Shape-Selective Supramolecular Capsules for Actinide Precipitation and Separation.
| Autor: | O'Connell-Danes J; EaStCHEM School of Chemistry, University of Edinburgh, Edinburgh EH9 3FJ, U.K., Ngwenya BT; School of Geosciences, University of Edinburgh, Edinburgh EH9 3FE, U.K., Morrison CA; EaStCHEM School of Chemistry, University of Edinburgh, Edinburgh EH9 3FJ, U.K., Nichol GS; EaStCHEM School of Chemistry, University of Edinburgh, Edinburgh EH9 3FJ, U.K., Delmau LH; Radioisotope Science and Technology Division, Oak Ridge National Laboratory, Oak Ridge, Tennessee 37831, United States., Love JB; EaStCHEM School of Chemistry, University of Edinburgh, Edinburgh EH9 3FJ, U.K. |
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| Jazyk: | angličtina |
| Zdroj: | JACS Au [JACS Au] 2024 Feb 12; Vol. 4 (2), pp. 798-806. Date of Electronic Publication: 2024 Feb 12 (Print Publication: 2024). |
| DOI: | 10.1021/jacsau.3c00793 |
| Abstrakt: | Improving actinide separations is key to reducing barriers to medical and industrial actinide isotope production and to addressing the challenges associated with the reprocessing of spent nuclear fuel. Here, we report the first example of a supramolecular anion recognition process that can achieve this goal. We have designed a preorganized triamidoarene receptor that induces quantitative precipitation of the early actinides Th(IV), Np(IV), and Pu(IV) from industrially relevant conditions through the formation of self-assembled hydrogen-bonded capsules. Selectivity over the later An(III) elements is shown through modulation of the nitric acid concentration, and no precipitation of actinyl or transition-metal ions occurs. The Np, Pu, and Am precipitates were characterized structurally by single-crystal X-ray diffraction and reveal shape specificity of the internal hydrogen-bonding array for the encapsulated hexanitratometalates. This work complements ion-exchange resins for 5f-element separations and illustrates the significant potential of supramolecular separation methods that target anionic actinide species. Competing Interests: The authors declare no competing financial interest. (© 2024 The Authors. Published by American Chemical Society.) |
| Databáze: | MEDLINE |
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