Sophie Dettmann, Nina Maria Huittinen, Jahn Nicolas, Jerome Kretzschmar, Michael Uwe Kumke, Tamara Kutyma, Janik Lohmann, Tobias Reich, Katja Schmeide, Salim Shams Aldin Azzam, Leon Spittler, Janina Stietz
- The retention of actinides in different oxidation states (An(X), X = III, IV, VI) by a calcium-silicate-hydrate (C-S-H) phase with a Ca/Si (C/S) ratio of 0.8 was investigated in the presence of gluconate (GLU). The actinides considered were Am(III), Th(IV), Pu(IV), and U(VI). Eu(III) was investigated as chemical analogue for Am(III) and Cm(III). In addition to the ternary systems An(X)/GLU/C-S-H, also binary systems An(X)/C-S-H, GLU/C-S-H, and An(X)/GLU were studied. Complementary analytical techniques were applied to address the different specific aspects of the binary and ternary systems. Time-resolved laser-induced luminescence spectroscopy (TRLFS) was applied in combination with parallel factor analysis (PARAFAC) to identify retained species and to monitor species-selective sorption kinetics. ¹³C and ²⁹Si magic-angle-spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy and X-ray photoelectron spectroscopy (XPS) were applied to determine the bulk structure and the composition of the C-S-H surface, respectively, in theThe retention of actinides in different oxidation states (An(X), X = III, IV, VI) by a calcium-silicate-hydrate (C-S-H) phase with a Ca/Si (C/S) ratio of 0.8 was investigated in the presence of gluconate (GLU). The actinides considered were Am(III), Th(IV), Pu(IV), and U(VI). Eu(III) was investigated as chemical analogue for Am(III) and Cm(III). In addition to the ternary systems An(X)/GLU/C-S-H, also binary systems An(X)/C-S-H, GLU/C-S-H, and An(X)/GLU were studied. Complementary analytical techniques were applied to address the different specific aspects of the binary and ternary systems. Time-resolved laser-induced luminescence spectroscopy (TRLFS) was applied in combination with parallel factor analysis (PARAFAC) to identify retained species and to monitor species-selective sorption kinetics. ¹³C and ²⁹Si magic-angle-spinning (MAS) nuclear magnetic resonance (NMR) spectroscopy and X-ray photoelectron spectroscopy (XPS) were applied to determine the bulk structure and the composition of the C-S-H surface, respectively, in the absence and presence of GLU. The interaction of Th(IV) with GLU in different electrolytes was studied by capillary electrophoresis-inductively coupled plasma mass spectrometry (CE-ICP-MS). The influence of GLU on An(X) retention was investigated for a large concentration range up to 10⁻² M. The results showed that GLU had little to no effect on the overall An(X) retention by C-S-H with C/S of 0.8, regardless of the oxidation state of the actinides. For Eu(III), the TRLFS investigations additionally implied the formation of a Eu(III)-bearing precipitate with dissolved constituents of the C-S-H phase, which becomes structurally altered by the presence of GLU. For U(VI) sorption on the C-S-H phase, only a small influence of GLU could be established in the luminescence spectroscopic investigations, and no precipitation of U(VI)-containing secondary phases could be identified.…
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MetadatenAuthor details: | Sophie Dettmann, Nina Maria Huittinen, Jahn Nicolas, Jerome Kretzschmar, Michael Uwe KumkeORCiDGND, Tamara Kutyma, Janik Lohmann, Tobias Reich, Katja Schmeide, Salim Shams Aldin Azzam, Leon Spittler, Janina Stietz |
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DOI: | https://doi.org/10.3389/fnuen.2023.1124856 |
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ISSN: | 2813-3412 |
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Title of parent work (English): | Frontiers in Nuclear Engineering |
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Publisher: | Frontiers Media |
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Place of publishing: | Lausanne |
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Publication type: | Article |
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Language: | English |
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Date of first publication: | 2023/03/01 |
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Publication year: | 2023 |
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Release date: | 2023/04/24 |
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Tag: | actinide; cementitious material; concrete; luminescence; organic ligand; sorption |
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Volume: | 2 |
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Number of pages: | 15 |
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Funding institution: | Universität Potsdam |
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Funding institution: | Deutsche Forschungsgemeinschaft (DFG) |
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Funding number: | PA 2023_014 |
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Funding number: | Projektnummer 491466077 |
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Organizational units: | Mathematisch-Naturwissenschaftliche Fakultät / Institut für Chemie |
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DDC classification: | 5 Naturwissenschaften und Mathematik / 54 Chemie / 540 Chemie und zugeordnete Wissenschaften |
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| 6 Technik, Medizin, angewandte Wissenschaften / 62 Ingenieurwissenschaften / 620 Ingenieurwissenschaften und zugeordnete Tätigkeiten |
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Peer review: | Referiert |
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Grantor: | Publikationsfonds der Universität Potsdam |
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Publishing method: | Open Access / Gold Open-Access |
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License (German): | CC-BY - Namensnennung 4.0 International |
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External remark: | Zweitveröffentlichung in der Schriftenreihe Zweitveröffentlichungen der Universität Potsdam : Mathematisch-Naturwissenschaftliche Reihe ; 1318 |
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