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Exploring electronic effects on the partitioning of actinides(III) from lanthanides(III) using functionalised bis-triazinyl phenanthroline ligands

The first examples of 4,7-disubstituted 2,9-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-1,2,4-benzo-triazin-3-yl)-1,10-phenanthroline (CyMe4-BTPhen) ligands are reported herein. Evaluating the kinetics, selectivity and stoichiometry of actinide(III) and lanthanide(III) radiotracer extractions has pro...

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Main Authors: Edwards, Alyn C. (Author) , Wagner, Christoph (Author) , Geist, Andreas (Author) , Burton, Neil A. (Author) , Sharrad, Clint A. (Author) , Adams, Ralph W. (Author) , Pritchard, Robin G. (Author) , Panak, Petra (Author) , Whitehead, Roger C. (Author) , Harwood, Laurence M. (Author)
Format: Article (Journal)
Language:English
Published: 29 July 2016
In: Dalton transactions
Year: 2016, Volume: 45, Issue: 45, Pages: 18102-18112
ISSN:1477-9234
DOI:10.1039/C6DT02474B
Online Access:Verlag, lizenzpflichtig, Volltext: https://doi.org/10.1039/C6DT02474B
Verlag, lizenzpflichtig, Volltext: https://pubs.rsc.org/en/content/articlelanding/2016/dt/c6dt02474b
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Author Notes:Alyn C. Edwards, Christoph Wagner, Andreas Geist, Neil A. Burton, Clint A. Sharrad, Ralph W. Adams, Robin G. Pritchard, Petra J. Panak, Roger C. Whitehead and Laurence M. Harwood
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Summary:The first examples of 4,7-disubstituted 2,9-bis(5,5,8,8-tetramethyl-5,6,7,8-tetrahydro-1,2,4-benzo-triazin-3-yl)-1,10-phenanthroline (CyMe4-BTPhen) ligands are reported herein. Evaluating the kinetics, selectivity and stoichiometry of actinide(III) and lanthanide(III) radiotracer extractions has provided a mechanistic insight into the extraction process. For the first time, it has been demonstrated that metal ion extraction kinetics can be modulated by backbone functionalisation and a promising new CHON compliant candidate ligand with enhanced metal ion extraction kinetics has been identified. The effects of 4,7-functionalisation on the equilibrium metal ion distribution ratios are far more pronounced than those of 5,6-functionalisation. The complexation of Cm(III) with two of the functionalised ligands was investigated by TRLFS and, at equilibrium, species of 1 : 2 [M : L] stoichiometry were observed exclusively. A direct correlation between the ELUMO-EHOMO energy gap and metal ion extraction potential is reported, with DFT studies reaffirming experimental findings.
Item Description:Gesehen am 05.05.2020
Physical Description:Online Resource
ISSN:1477-9234
DOI:10.1039/C6DT02474B

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