolysis strength of the corresponding aquo-ions. A significantly weaker sorption was observed for U and Pu under oxidizing conditions, although Rd values are manifestly higher for Pu than U. Thermodynamic calculations for the oxidizing conditions predicted the predominance of U(VI) and Pu(V)/Pu(IV), explaining observed differences in retention under oxidizing conditions. These results contribute to a quantitative description and a better understanding of the retention of redox-sensitive radionuclides in crystalline host rocks. Emphasis is placed on the importance of utilizing both redox-stable probes (e.g., Eu, Th) and redox-sensitive actinides (e.g., U, Pu), as well as well-defined redox conditions for accurate predictions of radionuclide retention.

Keywords: sorption; actinide elements; europium; granite; biotite gneiss; redox conditions
Corresponding authors: Xavier Gaona, Institute for Nuclear Waste Disposal (INE), Karlsruhe Institute of Technology, Karlsruhe 76344, Germany, E-mail: ; and Jong-Il Yun, Department of Nuclear and Quantum Engineering, KAIST, 291 Daehak-ro, Yuseong-gu, Daejeon 34141, Republic of Korea, E-mail:
Hyeonjin Eun and Peter Gyula Szabo contributed equally and should be regarded as co-first authors.

Acknowledgements

Max Bachert and Jonas Rentmeister (both KIT-INE) are kindly acknowledged for the SF-ICP-MS and TIC measurements.

  1. Research ethics: Not applicable.

  2. Informed consent: Not applicable.

  3. Author contributions: The authors have accepted responsibility for the entire content of this manuscript and approved its submission.

  4. Use of Large Language Models, AI and Machine Learning Tools: None declared.

  5. Conflict of interest: The authors state no conflict of interest.

  6. Research funding: This work was funded by Hyundai Engineering and Construction Co. Ltd, the Institute for Korea Spent Nuclear Fuel (iKSNF) and Korea Institute of Energy Technology Evaluation and Planning (KETEP) grant funded by the Korea government Ministry of Trade, Industry and Energy (MOTIE) (No. 1415176399, iKSNF_2021040101003C, and RS-2023-00236697).

  7. Data availability: The raw data can be obtained on request from the corresponding authors.

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Supplementary Material

This article contains supplementary material (https://doi.org/10.1515/ract-2024-0331).

Received: 2024-07-03
Accepted: 2024-12-05
Published Online: 2024-12-19
Published in Print: 2025-03-26

© 2024 Walter de Gruyter GmbH, Berlin/Boston

Articles in the same Issue

  1. Frontmatter
  2. Original Papers
  3. Single-atom-at-a-time adsorption studies of 211Bi and its precursor 211Pb on SiO2 surfaces
  4. Uptake of Eu, Th, U, and Pu by granite and biotite gneiss in Korean fresh groundwater under oxidizing and reducing conditions
  5. A new targetry system for cyclotron production of pharmaceutical grade indium-111 radioisotope
  6. Hierarchical macro/mesoporous γ-Al2O3 as column matrix for development of low specific activity 99Mo/99mTc generator via 100Mo (γ, n)99Mo reaction
  7. Design of a novel complex 99mTc-Nilutamide as a tracer for prostate cancer disorder detection in mice
  8. Dehydration of un-irradiated and gamma and electron-beam irradiated europium acetate hydrate under non-isothermal conditions: kinetics of the dehydration process of un-irradiated material
  9. Radiochromic liquid dosimeter based on p-arsanilic acid for gamma radiation monitoring
  10. Assessing carcinogenic radon levels in water from Er-Rachidia, Morocco using LR-115 nuclear track detectors
https://doi.org/10.1515/ract-2024-0331
Keywords for this article
sorption; actinide elements; europium; granite; biotite gneiss; redox conditions

Articles in the same Issue

  1. Frontmatter
  2. Original Papers
  3. Single-atom-at-a-time adsorption studies of 211Bi and its precursor 211Pb on SiO2 surfaces
  4. Uptake of Eu, Th, U, and Pu by granite and biotite gneiss in Korean fresh groundwater under oxidizing and reducing conditions
  5. A new targetry system for cyclotron production of pharmaceutical grade indium-111 radioisotope
  6. Hierarchical macro/mesoporous γ-Al2O3 as column matrix for development of low specific activity 99Mo/99mTc generator via 100Mo (γ, n)99Mo reaction
  7. Design of a novel complex 99mTc-Nilutamide as a tracer for prostate cancer disorder detection in mice
  8. Dehydration of un-irradiated and gamma and electron-beam irradiated europium acetate hydrate under non-isothermal conditions: kinetics of the dehydration process of un-irradiated material
  9. Radiochromic liquid dosimeter based on p-arsanilic acid for gamma radiation monitoring
  10. Assessing carcinogenic radon levels in water from Er-Rachidia, Morocco using LR-115 nuclear track detectors
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