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The structures of C...
The structures of CyMe4-BTBP complexes of americium(III) and europium(III) in solvents used in solvent extraction, explaining their separation properties
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- Ekberg, Christian, 1967 (author)
- Chalmers tekniska högskola,Chalmers University of Technology
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- Löfström Engdahl, Elin, 1983 (author)
- Chalmers tekniska högskola,Chalmers University of Technology
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- Aneheim, Emma, 1982 (author)
- Chalmers tekniska högskola,Chalmers University of Technology
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- Foreman, Mark, 1973 (author)
- Chalmers tekniska högskola,Chalmers University of Technology
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- Geist, A. (author)
- Karlsruher Institut für Technologie (KIT),Karlsruhe Institute of Technology (KIT)
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- Lundberg, Daniel (author)
- Swedish University of Agricultural Sciences,Sveriges lantbruksuniversitet,Institutionen för Kemi och Bioteknologi,The Department of Chemistry and Biotechnology
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- Denecke, M. (author)
- University of Manchester
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- Persson, Ingmar (author)
- Swedish University of Agricultural Sciences,Sveriges lantbruksuniversitet,Institutionen för kemi,Department of Chemistry
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(creator_code:org_t)
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- 2015
- 2015
- English.
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In: Dalton Transactions. - : Royal Society of Chemistry (RSC). - 1477-9226 .- 1477-9234. ; 44:42, s. 18395-18402
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Abstract
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- Separation of trivalent actinoid (An(III)) and lanthanoid (Ln(III)) ions is extremely challenging due to their similar ionic radii and chemical properties. Poly-aromatic nitrogen compounds acting as tetradentate chelating ligands to the metal ions in the extraction, have the ability to sufficiently separate An(III) from Ln(III). One of these compounds, 6,6'-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-benzol[1,2,4]triazin-3-y l)-[2,2]bipyridine, CyMe4-BTBP, has proven to be resistant towards acidic environments and strong radiation from radioactive decomposition. EXAFS studies of the dicomplexes of CyMe4-BTBP with americium(III) and europium(III) in nitrobenzene, cyclohexanone, 1-hexanol, 1-octanol and malonamide (DMDOHEMA) in 1-octanol have been carried out to get a deeper understanding of the parameters responsible for the separation. The predominating complexes independent of solvent used are [Am(CyMe4-BTBP)(2)(NO3)](2+) and [Eu(CyMe4-BTBP)(2)](3+), respectively, which are present as outer-sphere ion-pairs with nitrate ions in the studied solvents with low relative permittivity. The presence of a nitrate ion in the first coordination sphere of the americium(III) complex compensates the charge density of the complex considerably in comparison when only outer-sphere ion-pairs are formed as for the [Eu(CyMe4-BTBP)(2)](3+) complex. The stability and solubility of a complex in a solvent with low relative permittivity increase with decreasing charge density. The [Am(CyMe4-BTBP)(2)(NO3)](2+) complex will therefore be increasingly soluble and stabilized over the [Eu(CyMe4-BTBP)(2)](3+) complex in solvents with decreasing relative permittivity of the solvent. The separation of americium(III) from europium(III) with CyMe4-BTBP as extraction agent will increase with decreasing relative permittivity of the solvent, and thereby also with decreasing solubility of CyMe4-BTBP. The choice of solvent is therefore a balance of a high separation factor and sufficient solubility of the CyMe4-BTBP ligand.
Subject headings
- NATURVETENSKAP -- Fysik -- Subatomär fysik (hsv//swe)
- NATURAL SCIENCES -- Physical Sciences -- Subatomic Physics (hsv//eng)
- NATURVETENSKAP -- Kemi -- Oorganisk kemi (hsv//swe)
- NATURAL SCIENCES -- Chemical Sciences -- Inorganic Chemistry (hsv//eng)
Keyword
- ligands
- thermodynamics
- radiolytic stability
- btbp
- actinide(iii)/lanthanide(iii) separation
- lanthanides
- donor
- Chemistry
- quadridentate
- diluents
- actinides
- sanex
Publication and Content Type
- art (subject category)
- ref (subject category)
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