Abstract
The solvent, used in France in Purex reprocessing plants at La Hague is tributylphosphate (TBP) diluted to 30% with a mixture of branched alkanes, for which the main component is branched dodecane (70%). In order to minimize volumes of organic wastes, we have to maintain Purex solvent qualities and to get rid of degradation products. The subject of this memoir concerns among all the degradation products the heaviest molecules. The separation and the identification of these products have been carried out by preparative steric exclusion chromatography, followed by the analysis of the samples by various analytical methods. An inactive residue containing heavy degradation products was prepared according to the process used in the UP3 La Hague plant. The Analysis of this residue using steric exclusion chromatography and GPC/MS methods, shows the presence of three families of compounds heavier than TBP: the ''dimers of TBP'' (provided from the addition of two molecules of TBP), the ''TBP-alkanes'' (the main molecule is the result of the addition of dodecane with TBP), and ''the functionalized TBP'' (hydroxyled TBP, nitrous TBP, nitrated TBP). Plutonium (IV) retention tests were made on the various fractions generated by steric chromatography. They showed that ''the dimers of TBP'' and
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Citation Formats
Pozo, Claudine.
Application of steric exclusion chromatography for the separation of degradation products of the solvent used for the reprocessing of the nuclear fuels; Application de la chromatographie d'exclusion sterique a la separation de produits de degradation du solvant du retraitement des combustibles nucleaires.
France: N. p.,
1993.
Web.
Pozo, Claudine.
Application of steric exclusion chromatography for the separation of degradation products of the solvent used for the reprocessing of the nuclear fuels; Application de la chromatographie d'exclusion sterique a la separation de produits de degradation du solvant du retraitement des combustibles nucleaires.
France.
Pozo, Claudine.
1993.
"Application of steric exclusion chromatography for the separation of degradation products of the solvent used for the reprocessing of the nuclear fuels; Application de la chromatographie d'exclusion sterique a la separation de produits de degradation du solvant du retraitement des combustibles nucleaires."
France.
@misc{etde_10136763,
title = {Application of steric exclusion chromatography for the separation of degradation products of the solvent used for the reprocessing of the nuclear fuels; Application de la chromatographie d'exclusion sterique a la separation de produits de degradation du solvant du retraitement des combustibles nucleaires}
author = {Pozo, Claudine}
abstractNote = {The solvent, used in France in Purex reprocessing plants at La Hague is tributylphosphate (TBP) diluted to 30% with a mixture of branched alkanes, for which the main component is branched dodecane (70%). In order to minimize volumes of organic wastes, we have to maintain Purex solvent qualities and to get rid of degradation products. The subject of this memoir concerns among all the degradation products the heaviest molecules. The separation and the identification of these products have been carried out by preparative steric exclusion chromatography, followed by the analysis of the samples by various analytical methods. An inactive residue containing heavy degradation products was prepared according to the process used in the UP3 La Hague plant. The Analysis of this residue using steric exclusion chromatography and GPC/MS methods, shows the presence of three families of compounds heavier than TBP: the ''dimers of TBP'' (provided from the addition of two molecules of TBP), the ''TBP-alkanes'' (the main molecule is the result of the addition of dodecane with TBP), and ''the functionalized TBP'' (hydroxyled TBP, nitrous TBP, nitrated TBP). Plutonium (IV) retention tests were made on the various fractions generated by steric chromatography. They showed that ''the dimers of TBP'' and ''the functionalized TBP'' families are responsible for that retention. These results confirm the good efficiency of the solvent distillation system operated in UP3 plant which allow the elimination of heavy degradation products of the solvent with the residue and then restore excellent extracting properties for the recycled solvent. (author). [French] Le solvant. utilise au cours du procede Purex dans les usines de retraitement. est constitue en France de TBP dilue dans un melange d' alcanes ramifies contenant principalement 12 atomes de carbone. Le recyclage du solvant dans le procede impose l'elimination des produits de degradation qui pourraient en alterer les performances. Parmi les produits de degradation generes. ce sont les plus lourds qui font l'objet de ce memoire. La chromatographie d'exclusion sterique preparative, suivie de diverses methodes analytiques, a ete appliquee a la separation puis a l'identification de ces produits. Ils avaient ete concentres dans les residus de distillation provenant d'un solvant ne contenant pas d'element radioactif, sur lequel ont ete simulees les conditions de fonctionnement et de degradation du premier cycle de l'usine