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Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides

Abstract

In the field of long-lived radionuclides separation from waste generated during spent fuel reprocessing, the picolinamides have been chosen as potential extractants for the selective extraction of actinides (III) from lanthanides (III). The first studies initiated on the most simple molecule of the picolinamide family, namely 2-pyridinecarboxamide, pointed out that in an aqueous media the complexation stability constant between this ligand and Am(III) is roughly 10 times higher than the ones corresponding to Ln(III). The synthesis of lipophilic derivatives of 2-pyridinecarboxamide leaded to extraction experiments. The extraction of metallic cation by lipophilic picolinamides, according to a solvatation mechanism, is strongly dependent on the nature of the amide function: a primary amide function (group I) leads to a good extraction; on the contrary, there is a decrease for secondary (group II) and tertiary (group III) amide functions. From a theoretical point of view, this work leads finally to the following conclusions: confirmation of the importance of the presence of soft donor atoms within the extractants (nitrogen in our case) for An(III)/Ln(III). Also, sensitivity of this soft donor atom regarding the protonation reaction; prevalence in our case of the affinity of the extractant for the metallic cation over the lipophilia of the  More>>
Authors:
Cordier, P Y [1] 
  1. CEA Marcoule, Departement de Recherche en Retraitement et en Vitrification, 30 - Bagnols-sur-Ceze (France)
Publication Date:
Jul 01, 1996
Product Type:
Thesis/Dissertation
Report Number:
CEA-R-5762
Reference Number:
SCA: 400105; 050800; PA: AIX-29:061104; EDB-98:120345; SN: 98002033130
Resource Relation:
Other Information: DN: 105 refs.; TH: These (D. es Sc.); PBD: Jul 1996
Subject:
40 CHEMISTRY; 05 NUCLEAR FUELS; ACTINIDE COMPLEXES; AMIDES; CHEMICAL PREPARATION; CHEMICAL PROPERTIES; INFRARED SPECTRA; MOLECULAR MODELS; NMR SPECTRA; PHYSICAL PROPERTIES; PYRIDINES; RAMAN SPECTRA; RARE EARTHS; REPROCESSING; SOLUBILITY; SOLVATION; SOLVENT EXTRACTION; SPENT FUELS; ULTRAVIOLET SPECTRA; YEARS LIVING RADIOISOTOPES
OSTI ID:
668987
Research Organizations:
CEA Marcoule, Departement de Recherche en Retraitement et en Vitrification, 30 - Bagnols-sur-Ceze (France)
Country of Origin:
France
Language:
French
Other Identifying Numbers:
Other: ON: DE99606801; TRN: FR9803954061104
Availability:
INIS; OSTI as DE99606801
Submitting Site:
FRN
Size:
249 p.
Announcement Date:
Dec 07, 1998

Citation Formats

Cordier, P Y. Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides. France: N. p., 1996. Web.
Cordier, P Y. Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides. France.
Cordier, P Y. 1996. "Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides." France.
@misc{etde_668987,
title = {Separation by liquid-liquid extraction of actinides(III) from lanthanides(III) using new molecules: the picolinamides; Separation par extraction liquide-liquide des actinides(III) des lanthanides(III) par de nouvelles molecules: les picolinamides}
author = {Cordier, P Y}
abstractNote = {In the field of long-lived radionuclides separation from waste generated during spent fuel reprocessing, the picolinamides have been chosen as potential extractants for the selective extraction of actinides (III) from lanthanides (III). The first studies initiated on the most simple molecule of the picolinamide family, namely 2-pyridinecarboxamide, pointed out that in an aqueous media the complexation stability constant between this ligand and Am(III) is roughly 10 times higher than the ones corresponding to Ln(III). The synthesis of lipophilic derivatives of 2-pyridinecarboxamide leaded to extraction experiments. The extraction of metallic cation by lipophilic picolinamides, according to a solvatation mechanism, is strongly dependent on the nature of the amide function: a primary amide function (group I) leads to a good extraction; on the contrary, there is a decrease for secondary (group II) and tertiary (group III) amide functions. From a theoretical point of view, this work leads finally to the following conclusions: confirmation of the importance of the presence of soft donor atoms within the extractants (nitrogen in our case) for An(III)/Ln(III). Also, sensitivity of this soft donor atom regarding the protonation reaction; prevalence in our case of the affinity of the extractant for the metallic cation over the lipophilia of the extractant to ensure good distribution coefficients. The extraction and Am(III)/Ln(III) separation performances of the picolinamides from pertechnetic media leads to the design of a possible flowsheet for the reprocessing of high level liquid waste, with the new idea of an integrated technetium reflux. (author) 105 refs.}
place = {France}
year = {1996}
month = {Jul}
}