Complexation and Extraction Studies of Trivalent Actinides and Lanthanides with Water-Soluble and CHON-Compatible Ligands for the Selective Extraction of Americium

Autor: Patrik Weßling, Melina Maag, Giana Baruth, Thomas Sittel, Fynn S. Sauerwein, Andreas Wilden, Giuseppe Modolo, Andreas Geist, Petra J. Panak
Jazyk: angličtina
Rok vydání: 2022
Předmět:
Zdroj: Inorganic chemistry 61(44), 17719–17729 (2022). doi:10.1021/acs.inorgchem.2c02871
Inorganic Chemistry, 61 (44), 17719–17729
ISSN: 0020-1669
1520-510X
DOI: 10.1021/acs.inorgchem.2c02871
Popis: Novel hydrophilic ligands to selectively separate Am(III) are synthesized: 3,3′-([2,2′-bipyridine]-6,6′-diylbis(1H-1,2,3-triazole-4,1-diyl))bis(propan-1-ol) (PrOH-BPTD) and 3,3′-([2,2′-bipyridine]-6,6′-diylbis(1H-1,2,3-triazole-4,1-diyl))bis(ethan-1-ol) (EtOH-BPTD). The complexation of An(III) and Ln(III) with PrOH- and EtOH-BPTD is studied by time-resolved laser fluorescence spectroscopy. [ML2]3+ is found for both Cm(III) and Eu(III), while [ML]3+ is only formed with Cm(III). Stability constants show a preferential coordination of Cm(III) over Eu(III) with PrOH-BPTD being the stronger ligand. The distribution of Am(III), Cm(III), and Ln(III) between an organic phase containing the extracting agent N,N,N′,N′-tetra-n-octyl-3-oxapentanediamide (TODGA) and aqueous phases containing PrOH-BPTD is studied as a function of time and temperature as well as the TODGA, BPTD, and HNO3 concentrations. A system composed of 0.2 mol/L TODGA and 0.04 mol/L PrOH-BPTD in 0.33–0.39 mol/L HNO3 allows for selective Am(III) back-extraction into the aqueous phase while keeping Cm(III) and Ln(III) in the organic phase, marking PrOH-BPTD as an excellent complexant for an optimized AmSel process (Am(III) selective extraction).
Databáze: OpenAIRE