An Improved Hydrolytically-Stable Bis-Triazinyl-Pyridine (BTP) for Selective Actinide Extraction

Trumm, Sascha; Geist, Andreas; Panak, Petra J.; Fanghänel, Thomas

doi:10.1080/07366299.2011.539129

Cited by 123 publications

(95 citation statements)

References 36 publications

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“…More recently, a symmetrical BTP ligand derived from camphor has shown both improved solubility and fast extraction kinetics compared to related BTP ligands. [14] However, this ligand is susceptible to precipitate formation in contact with nitric acid solutions of high acidity. A high extractant solubility is desirable for the treatment of waste solutions containing high concentrations of metal ions, such as those produced in the PUREX process.…”

Section: Introductionmentioning

confidence: 99%

Synthesis and Evaluation of Lipophilic BTBP Ligands for An/Ln Separation in Nuclear Waste Treatment: The Effect of Alkyl Substitution on Extraction Properties and Implications for Ligand Design

et al. 2012

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Northumbria University has developed Northumbria Research Link (NRL) to enable users to access the University's research output. Copyright © and moral rights for items on NRL are retained by the individual author(s) and/or other copyright owners. Single copies of full items can be reproduced, displayed or performed, and given to third parties in any format or medium for personal research or study, educational, or not-for-profit purposes without prior permission or charge, provided the authors, title and full bibliographic details are given, as well as a hyperlink and/or URL to the original metadata page. The content must not be changed in any way. Full items must not be sold commercially in any format or medium without formal permission of the copyright holder. The full policy is available online: http://nrl.northumbria.ac.uk/policies.html This document may differ from the final, published version of the research and has been made available online in accordance with publisher policies. To read and/or cite from the published version of the research, please visit the publisher's website (a subscription may be required.) Karel Stamberg, [b] Ana Núñez, [c] Hitos Galán [c] and Amparo G. Espartero [c] Keywords: Ligands / Actinides / Lanthanides / Nuclear waste / Extraction Submitted to the European Journal of Organic ChemistryFour new 6,6'-bis(1,2,4-triazin-3-yl)-2,2'-bipyridine (BTBP) ligands containing either additional alkyl groups on the pyridine rings, or 7-membered aliphatic rings attached to the triazine rings, have been synthesized, and the effects of additional alkyl substitution in the 4-and 4'-positions of the pyridine rings on their extraction properties with Ln(III) and An(III) cations in simulated nuclear waste solutions were studied. The speciation of ligand 13 with some trivalent lanthanide nitrates was elucidated by 1 H NMR titrations and electrospray-ionization mass spectrometry. Whereas ligand 13 formed both 1:1 and 1:2 complexes with La(III) and Y(III), only 1:2 complexes were observed with Eu(III) and Ce(III).Quite unexpectedly, both alkyl-substituted ligands 12 and 13 showed lower solubilities in certain diluents than the nonsubstituted ligand CyMe 4 -BTBP. Compared to CyMe 4 -BTBP, alkyl-substitution was found to decrease the rates of metal ion extraction of the BTBPs in both 1-octanol and cyclohexanone. A highly efficient (D Am > 10) and selective (SF Am/Eu > 90) extraction was observed for BTBPs 12 and 13 in cyclohexanone, and for BTBP 13 in 1-octanol in the presence of a phase-transfer agent. The implications of these results for the design of improved extractants for radioactive waste treatment are discussed. IntroductionOne of the major goals in the treatment of nuclear waste arising from the PUREX process is the selective removal of the radiotoxic minor actinides (Am and Cm) from the lanthanides in a solvent extraction process, known as the SANEX process.[1] Once removed, the oxides of these elements may be converted by high-energy neutrons (transmutation) into less radiotoxic or no...

