Steric hindrance of phenanthroline diamides enables a hundredfold increase in Am(III) extraction efficiency

Avagyan, N.A.; Zonov, R.V.; Lemport, P.S.; Evsiunina, M.V.; Matveev, P.I.; Roznyatovsky, V.A.; Averin, A.D.; Kalle, P.; Tafeenko, V.A.; Soloveva, S.A.; Nelyubina, Y.V.; Petrov, V.G.; Ustynyuk, Y.A.; Nenajdenko, V.G.

Авторы: Avagyan Nane A., Zonov Roman V., Lemport Pavel S., Evsiunina Mariia V., Matveev Petr I., Roznyatovsky Vitaly A., Averin Alexei D., Kalle Paulina, Tafeenko Victor A., Soloveva Svetlana A., Nelyubina Yulia V., Petrov Vladimir G., Ustynyuk Yuri A., Nenajdenko Valentine G.
Журнал: Dalton Transactions
Том: 54
Год издания: 2025
Издательство: Royal Society of Chemistry
Местоположение издательства: United Kingdom
Первая страница: 5425
Последняя страница: 5437
DOI: 10.1039/d5dt00076a
Аннотация: Three novel 1,10-phenanthroline-2,9-dicarboxamides (DAPhen) were prepared and investigated in detail. The presence of alkyl groups in ortho-positions of aryl substituent in the ligand amide functions results in completely inhibited rotation around N-Ar bond and complicated conformational behavior. Very significant effect of ligand steric hindrance on a solvent extraction of lanthanides(III) and Am(III) from nitric acid solution was demonstrated. The extraction tests indicated that all three ligands L1-L3 extract Am better than all lanthanides. Very high separation factors of Am from the early lanthanides (La, Ce) SFAm/Lа,Се > 40 were observed. For all three ligands, the separation factors from all lanthanides are also high (SFAm/Ln > 10), which makes them suitable for practical applications for spent nuclear fuel (SNF) reprocessing. The extraction efficiency (distribution ratio) increases by almost two orders of magnitude for all tested f-elements while maintaining an overall extraction trend. Since the solvent extraction of Ln(III) and/or Am(III) involves the formation of corresponding complex compounds, a detailed investigation of coordination chemistry of novel DAPhen sterically hindered ligands toward lanthanides and americium nitrates was performed. A combination of single-crystal X-ray analysis, spectral techniques and quantum-chemical calculations allowed us to explain nearly hundredfold increase of Am(III) extraction efficiency when moving from ortho-methyl substituents toward more bulky ortho-isopropyl groups.
Добавил в систему: Авакян Нанэ Арменовна

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Steric hindrance of phenanthroline diamides enables a hundredfold increase in Am(III) extraction efficiencyстатья Исследовательская статья

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