Extraction, characterization, and stability studies of bistriazinyl-derived carboxylic acids
Separation of An(III) and Ln(III) ions will benefit the recycling of used nuclear fuel (UNF). For this purpose, many ligands have been tested over the years, and several separation processes have been successfully demonstrated on the laboratory scale. Current research aims at the development of ne...
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| Auteurs principaux: | , , , , , , , , |
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| Format: | Article (Journal) |
| Langue: | anglais |
| Publié: |
March 25, 2026
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| In: |
Industrial & engineering chemistry research
Year: 2026, Volume: 65, Numéro: 11, Pages: 6127-6142 |
| ISSN: | 1520-5045 |
| DOI: | 10.1021/acs.iecr.5c04766 |
| Accès en ligne: | Resolving-System, kostenfrei, Volltext: https://doi.org/10.1021/acs.iecr.5c04766 Verlag, kostenfrei, Volltext: https://pubs.acs.org/iecred/article/65/11/6127/5073040/Extraction-Characterization-and-Stability-Studies 
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| Notes sur l'auteur: | Laura Diaz Gomez, Patrik Weßling, Andreas Wilden, Petra J. Panak, Gregory P. Horne, Stephen P. Mezyk, Julie R. Peller, Andreas Geist, and Giuseppe Modolo |
| Résumé: | Separation of An(III) and Ln(III) ions will benefit the recycling of used nuclear fuel (UNF). For this purpose, many ligands have been tested over the years, and several separation processes have been successfully demonstrated on the laboratory scale. Current research aims at the development of new ligands that are built only with carbon, hydrogen, oxygen, and nitrogen (CHON), as they can be incinerated completely without secondary waste production. Here, we tested a new class of water-soluble ligands, the bistriazinyl-octa-carboxylic acids. - One member, in particular, 2,6-bis-[5,6-di(3,4-dicarboxyphenyl)-1,2,4-triazin-3-yl]-pyridine - (BTPOA), was found to be suitable for the selective separation of - Am(III) and Cm(III) ions from Ln(III) ions and may act as a CHON alternative - to its sulfonated analogue (SO3-Ph-BTP). BTPOA exhibited - good extraction results and a high selectivity for Am(III) over Eu(III) - ions. This ligand’s complexation of metal ions was further - studied using potentiometric spectroscopy, as well as time-resolved - laser-induced spectroscopy with Cm(III) and Eu(III) in aqueous HClO4 and HNO3 media. Conditional stability constants - of each formed species were determined. In the HClO4 system, - Cm(III) formed three species (1:1, 1:2, and 1:3) through the stepwise - addition of a single BTPOA molecule. On the other hand, in HNO3, Cm(III) formed two 1:2 complexes and one 1:3 complex, while - the stepwise formation of three species was observed for Eu(III). - The stability constants are comparable to the values for SO3-Ph-BTP. The radiolytic behavior of BTPOA was also investigated using - electron pulse irradiation measurements to determine absolute rate - coefficients (k) under ambient temperature conditions - for the reaction of BTPOA with typical UNF reprocessing radical radiolysis - productsthe hydrated electron (eaq-, k = (1.60 ± 0.02) × 1010 M-1 s-1), the hydrogen atom (H•, k = (2.17 ± 0.03) × 109 M-1 s-1), and hydroxyl - (•OH, k = (6.95 ± 0.06) × - 109 M-1 s-1) and nitrate - (NO3•, k = (0.37 ± - 0.02) × 107 M-1 s-1) radicals. These rate coefficients indicate that the radiolytic - longevity of BTPOA should increase with HNO3 concentration, - owing to the consumption of eaq-/H•, by nitrate anions, and the replacement of •OH by the less reactive NO3•. |
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| Description: | Online veröffentlicht am: 13. März 2026 Gesehen am 21.08.2026 |
| Description matérielle: | Online Resource |
| ISSN: | 1520-5045 |
| DOI: | 10.1021/acs.iecr.5c04766 |