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Section: Introductionmentioning

confidence: 99%

Synthesis and Evaluation of Lipophilic BTBP Ligands for An/Ln Separation in Nuclear Waste Treatment: The Effect of Alkyl Substitution on Extraction Properties and Implications for Ligand Design

et al. 2012

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“…The adsorption behavior of isobutyl-BTP/SiO 2 -P adsorbent toward 241 Am(III), Y(III), middle and heavy Ln(III) shared the similar adsorption tendency. The adsorption firstly increased as NO 3 -concentration increased since the adsorption reaction needs the participation of NO 3 - [15,24]. Then the maximium adsorption was achieved around 1-2 M NO 3 -, and later the adsorption showed slightly decrease tendency as NO 3 -concentration further increased.…”

Section: Effect Of Nitrate Concentration On Adsorptionmentioning

confidence: 94%

“…Besides selectivity, the stability against nitric acid and radiation is also essential in the application to HLLW separation. As the BTPs with straight side chains such as methyl-BTP, n-propyl-BTP, n-butyl-BTP showed poor stability against nitric acid and radiation [10,[13][14][15][16], the BTPs with branched alkyl group such as isopropyl-BTP, isobutyl-BTP, isohexyl-BTP [17][18][19][20][21][22][23] and the BTPs with cycle structures, e.g., CA-BTP, CyMe 4 -BTP, Me 2 -CA-BTP [14,24,25] have been designed and synthesized for the purpose of improving the stability.…”

Section: Introductionmentioning

confidence: 99%

“…As S containing molecules are not as environment friendly as N-donor molecules, they are not optimal candidates. In recent 10 years, the new N-donor ligands, BTPs (BTP: 2,6-bis-(5,6-dialkyl-1,2,4-triazin-3-yl)-pyridines), which were firstly used for MA(III) separation from HLLW by Kolarik [11,12], have received wide attention due to their high selectivity of MA(III) over Ln(III) from nitrate solution with the separation factor (SF Am/Eu ) around 100 [9][10][11][12][13][14][15][16][17][18][19][20][21][22][23][24][25]. Moreover, as BTPs molecules contain only C, H, N atoms and fullfill the CHON principle, they can be completely burnt into gasous products after use up, which will reduce the secondary radioactive waste amount.…”

Section: Introductionmentioning

confidence: 99%

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Adsorption behavior and mechanism of isobutyl-BTP/SiO2-P adsorbent for Am(III) and Ln(III) in nitrate solution

Wang

Ning

Zou

et al. 2015

J Radioanal Nucl Chem

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Porous isobutyl-BTP/SiO 2 -P adorbent was prepared to separate MA(III) from HLLW. The adsorption behavior of isobutyl-BTP/SiO 2 -P toward 241 Am(III), Y(III) and Ln(III) in 0.01 M HNO 3 -NaNO 3 solution was studied. Isobutyl-BTP/SiO 2 -P showed high adsorption selectivity toward 241 Am(III) over Y(III) and Ln(III) fission products. Adsorption kinetics of Dy(III) followed pseudo-secondorder rate equation, and its adsorption isotherm matched the Langmuir isotherm equation well. Moreover, the adsorption product of Dy(III) on isobutyl-BTP/SiO 2 -P was studied using extended X-ray absorption fine structure (EAXFS) method and Dy(isobutyl-BTP/SiO 2 -P) 3 3? was supposed as the main adsorption species.

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“…In THP/1-octanol (7 : 3 vol), equilibrium was reached in ~10 min and S.F.Am/Eu values ≤ 100 (0.5 M HNO3) were obtained. 245 On changing the solvent system to PTMS, the solubility as well as the resistance to third phase formation increased (the highest HNO3 concentration usable U and Pu were extracted. Since CyMe4-BTBP preferentially extracts trivalent An, the extraction of tetra-and hexavalent An was due to an interaction with the diluent.…”

Section: Bis-triazinyl and Related Ligandsmentioning

confidence: 99%

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

Leoncini

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An Improved Hydrolytically-Stable Bis-Triazinyl-Pyridine (BTP) for Selective Actinide Extraction

Cited by 123 publications

References 36 publications

Synthesis and Evaluation of Lipophilic BTBP Ligands for An/Ln Separation in Nuclear Waste Treatment: The Effect of Alkyl Substitution on Extraction Properties and Implications for Ligand Design

Synthesis and Evaluation of Lipophilic BTBP Ligands for An/Ln Separation in Nuclear Waste Treatment: The Effect of Alkyl Substitution on Extraction Properties and Implications for Ligand Design

Adsorption behavior and mechanism of isobutyl-BTP/SiO2-P adsorbent for Am(III) and Ln(III) in nitrate solution

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

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