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Leaching of irradiated polymers: solution characterization and actinides complexation

Identifieur interne : 000089 ( Hal/Curation ); précédent : 000088; suivant : 000090

Leaching of irradiated polymers: solution characterization and actinides complexation

Auteurs : Elodie Fromentin [France]

Source :

RBID : Hal:tel-01622137

Descripteurs français

mix :
- complexation , europium, hydrolyse , molécules hydrosolubles , radio-oxydation , polyuréthane .

English descriptors

mix :
- hydrolysis , hydrosoluble molecules , radio-oxidation .

Abstract

The first aim of this work is to study the degradation of an industrial polyesterurethane (PURm) by radio-oxidation and then by leaching in an alkaline aqueous solution. The second aim is to measure the complexing power of hydrosoluble degradation products (HDP) with actinides. To reach these goals, PURm was first characterized and then radio-oxidized at room temperature with gamma-rays up to 10 MGy. Second, it was leached at pH 13.3 at different temperature values. Numerous analytical techniques were employed in order to characterize the HDP which were obtained. Europium(III) was used as an analogue of actinides(III) and the behavior of HDP with europium(III) was analyzed by time-resolved luminescence spectroscopy (TRLS). Whatever the received dose by PURm, adipic acid and butane-1,4-diol are the two main HDP in leachates. The leaching data acquired at 40 and 60°C, on the 1 MGy radio-oxidized PURm, correlate with the model given by Yoon et al. (1997). However, the data at room temperature (22°C in average) are not in agreement with the model. Nevertheless, it seems that the plateau which was reached at long-term leaching is the same whatever the temperature used in this study.The results allow to conclude that the predominant mechanism occurring during the leaching of unirradiated and radio-oxidized PURm in an alkaline medium is the hydrolysis of the soft segments ester groups.The complexation of europium(III) by HDP in alkaline medium was demonstrated. The measurement of the complexing power and the identification of ligands was achieved under certain conditions.

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Le document en format XML

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<title xml:lang="fr">Lixiviation des polymères irradiés : caractérisation de la solution et complexation des actinides</title>
<author><name sortKey="Fromentin, Elodie" sort="Fromentin, Elodie" uniqKey="Fromentin E" first="Elodie" last="Fromentin">Elodie Fromentin</name>
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<term> europium</term>
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<front><div type="abstract" xml:lang="en">The first aim of this work is to study the degradation of an industrial polyesterurethane (PURm) by radio-oxidation and then by leaching in an alkaline aqueous solution. The second aim is to measure the complexing power of hydrosoluble degradation products (HDP) with actinides. To reach these goals, PURm was first characterized and then radio-oxidized at room temperature with gamma-rays up to 10 MGy. Second, it was leached at pH 13.3 at different temperature values. Numerous analytical techniques were employed in order to characterize the HDP which were obtained. Europium(III) was used as an analogue of actinides(III) and the behavior of HDP with europium(III) was analyzed by time-resolved luminescence spectroscopy (TRLS). Whatever the received dose by PURm, adipic acid and butane-1,4-diol are the two main HDP in leachates. The leaching data acquired at 40 and 60°C, on the 1 MGy radio-oxidized PURm, correlate with the model given by Yoon et al. (1997). However, the data at room temperature (22°C in average) are not in agreement with the model. Nevertheless, it seems that the plateau which was reached at long-term leaching is the same whatever the temperature used in this study.The results allow to conclude that the predominant mechanism occurring during the leaching of unirradiated and radio-oxidized PURm in an alkaline medium is the hydrolysis of the soft segments ester groups.The complexation of europium(III) by HDP in alkaline medium was demonstrated. The measurement of the complexing power and the identification of ligands was achieved under certain conditions.</div>
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            <title xml:lang="fr">Lixiviation des polymères irradiés : caractérisation de la solution et complexation des actinides</title>
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                <author role="aut">                  <persName>                    <forename type="first">Elodie</forename>
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                <term xml:lang="fr"> complexation </term>
                <term xml:lang="fr"> europium</term>
                <term xml:lang="fr">polyuréthane </term>
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            <abstract xml:lang="en">The first aim of this work is to study the degradation of an industrial polyesterurethane (PURm) by radio-oxidation and then by leaching in an alkaline aqueous solution. The second aim is to measure the complexing power of hydrosoluble degradation products (HDP) with actinides. To reach these goals, PURm was first characterized and then radio-oxidized at room temperature with gamma-rays up to 10 MGy. Second, it was leached at pH 13.3 at different temperature values. Numerous analytical techniques were employed in order to characterize the HDP which were obtained. Europium(III) was used as an analogue of actinides(III) and the behavior of HDP with europium(III) was analyzed by time-resolved luminescence spectroscopy (TRLS). Whatever the received dose by PURm, adipic acid and butane-1,4-diol are the two main HDP in leachates. The leaching data acquired at 40 and 60°C, on the 1 MGy radio-oxidized PURm, correlate with the model given by Yoon et al. (1997). However, the data at room temperature (22°C in average) are not in agreement with the model. Nevertheless, it seems that the plateau which was reached at long-term leaching is the same whatever the temperature used in this study.The results allow to conclude that the predominant mechanism occurring during the leaching of unirradiated and radio-oxidized PURm in an alkaline medium is the hydrolysis of the soft segments ester groups.The complexation of europium(III) by HDP in alkaline medium was demonstrated. The measurement of the complexing power and the identification of ligands was achieved under certain conditions.</abstract>
            <abstract xml:lang="fr">L’objectif de ce travail est d’étudier la dégradation d’un polyesteruréthane industriel (PURm) par radio-oxydation puis par lixiviation en solution aqueuse à pH basique, dans le but d’évaluer le pouvoir complexant des produits de dégradation hydrosolubles (PDH) avec les actinides. Afin d’atteindre ces objectifs, le PURm a été caractérisé puis radio-oxydé à température ambiante aux rayonnements gamma jusqu’à 10 MGy. Il a ensuite été lixivié à pH 13,3 à différentes températures. De nombreuses techniques analytiques ont été employées afin de caractériser les PDH obtenus. De l’europium(III), simulant les actinides(III), a été mis en solution avec les PDH et l’interaction Eu-PDH a été analysée par spectrofluorimétrie laser à résolution temporelle (SLRT).Quelle que soit la dose reçue par le PURm, l’acide adipique et le butane-1,4-diol sont les deux PDH majoritaires dans les lixiviats. Les données de lixiviation acquises à 40 et 60°C, sur le PURm radio-oxydé jusqu’à 1 MGy, corrèlent avec le modèle proposé par Yoon et al. (1997). Cependant, les données à température ambiante (22°C en moyenne) ne sont pas en accord avec ce modèle. Il semble néanmoins qu’aux temps de lixiviation longs, le plateau atteint soit similaire quelle que soit la température employée dans cette étude.Les résultats obtenus permettent de conclure que le mécanisme prédominant lors de la lixiviation en milieu basique du PURm non irradié et radio-oxydé est l’hydrolyse des groupes esters des segments souples.La complexation de l’europium(III) par les PDH à pH basique a été mise en évidence. La détermination de la constante de complexation et l’identification des ligands, dans certaines conditions, a été réalisée.</abstract>
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Leaching of irradiated polymers: solution characterization and actinides complexation

Leaching of irradiated polymers: solution characterization and actinides complexation

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Descripteurs français

English descriptors

Abstract

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