New bis(triazinyl) pyridines for selective extraction of americium(iii)

Hudson, Michael J.; Boucher, Carole; Braekers, Damien; Desreux, Jean F.; Drew, Michael G. B.; Foreman, Mark; Harwood, Laurence M.; Hill, C.; Madic, C.; Marken, Frank; Youngs, Tristan G. A.

doi:10.1039/b514108g

Cited by 176 publications

(142 citation statements)

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“…Note however that, whereas such a stoichiometry is effectively found for RBTP complexes under extraction conditions, 15,19,56,57 terpy generally presents lower and variable stoichiometries with f elements. 23, 58 Yet, this 1 : 3 coordination mode is interesting therein for three main reasons.…”

Section: Computational Detailsmentioning

confidence: 85%

“…3 Resistance to hydrolysis and radiolysis is also of major concern for a potential use of BTP at the industrial scale. 15 Various studies have proved that they contribute to the exceptional 1 : 3 stoichiometry of alkyl-BTP ligands by limiting protonation and H-bonding. 16,19 Neglecting alkyl groups is thus not trivial, 71 and for this reason we felt that it was relevant to investigate HBTP and MeBTP properties.…”

Section: Discussionmentioning

confidence: 99%

“…[6][7][8][9][10][11]. Tridentate nitrogen molecules were found to feature very good extracting properties, 7,[12][13][14][15][16] and in particular the so-called RBTP (alkylated 2,6-di(1,2,4-triazin-3-yl)pyridine) was identified as the most selective nitrogen ligand to date. 7, 15 An effort was made to determine the role of different chemical parameters like substituents, ligand concentration, solvent or number of nitrogen atoms onto the extraction efficiency.…”

Section: Introductionmentioning

confidence: 99%

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DFT modeling of the relative affinity of nitrogen ligands for trivalent f elements: an energetic point of view

et al. 2007

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aIn many theoretical studies dealing with the selective complexation of trivalent actinides with respect to trivalent lanthanides, the method of calculation is assessed by comparing computed geometries with crystal structures that are often available. Yet, the selectivity is better rationalized through thermodynamic data, as enthalpy and entropy terms. In this article, we have theoretically modeled competing complexation reactions of [Ce(terpy) 3+ systems (terpy = 2,2 0 :6 0 2 00 -terpyridine; MeBTP = methyl-2,6-di(1,2,4-triazin-3-yl)pyridine) within the framework of the Density Functional Theory. Our calculations manage to qualitatively account for the experimental relative stabilities of terpy and MeBTP complexes, and in particular for the better coordinating strength of MeBTP for trivalent uranium. We also show by comparing the MeBTP ligand with its non-alkylated form (HBTP) that model systems often used in quantum chemistry must be carefully chosen when energetic comparisons are undertaken.

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Section: Computational Detailsmentioning

confidence: 85%

Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

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DFT modeling of the relative affinity of nitrogen ligands for trivalent f elements: an energetic point of view

et al. 2007

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“…Plutonium tracer (mainly 239 Pu) was purified from 241 Am 34 and the 233 U tracer was purified from 229 Th using standard ion-exchange methods reported before. 32 The valency of Pu was adjusted to the +4 state by using NaNO 2 and ammonium metavanadate as the holding oxidant.…”

Section: Methodsmentioning

confidence: 99%

“…237,238 In particular, CyMe4-BTP (Chart 2.45) had good solubility, resistance to radiolysis and hydrolysis, and exceptional extraction properties (DAm up to 500, S.F.Am/Eu up to 5000). 239 The extension of the aromatic system to the tetradentate ligand CyMe4-BTBP Chart 2. 44 (Chart 2.45) allowed for good stripping properties at the cost of very slow extraction kinetics, without losing selectivity.…”

Section: ) No Extraction Of Am(iii) or Eu(iii) Wasmentioning

confidence: 99%

Alkylation and pre-organisation of diglycolamide ligands on flexible platforms for nuclear waste treatment

Leoncini

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Controlling Actinide Extraction Chemistry (Separation of Actinides from Lanthanides as Part of Nuclear Fuel Recycling)

Westwood

Harwood

2018

Encyclopedia of Inorganic and Bioinorganic Chemistry

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This article outlines some of the techniques and processes involved in the extraction of actinides that are present in spent nuclear fuel (SNF). Owing to the very similar chemistries of the actinides and lanthanides, it is difficult to differentiate the elements in a complex matrix of elements that are present in SNF. However, exploiting subtle covalent differences in the actinide bonding with certain ligands has opened a whole area of research aimed toward the development of actinide‐selective ligands. It is vitally important to separate the actinides from the spent fuel removed from nuclear reactors as it is the actinides themselves, and specifically the minor actinides (americium, curium, and neptunium) that contribute to the long‐lasting radiotoxic properties of the used fuel. Once separated, these elements can be transmuted into shorter‐lived, more stable isotopes by bombardment with neutrons in fast neutron reactors (Generation IV), which are due to phase online over next decade. The much larger concentration of neutron absorbing lanthanides in the spent fuel, together with their very similar chemistry to the actinides, renders the separation a very difficult challenge.

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New bis(triazinyl) pyridines for selective extraction of americium(iii)

Cited by 176 publications

References 37 publications

DFT modeling of the relative affinity of nitrogen ligands for trivalent f elements: an energetic point of view

DFT modeling of the relative affinity of nitrogen ligands for trivalent f elements: an energetic point of view

Alkylation and pre-organisation of diglycolamide ligands on flexible platforms for nuclear waste treatment

Controlling Actinide Extraction Chemistry (Separation of Actinides from Lanthanides as Part of Nuclear Fuel Recycling)

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