Published November 21, 2012 | Version v1
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Study of the interactions between Eu(III) and Al2O3 particles in the presence of phenolic acids

Description

In the framework of environmental pollution by radionuclides, this work was focused on the interactions occurring in systems containing europium(III) - as a chemical analogue for the actinides Am(III) and Cm(III) -, phenolic acids - lignin degradation products and anti-fungi, naturally occurring in soils, and alumina - representative of sorption sites found in the environment. This study was conducted at different scales of description: the macroscopic scale - to quantify Eu(III) and/or phenolic acids adsorption onto the mineral surface -, and the microscopic scale - to study the chemical environment of Eu(III) using Time-Resolved Luminescence Spectroscopy (TRLS). First, the binary systems, i.e. systems containing only two entities among the three previously cited, were characterized. Complexation constants of Eu(III) by three phenolic acids (4-hydroxybenzoic, 3,4-dihydroxybenzoic, and 3,4,5-trihydroxybenzoic acids) were determined and quantum calculations (DFT) were carried out on La(III)-acid complex analogues. Sorption of the acids onto aluminol sites was modelled using surface complexation concepts. Analyses of two ternary systems (containing 4-hydroxybenzoic and 3,4-dihydroxybenzoic acids) revealed synergistic processes for Eu(III) and phenolic acids sorption onto Al2O3. A spectral fingerprint of ternary complex involving Eu(III)/4-hydroxybenzoic acid/Al2O3 surface sites was evidenced. (author)

Abstract (French)

Dans le cadre de la comprehension des mecanismes de pollution environnementale par les elements radioactifs, ce travail de these s'est interesse aux interactions existant dans des systemes comprenant les trois entites europium(III) (pris comme analogue des actinides Am(III) et Cm(III)), acides phenoliques (produits de degradation de la lignine et antifongiques presents naturellement dans les sols) et l'alumine (representatif des sites de surface presents dans l'environnement). Differents niveaux d'analyse ont ete employes pour cette etude: l'echelle macroscopique - par la quantification de l'adsorption de Eu(III) et/ou des acides phenoliques sur la surface - et l'echelle microscopique - par l'etude de l'environnement chimique de Eu(III) par spectroluminescence laser a resolution temporelle (SLRT). Au prealable, les systemes binaires, c'est a dire des systemes contenant deux des trois entites citees precedemment, ont ete etudies. Ainsi, les constantes de complexation de Eu(III) par trois acides phenoliques (acides 4-hydroxybenzoique, 3,4-dihydroxybenzoique et 3,4,5 trihydroxybenzoique) ont ete determinees par SLRT et une etude en modelisation moleculaire (DFT) a ete realisee sur des systemes analogues La(III)-acides. La sorption des trois acides sur les sites aluminol a ete modelisee a l'aide de modeles de complexation de surface. Les analyses menees sur deux systemes ternaires (acides 4-hydroxybenzoique, 3,4-dihydroxybenzoique) ont mis en evidence une synergie pour la sorption de Eu(III) par ces acides sur Al2O3. Une empreinte spectrale d'un complexe ternaire a ete isolee dans le cas du systeme Eu(III)/acide 4-hydroxybenzoique/Al2O3

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Additional details

Additional titles

Original title (French)
Etude des interactions entre Eu(III) et des particules d'alumine en presence d'acides phenoliques

Publishing Information

Imprint Pagination
268 p.
Report number
FRCEA-TH--3827

INIS

Country of Publication
France
Country of Input or Organization
France
INIS RN
44048739
Subject category
S54: ENVIRONMENTAL SCIENCES;
Resource subtype / Literary indicator
Thesis
Descriptors DEI
ADSORPTION; ALUMINIUM OXIDES; DENSITY FUNCTIONAL METHOD; EUROPIUM; EUROPIUM COMPLEXES; RADIOISOTOPES
Descriptors DEC
ALUMINIUM COMPOUNDS; CALCULATION METHODS; CHALCOGENIDES; COMPLEXES; ELEMENTS; ISOTOPES; METALS; OXIDES; OXYGEN COMPOUNDS; RARE EARTH COMPLEXES; RARE EARTHS; SORPTION; VARIATIONAL METHODS

Optional Information

Notes
refs.; Available from the INIS Liaison Officer for France, see the 'INIS contacts' section of the INIS-NKM website for current contact and E-mail addresses: http://www.iaea.org/INIS/contacts/