UP3 de La Hague. Les resultats fournis principalement par la CPG/SM ont permis de determiner trois familles principales de composes plus lourds que le TBP : les ''dimeres du TBP'' (provenant de l'addition de deux molecules de TBP), les ''TBP-alcanes'' (dont le representant majoritaire resulte de l'addition d'une molecule de dodecane sur du TBP), les ''TBP fonctionnalises'' (TBP hydroxyles, TBP nitres et TBP nitrates). Sur les fractions obtenues par chromatographie. des tests de retention du plutonium ont ete pratiques. Ils ont montre que ce sont les familles de dimeres de TBP et de TBP fonctionnalises qui sont essentiellement responsables de la retention de ce cation metallique. Le fonctionnement de l'usine UP3. utilisant la distillation pour regenerer une partie du solvant. permet d'eliminer au fur et a mesure les composes de degradation lourds dans le residu de distillation. Ceux-ci peuvent etre a terme genants pour le bon fonctionnement du procede puisque certains sont des complexants efficaces du plutonium. Ils pourraient egalement. s'ils n'etaient pas elimines. generer au sein du milieu reactionnel des produits encore plus lourds. (auteur)}
place = {France}
year = {1993}
month = {Aug}
}
title = {Application of steric exclusion chromatography for the separation of degradation products of the solvent used for the reprocessing of the nuclear fuels; Application de la chromatographie d'exclusion sterique a la separation de produits de degradation du solvant du retraitement des combustibles nucleaires}
author = {Pozo, Claudine}
abstractNote = {The solvent, used in France in Purex reprocessing plants at La Hague is tributylphosphate (TBP) diluted to 30% with a mixture of branched alkanes, for which the main component is branched dodecane (70%). In order to minimize volumes of organic wastes, we have to maintain Purex solvent qualities and to get rid of degradation products. The subject of this memoir concerns among all the degradation products the heaviest molecules. The separation and the identification of these products have been carried out by preparative steric exclusion chromatography, followed by the analysis of the samples by various analytical methods. An inactive residue containing heavy degradation products was prepared according to the process used in the UP3 La Hague plant. The Analysis of this residue using steric exclusion chromatography and GPC/MS methods, shows the presence of three families of compounds heavier than TBP: the ''dimers of TBP'' (provided from the addition of two molecules of TBP), the ''TBP-alkanes'' (the main molecule is the result of the addition of dodecane with TBP), and ''the functionalized TBP'' (hydroxyled TBP, nitrous TBP, nitrated TBP). Plutonium (IV) retention tests were made on the various fractions generated by steric chromatography. They showed that ''the dimers of TBP'' and ''the functionalized TBP'' families are responsible for that retention. These results confirm the good efficiency of the solvent distillation system operated in UP3 plant which allow the elimination of heavy degradation products of the solvent with the residue and then restore excellent extracting properties for the recycled solvent. (author). [French] Le solvant. utilise au cours du procede Purex dans les usines de retraitement. est constitue en France de TBP dilue dans un melange d' alcanes ramifies contenant principalement 12 atomes de carbone. Le recyclage du solvant dans le procede impose l'elimination des produits de degradation qui pourraient en alterer les performances. Parmi les produits de degradation generes. ce sont les plus lourds qui font l'objet de ce memoire. La chromatographie d'exclusion sterique preparative, suivie de diverses methodes analytiques, a ete appliquee a la separation puis a l'identification de ces produits. Ils avaient ete concentres dans les residus de distillation provenant d'un solvant ne contenant pas d'element radioactif, sur lequel ont ete simulees les conditions de fonctionnement et de degradation du premier cycle de l'usine UP3 de La Hague. Les resultats fournis principalement par la CPG/SM ont permis de determiner trois familles principales de composes plus lourds que le TBP : les ''dimeres du TBP'' (provenant de l'addition de deux molecules de TBP), les ''TBP-alcanes'' (dont le representant majoritaire resulte de l'addition d'une molecule de dodecane sur du TBP), les ''TBP fonctionnalises'' (TBP hydroxyles, TBP nitres et TBP nitrates). Sur les fractions obtenues par chromatographie. des tests de retention du plutonium ont ete pratiques. Ils ont montre que ce sont les familles de dimeres de TBP et de TBP fonctionnalises qui sont essentiellement responsables de la retention de ce cation metallique. Le fonctionnement de l'usine UP3. utilisant la distillation pour regenerer une partie du solvant. permet d'eliminer au fur et a mesure les composes de degradation lourds dans le residu de distillation. Ceux-ci peuvent etre a terme genants pour le bon fonctionnement du procede puisque certains sont des complexants efficaces du plutonium. Ils pourraient egalement. s'ils n'etaient pas elimines. generer au sein du milieu reactionnel des produits encore plus lourds. (auteur)}
place = {France}
year = {1993}
month = {Aug}
}